List of Edited Articles

@article{nokey,

title = {Reproducibility and transparency: what’s going on and how can we help (Q&A article)},

author = {Brian Nosek and Christine Mummery and Leonardo Scarabelli and Vitaly Podzorov },

url = {https://www.nature.com/articles/s41467-024-54614-2.pdf},

doi = {10.1038/s41467-024-54614-2},

year  = {2024},

date = {2024-12-04},

urldate = {2024-12-04},

journal = {Nature Communications},

volume = {15},

abstract = {Problems with experimental reproducibility affect every field of science. However, the opinions on the causes of the reproducibility “crisis” and how we all can help vary amongst fields as well as individual scientists. Here, we talk to experts from different fields of science to get their insights on this endemic issue. Professor Brian Nosek is a social psychologist at the University of Virginia and executive director of the Center for Open Science. Professor Christine Mummery is a developmental biologist at Leiden University Medical Center and the former President of the International Society of Stem Cell Research. Dr Leonardo Scarabelli is a chemist and group leader at the University of Cantabria. Professor Vitaly Podzorov is a physicist at Rutgers, the State University of New Jersey, and current Donald H. Jacobs Chair in Applied Physics.},

note = {Problems with experimental reproducibility affect every field of science. However, the opinions on the causes of the reproducibility “crisis” and how we all can help vary amongst fields as well as individual scientists. Here, we talk to experts from different fields of science to get their insights on this endemic issue.},

keywords = {},

pubstate = {forthcoming},

tppubtype = {article}

}

@article{nokey,

title = {Stress-eliminated liquid-phase fabrication of colloidal films above the critical crack thickness},

author = {Shiyuan Liu and Ying Hong and Wang Hong and Yi Zheng and Xiaodan Yang and Xuemu Li and Zhuomin Zhang and Xiaodong Yan and Yao Shan and Weikang Lin and Zehua Peng and Xingqi Zhang and Xi Yao and Zuankai Wang and Zhengbao Yang },

url = {https://www.nature.com/articles/s41467-024-54412-w.pdf},

doi = {10.1038/s41467-024-54412-w},

year  = {2024},

date = {2024-12-02},

urldate = {2024-12-02},

journal = {Nature Communications},

volume = {15},

number = {10136},

abstract = {The thickness of film materials is a critical factor influencing properties such as energy density, optical performance, and mechanical strength. However, the long-standing challenge of the intrinsic thermodynamic limit on maximum thickness often leads to detrimental cracking, compromising these desirable properties. In this study, we present an approach called the stress-eliminated liquid-phase fabrication (SELF) method. The SELF method eliminates the need for substrates to support the precursor solution used for film fabrication. We harness the intrinsic surface tension of the solution by confining it within specifically designed grids in a framework, forming suspended liquid bridges. This technique enables fabrication of crack-free ceramic films within a broad thickness range from 1 to 100 μm. Furthermore, the fabricated PZT films exhibit a high piezoelectric coefficient (d33) of 229 pC N−1. The customizable grids not only offer design freedom for film topologies but also facilitate the fabrication of diverse film arrays without the need for destructive cutting processes. Moreover, the freestanding nature of these films enhances their adaptability for MEMS processing, and the “capillary bridge” topology allows the PZT films to be used in ultrasound focusing transmitter, providing possibilities in the medical imaging.},

note = {There is a critical crack thickness in the production of thin films. Here, the authors utilize the surface tension of the liquid to eliminate the stresses within the film and produce ceramic layers with a controllable thickness and shape.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Measuring competing outcomes of a single-molecule reaction reveals classical Arrhenius chemical kinetics},

author = {Pieter J. Keenan and Rebecca M. Purkiss and Tillmann Klamroth and Peter A. Sloan and Kristina R. Rusimova 

},

url = {https://www.nature.com/articles/s41467-024-54677-1.pdf},

doi = {10.1038/s41467-024-54677-1},

year  = {2024},

date = {2024-11-28},

journal = {Nature Communications},

volume = {15},

number = {10322},

abstract = {Programming matter one molecule at a time is a long-standing goal in nanoscience. The atomic resolution of a scanning tunnelling microscope (STM) can give control over the probability of inducing single-outcome single-molecule reactions. Here we show it is possible to measure and influence the outcome of a single-molecule reaction with multiple competing outcomes. By precise injection of electrons from an STM tip, toluene molecules are induced to react with two outcomes: switching to an adjacent site or desorption. Within a voltage range set by the electronic structure of the molecule-surface system, we see that the branching ratio between these two outcomes is dependent on the excess energy the exciting electron carries. Using known values, ab-initio DFT calculations and empirical models, we conclude that this excess energy leads to a heating of a common intermediate physisorbed state and gives control over the two outcomes via their energy barriers and prefactors.},

note = {Controlling matter one molecule at a time is the ultimate goal of nanotechnology. Here, the authors show that it is possible to use a scanning tunnelling microscope to measure and influence the outcome of a single-molecule reaction with multiple competing outcomes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Enantioselective adsorption on chiral ceramics with medium entropy},

author = {Chao Chen and Yinglin Ma and Kunda Yao and Qingmin Ji and Wei Liu },

url = {https://www.nature.com/articles/s41467-024-54414-8.pdf},

doi = {10.1038/s41467-024-54414-8},

year  = {2024},

date = {2024-11-21},

urldate = {2024-11-21},

journal = {Nature Communications},

volume = {15},

number = {10105},

abstract = {Chiral metal surfaces provide an environment for enantioselective adsorption in various processes such as asymmetric catalysis, chiral recognition, and separation. However, they often suffer from limitations such as reduced enantioselectivity caused by kink coalescence and atomic roughness. Here, we present an approach using medium-entropy ceramic (MEC), specifically (CrMoTa)Si2 with a C40 hexagonal crystal structure, which overcomes the trade-off between thermal stability and enantioselectivity. Experimental confirmation is provided by employing quartz crystal microbalance (QCM), where the electrode is coated with MEC films using non-reactive magnetron sputtering technology. The chiral nature is verified through transmission electron microscopy and circular dichroism. Density-functional theory (DFT) calculations show that the stability of MEC films is significantly higher than that of high-index Cu surfaces. Through a combination of high-throughput DFT calculations and theoretical modeling, we demonstrate the high enantioselectivity (42% e.e.) of the chiral MEC for serine, a prototype molecule for studying enantioselective adsorption. The QCM results show that the adsorption amount of L-serine is 1.58 times higher than that of D-serine within a concentration range of 0-60 mM. These findings demonstrate the potential application of MECs in chiral recognition.},

note = {Chiral metals often suffer from limitations such as reduced selectivity caused by kink coalescence and atomic roughness. Here, the authors present chiral medium-entropy ceramics and overcome the trade-off between stability and enantioselectivity.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Light patterning semiconductor nanoparticles by modulating surface charges},

author = {Xiaoli He and Hongri Gu and Yanmei Ma and Yuhang Cai and Huaide Jiang and Yi Zhang and Hanhan Xie and Ming Yang and Xinjian Fan and Liang Guo and Zhan Yang and Chengzhi Hu },

url = {https://www.nature.com/articles/s41467-024-53926-7.pdf},

doi = {10.1038/s41467-024-53926-7},

year  = {2024},

date = {2024-11-13},

journal = {Nature Communications},

volume = {15},

number = {9843},

abstract = {Optical patterning of colloidal particles is a scalable and cost-effective approach for creating multiscale functional structures. Existing methods often use high-intensity light sources and customized optical setups, making them less feasible for large-scale microfabrication processes. Here, we report an optical patterning method for semiconductor nanoparticles by light-triggered modulation of their surface charge. Rather than using light as the primary energy source, this method utilizes UV-induced cleavage of surface ligands to modify surface charges, thereby facilitating the self-assembly of nanoparticles on a charged substrate via electrostatic interactions. By using citrate-treated ZnO nanoparticles, uniform ZnO patterns with variable thicknesses can be achieved. These multilayered ZnO patterns are fabricated into a UV detector with an on/off ratio exceeding 10^4. Our results demonstrate a simple yet effective way to pattern semiconductor nanoparticles, facilitating the large-scale integration of functional nanomaterials into emerging flexible and robotic microdevices.},

note = {The integration of colloidal nanoparticles into microdevices is essential for several advanced technologies. Here, the authors have developed a scalable method of UV-triggered surface charge modulation for the rapid surface patterning with semiconductor nanoparticles.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The role of surface substitution in the atomic disorder-to-order phase transition in multi-component core–shell structures},

author = {Wencong Zhang and Fan Li and Yi Li and Anran Song and Kun Yang and Dongchang Wu and Wen Shang and Zhenpeng Yao and Wenpei Gao and Tao Deng and Jianbo Wu },

url = {https://www.nature.com/articles/s41467-024-54104-5.pdf},

doi = {10.1038/s41467-024-54104-5},

year  = {2024},

date = {2024-11-11},

journal = {Nature Communications},

volume = {15},

number = {9762},

abstract = {Intermetallic phases with atomic ordering are highly active and stable in catalysts. However, understanding the atomistic mechanisms of disorder-to-order phase transition, particularly in multi-component systems, remains challenging. Here, we investigate the atom diffusion and phase transition within Pd@Pt-Co cubic nanoparticles during annealing, using in-situ electron microscopy and ex-situ atomic resolution element analysis. We reveal that initial outward diffusing Pd partially substitutes Pt, forming a (Pt, Pd)-Co ternary system in the surface region, enabling the phase transition at a low temperature of 400 °C, followed by shape-preserved inward propagation of the ordered phase. At higher temperatures, excessive interdiffusion across the interface changes the stoichiometric ratio, diminishing the atomic ordering, leading to obvious change in morphology. Calculations indicate that the Pd-substitute in (Pt, Pd)-Co system leads to a significantly lower phase transition temperature compared to that of Pt-Co alloy and thus a lower activation energy for atomic diffusion. These insights into atomistic behavior are crucial for future design of multi-component systems.},

note = {Understanding atomic-level ordering in multi-component systems is a challenge. Here, the authors investigate atom diffusion in cubic Pd@Pt-Co nanoparticles and find that substitution of Pd into (Pt, Pd)-Co lowers the phase transition temperature.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fluorescence from a single-molecule probe directly attached to a plasmonic STM tip},

author = {Niklas Friedrich and Anna Rosławska and Xabier Arrieta and Katharina Kaiser and Michelangelo Romeo and Eric Le Moal and Fabrice Scheurer and Javier Aizpurua and Andrei G. Borisov and Tomáš Neuman and Guillaume Schull },

url = {https://www.nature.com/articles/s41467-024-53707-2.pdf},

doi = {10.1038/s41467-024-53707-2},

year  = {2024},

date = {2024-11-10},

journal = {Nature Communications},

volume = {15},

number = {9733},

abstract = {The scanning tunneling microscope (STM) provides access to atomic-scale properties of a conductive sample. While single-molecule tip functionalization has become a standard procedure, fluorescent molecular probes remained absent from the available tool set. Here, the plasmonic tip of an STM is functionalized with a single fluorescent molecule and is scanned on a plasmonic substrate. The tunneling current flowing through the tip-molecule-substrate junction generates a narrow-line emission of light corresponding to the fluorescence of the negatively charged molecule suspended at the apex of the tip, i.e., the emission of the excited molecular anion. The fluorescence of this molecular probe is recorded for tip-substrate nanocavities featuring different plasmonic resonances, for different tip-substrate distances and applied bias voltages, and on different substrates. We demonstrate that the width of the emission peak can be used as a probe of the exciton-plasmon coupling strength and that the energy of the emitted photons is governed by the molecule interactions with its environment. Additionally, we theoretically elucidate why the direct contact of the suspended molecule with the metallic tip does not totally quench the radiative emission of the molecule.},

note = {Scanning tunneling microscopy (STM) gives access to the atomic-scale properties of matter. Here, the authors showcase the fluorescent functionalization of an STM tip using a single molecule in direct metal contact, permitting the local electrostatic and -dynamic environment to be probed.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Photochemistry dominates over photothermal effects in the laser-induced reduction of graphene oxide by visible light},

author = {Maxim Fatkullin and Dmitry Cheshev and Andrey Averkiev and Alina Gorbunova and Gennadiy Murastov and Jianxi Liu and Pavel Postnikov and Chong Cheng and Raul D. Rodriguez and Evgeniya Sheremet },

url = {https://www.nature.com/articles/s41467-024-53503-y.pdf},

doi = {10.1038/s41467-024-53503-y},

year  = {2024},

date = {2024-11-09},

journal = {Nature Communications},

volume = {15},

number = {9711},

abstract = {Graphene oxide (GO) possesses specific properties that are revolutionizing materials science, with applications extending from flexible electronics to advanced nanotechnology. A key method for harnessing GO’s potential is its laser-induced reduction, yet the exact mechanisms — photothermal versus photochemical effects — remain unclear. Herein, we discover the dominant role of photochemical reactions in the laser reduction of GO under visible light, challenging the prevailing assumption that photothermal effects are dominant. Employing a combination of Raman thermometry, X-ray photoelectron and photoluminescence spectroscopies, and electrical atomic force microscopy, we quantify the temperature and map the reduction process across micro and nano scales. Our findings demonstrate that the photochemical cleavage of oxygen-containing groups below a reduction threshold temperature is a decisive factor in GO reduction, leading to distinct characteristics that cannot be replicated by heating alone. This work clarifies the fundamental mechanisms of GO transformation under visible laser irradiation, highlighting the dominant role of photochemical processes. Distinguishing these subtleties enables the development of laser-reduced GO platforms for graphene-based applications compatible with industrial scales. We illustrate this potential by encoding information on GO surfaces as optical storage, allowing us to write binary sequences in long-term memory encoding invisible even through an optical microscope.},

note = {Laser reduction of graphene oxide is generally assumed to be primarily driven by heat. Here the authors show that light-triggered chemical reactions dominate over photothermal effects.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Atomically resolved imaging of the conformations and adsorption geometries of individual β-cyclodextrins with non-contact AFM},

author = {Márkó Grabarics and Benjamín Mallada and Shayan Edalatmanesh and Alejandro Jiménez-Martín and Martin Pykal and Martin Ondráček and Petra Kührová and Weston B. Struwe and Pavel Banáš and Stephan Rauschenbach and Pavel Jelínek and Bruno de la Torre },

url = {https://www.nature.com/articles/s41467-024-53555-0.pdf},

doi = {10.1038/s41467-024-53555-0},

year  = {2024},

date = {2024-11-02},

journal = {Nature Communications},

volume = {15},

number = {9482},

abstract = {Glycans, consisting of covalently linked sugar units, are a major class of biopolymers essential to all known living organisms. To better understand their biological functions and further applications in fields from biomedicine to materials science, detailed knowledge of their structure is essential. However, due to the extraordinary complexity and conformational flexibility of glycans, state-of-the-art glycan analysis methods often fail to provide structural information with atomic precision. Here, we combine electrospray deposition in ultra-high vacuum with non-contact atomic force microscopy and theoretical calculations to unravel the structure of β-cyclodextrin, a cyclic glucose oligomer, with atomic-scale detail. Our results, established on the single-molecule level, reveal the different adsorption geometries and conformations of β-cyclodextrin. The position of individual hydroxy groups and the location of the stabilizing intramolecular H-bonds are deduced from atomically resolved images, enabling the unambiguous assignment of the molecular structure and demonstrating the potential of the method for glycan analysis.},

note = {Glycans are structurally complex biomolecules and very challenging to analyse. Here the authors show atomically resolved imaging of β-cyclodextrins with non-contact atomic force microscopy, revealing the structure of individual glycans with atomic detail.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Chiral plasmonic-dielectric coupling enables strong near-infrared chiroptical responses from helicoidal core-shell nanoparticles},

author = {Xiali Lv and Yu Tian and Fengxia Wu and Xiaoxi Luan and Fenghua Li and Zhili Shen and Guobao Xu and Kun Liu and Wenxin Niu },

url = {https://www.nature.com/articles/s41467-024-53705-4.pdf},

doi = {10.1038/s41467-024-53705-4},

year  = {2024},

date = {2024-10-25},

urldate = {2024-10-25},

journal = {Nature Communications},

volume = {15},

number = {9234},

abstract = {Helicoid plasmonic nanoparticles with intrinsic chirality are an emerging class of artificial chiral materials with tailorable properties. The ability to extend their chiroplasmonic responses to the near-infrared (NIR) range is critically important for biomedical and nanophotonic applications, yet the rational design of such materials remains challenging. Herein, a strategy employing chiral plasmon-dielectric coupling is proposed to manipulate the chiroptical responses into the NIR region with high optical anisotropy. Through this strategy, the helicoid Au@Cu2O nanoparticles with structural chirality are designed and synthesized with tunable and enriched NIR chiroptical responses. Specially, a high optical anisotropy (g-factor) with a value of 0.35 is achieved in the NIR region, and multi-band chiroptical behaviors are observed. Spectral and electromagnetic simulations elucidate that strong coupling between chiroplasmonic core and chiral dielectric shell with high refractive index contributes to the rich and strong chiroptical responses, which are related to the interplay between various emerged and enhanced electric and magnetic multipolar resonance modes proved by multipole expansion analysis. Moreover, the helicoid Au@Cu2O nanoparticles display greater polarization rotation capability than the helicoid Au nanoparticles. This work offers mechanistic insights into chiral plasmon-dielectric coupling and suggests a general approach of creating NIR chiroplasmonic materials.},

note = {The rational design of chiroplasmonic nanomaterials with near-infrared (NIR) responses remains a challenge. Here, the authors propose a strategy utilizing chiral plasmonic-dielectric coupling to achieve strong chiroptical responses in the NIR region.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Design rules for catalysis in single-particle plasmonic nanogap reactors with precisely aligned molecular monolayers},

author = {Gyeongwon Kang and Shu Hu and Chenyang Guo and Rakesh Arul and Sarah M. Sibug-Torres and Jeremy J. Baumberg },

url = {https://www.nature.com/articles/s41467-024-53544-3.pdf},

doi = {10.1038/s41467-024-53544-3},

year  = {2024},

date = {2024-10-25},

urldate = {2024-10-25},

journal = {Nature Communications},

volume = {15},

pages = {9220},

abstract = {Plasmonic nanostructures can both drive and interrogate light-driven catalytic reactions. Sensitive detection of reaction pathways is achieved by confining optical fields near the active surface. However, effective control of the reaction kinetics remains a challenge to utilize nanostructure constructs as efficient chemical reactors. Here we present a nanoreactor construct exhibiting high catalytic and optical efficiencies, based on a nanoparticle-on-mirror (NPoM) platform. We observe and track pathways of the Pd-catalysed C-C coupling reaction of molecules within a set of nanogaps presenting different chemical surfaces. Atomic monolayer coatings of Pd on the different Au facets enable tuning of the reaction kinetics of surface-bound molecules. Systematic analysis shows the catalytic efficiency of NPoM-based nanoreactors greatly improves on platforms based on aggregated nanoparticles. More importantly, we show Pd monolayers on the nanoparticle or on the mirror play significantly different roles in the surface reaction kinetics. Our data provides clear evidence for catalytic dependencies on molecular configuration in well-defined nanostructures. Such nanoreactor constructs therefore yield clearer design rules for plasmonic catalysis.},

note = {Plasmonic nanostructures can drive light-driven catalytic reactions, but controlling reaction kinetics remains challenging. Here, the authors design plasmonic nanoreactors that enhance control of catalytic reactions, revealing distinct kinetics based on molecular configuration and monolayer placement.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In situ atomic observations of aggregation growth and evolution of penta-twinned gold nanocrystals},

author = {Miao Song and Dingri Zhang and Dan Leng and Jaewon Lee and Ziang Yang and Jiaxuan Chen and Dan Li and Lei Wang and Gang Zhou and Rui Yang and Kechao Zhou },

url = {https://www.nature.com/articles/s41467-024-53501-0.pdf},

doi = {10.1038/s41467-024-53501-0},

year  = {2024},

date = {2024-10-25},

journal = {Nature Communications},

volume = {15},

number = {9217},

abstract = {The twin boundaries and inherent lattice strain of five-fold twin (5-FT) structures offer a promising and innovative approach to tune nanocrystal configurations and properties, enriching nanomaterial performance. However, a comprehensive understanding of the nonclassical growth models governing 5-FT nanocrystals remains elusive, largely due to the constraints of their small thermodynamically stable size and complex twin configurations. Here, we conducted in situ investigations to elucidate the atomic-scale mechanisms driving size-dependent and twin configuration-related aggregation phenomena between 5-FT and other nanoparticles at the atomic scale. Our results reveal that surface diffusion significantly shapes the morphology of aggregated nanoparticles, promoting the symmetrical formation of 5-FT, especially in smaller nanoparticles. Moreover, the inherent structural characteristics of 5-FT mitigate the dominance of surface diffusion in its morphological evolution, retarding the aggregation evolution process and fostering intricate twin structures. These findings contribute to advancing our capacity to manipulate the configuration of twinned particles, enabling more predictable synthesis of functional nanomaterials for advanced engineering applications.},

note = {The mechanisms underlying the nonclassical growth of penta-twinned gold nanocrystals remain unclear. Here, the authors elucidate the atomic-level processes that drive size-dependent and twin configuration-related aggregation phenomena.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {On-chip phonon-enhanced IR near-field detection of molecular vibrations},

author = {Andrei Bylinkin and Sebastián Castilla and Tetiana M. Slipchenko and Kateryna Domina and Francesco Calavalle and Varun-Varma Pusapati and Marta Autore and Fèlix Casanova and Luis E. Hueso and Luis Martín-Moreno and Alexey Y. Nikitin and Frank H. L. Koppens and Rainer Hillenbrand },

url = {https://www.nature.com/articles/s41467-024-53182-9.pdf},

doi = {10.1038/s41467-024-53182-9},

year  = {2024},

date = {2024-10-16},

journal = {Nature Communications},

volume = {15},

number = {8907},

abstract = {Phonon polaritons – quasiparticles formed by strong coupling of infrared (IR) light with lattice vibrations in polar materials – can be utilized for surface-enhanced infrared absorption (SEIRA) spectroscopy and even for vibrational strong coupling with nanoscale amounts of molecules. Here, we introduce and demonstrate a compact on-chip phononic SEIRA spectroscopy platform, which is based on an h-BN/graphene/h-BN heterostructure on top of a metal split-gate creating a p-n junction in graphene. The metal split-gate concentrates the incident light and launches hyperbolic phonon polaritons (HPhPs) in the heterostructure, which serves simultaneously as SEIRA substrate and room-temperature infrared detector. When thin organic layers are deposited directly on top of the heterostructure, we observe a photocurrent encoding the layer’s molecular vibrational fingerprint, which is strongly enhanced compared to that observed in standard far-field absorption spectroscopy. A detailed theoretical analysis supports our results, further predicting an additional sensitivity enhancement as the molecular layers approach deep subwavelength scales. Future on-chip integration of infrared light sources such as quantum cascade lasers or even electrical generation of the HPhPs could lead to fully on-chip phononic SEIRA sensors for molecular and gas sensing.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Electrical monitoring of single-event protonation dynamics at the solid-liquid interface and its regulation by external mechanical forces},

author = {Cong Zhao and Jiazheng Diao and Zhao Liu and Jie Hao and Suhang He and Shaojia Li and Xingxing Li and Guangwu Li and Qiang Fu and Chuancheng Jia and Xuefeng Guo },

url = {https://www.nature.com/articles/s41467-024-53179-4.pdf},

doi = {10.1038/s41467-024-53179-4},

year  = {2024},

date = {2024-10-13},

urldate = {2024-10-13},

journal = {Nature Communications},

volume = {15},

number = {8835},

abstract = {Detecting chemical reaction dynamics at solid-liquid interfaces is important for understanding heterogeneous reactions. However, there is a lack of exploration of interface reaction dynamics from the single-molecule perspective, which can reveal the intrinsic reaction mechanism underlying ensemble experiments. Here, single-event protonation reaction dynamics at a solid-liquid interface are studied in-situ using single-molecule junctions. Molecules with amino terminal groups are used to construct single-molecule junctions. An interfacial cationic state present after protonation is discovered. Real-time electrical measurements are used to monitor the reversible reaction between protonated and deprotonated states, thereby revealing the interfacial reaction mechanism through dynamic analysis. The protonation reaction rate constant has a linear positive correlation with proton concentration, whereas the deprotonation reaction rate constant has a linear negative correlation. In addition, external mechanical forces can effectively regulate the protonation reaction process. This work provides a single-molecule perspective for exploring interface science, which will contribute to the development of heterogeneous catalysis and electrochemistry.},

note = {Direct detection of chemical reactions at solid-liquid interfaces is important for a more complete understanding of interfacial effects. Here, the authors study single-event interfacial protonation reaction dynamics by single-molecule junctions and thereby identify an interfacial cationic state.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Nanopore ion sources deliver individual ions of amino acids and peptides directly into high vacuum},

author = {Nicholas Drachman and Mathilde Lepoitevin and Hannah Szapary and Benjamin Wiener and William Maulbetsch and Derek Stein },

url = {https://www.nature.com/articles/s41467-024-51455-x.pdf},

doi = {10.1038/s41467-024-51455-x},

year  = {2024},

date = {2024-09-05},

urldate = {2024-09-05},

journal = {Nature Communications},

volume = {15},

number = {7709},

abstract = {Electrospray ionization is widely used to generate vapor phase ions for analysis by mass spectrometry in proteomics research. However, only a small fraction of the analyte enters the mass spectrometer due to losses that are fundamentally linked to the use of a background gas to stimulate the generation of ions from electrosprayed droplets. Here we report a nanopore ion source that delivers ions directly into high vacuum from aqueous solutions. The ion source comprises a pulled quartz pipette with a sub-100 nm opening. Ions escape an electrified meniscus by ion evaporation and travel along collisionless trajectories to the ion detector. We measure mass spectra of 16 different amino acid ions, post-translationally modified variants of glutathione, and the peptide angiotensin II, showing that these analytes can be emitted as desolvated ions. The emitted current is composed of ions rather than charged droplets, and more than 90% of the current can be recovered in a distant collector.},

note = {Electrospray ionization loses most ions upon transfer into high vacuum in a mass spectrometer. Here, the authors present a nanopore ion source that emits ions directly into vacuum from aqueous solutions, achieving an ion transmission efficiency of over 90%.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Three-dimensional atomic insights into the metal-oxide interface in Zr-ZrO2 nanoparticles},

author = {Yao Zhang and Zezhou Li and Xing Tong and Zhiheng Xie and Siwei Huang and Yue-E Zhang and Hai-Bo Ke and Wei-Hua Wang and Jihan Zhou },

url = {https://www.nature.com/articles/s41467-024-52026-w.pdf},

doi = {10.1038/s41467-024-52026-w},

year  = {2024},

date = {2024-09-02},

journal = {Nature Communications},

volume = {15},

number = {7624},

abstract = {Metal-oxide interfaces with poor coherency have specific properties comparing to bulk materials and offer broad applications in heterogeneous catalysis, battery, and electronics. However, current understanding of the three-dimensional (3D) atomic metal-oxide interfaces remains limited because of their inherent structural complexity and the limitations of conventional two-dimensional imaging techniques. Here, we determine the 3D atomic structure of metal-oxide interfaces in zirconium-zirconia nanoparticles using atomic-resolution electron tomography. We quantitatively analyze the atomic concentration and the degree of oxidation, and find the coherency and translational symmetry of the interfaces are broken. Atoms at the interface have low structural ordering, low coordination, and elongated bond length. Moreover, we observe porous structures such as Zr vacancies and nano-pores, and investigate their distribution. Our findings provide a clear 3D atomic picture of metal-oxide interface with direct experimental evidence. We anticipate this work could encourage future studies on fundamental problems of oxides, such as interfacial structures in semiconductor and atomic motion during oxidation process.},

note = {A detailed understanding of metal-oxide interfaces is essential for uncovering their intrinsic properties. Here, the authors investigate the 3D atomic structure of metal-oxide interfaces in Zr-ZrO2 nanoparticles using atomic-resolution electron tomography.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In-situ atomic tracking of intermetallic compound formation during thermal annealing},

author = {Xiao Han and Yanan Zhou and Xiaolin Tai and Geng Wu and Cai Chen and Xun Hong and Lei Tong and Fangfang Xu and Hai-Wei Liang and Yue Lin },

url = {https://www.nature.com/articles/s41467-024-51541-0.pdf},

doi = {10.1038/s41467-024-51541-0},

year  = {2024},

date = {2024-08-22},

journal = {Nature Communications},

volume = {15},

number = {7200},

abstract = {Intermetallic compounds (IMCs) with ordered atomic structure have gained great attention as nanocatalysts for its enhanced activity and stability. Although the reliance of IMC preparation on high-temperature annealing is well known, a comprehensive understanding of the formation mechanisms of IMCs in this process is currently lacking. Here, we employ aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM) to track the formation process of IMCs on carbon supports during in-situ annealing, by taking PtFe as a case study within an industry-relevant impregnation synthesis framework. We directly discern five different stages at the atomic level: initial atomic precursors; Pt cluster formation; Pt-Fe disordered alloying; structurally ordered Pt3Fe formation, and final Pt3Fe-PtFe IMC conversion. In particular, we find that the crucial role of high-temperature annealing resides in facilitating the diffusion of Fe towards Pt, enabling the creation of alloys with the targeted stoichiometric ratio, which in turn provides the thermodynamic driving force for the disorder-to-order transition.},

note = {The mechanisms of intermetallic compound (IMC) formation during annealing are poorly understood. Here, the authors identify five stages of PtFe-IMC formation at the atomic level using in-situ STEM, emphasizing the role of high temperature in achieving the targeted stoichiometric ratio.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Interplay of kernel shape and surface structure for NIR luminescence in atomically precise gold nanorods},

author = {Xian-Kai Wan and Xu-Shuang Han and Zong-Jie Guan and Wan-Qi Shi and Jiao-Jiao Li and Quan-Ming Wang },

url = {https://www.nature.com/articles/s41467-024-51642-w.pdf},

doi = {10.1038/s41467-024-51642-w},

year  = {2024},

date = {2024-08-22},

journal = {Nature Communications},

volume = {15},

number = {7214},

abstract = {It is challenging to attain strong near-infrared (NIR) emissive gold nanoclusters. Here we show a rod-shaped cluster with the composition of [Au28(p-MBT)14(Hdppa)3](SO3CF3)2 (1 for short, Hdppa is N,N-bis(diphenylphosphino)amine, p-MBT is 4-methylbenzenethiolate) has been synthesized. Single crystal X-ray structural analysis reveals that it has a rod-like face-centered cubic (fcc) Au22 kernel built from two interpenetrating bicapped cuboctahedral Au15 units. 1 features NIR luminescence with an emission maximum at 920 nm, and the photoluminescence quantum yield (PLQY) is 12%, which is 30-fold of [Au21(m-MBT)12(Hdppa)2]SO3CF3 (2, m-MBT is 3-methylbenzenethiolate) with a similar composition and 60-fold of Au30S(S‑t‑Bu)18 with a similar structure. time-dependent DFT(TDDFT)calculations reveal that the luminescence of 1 is associated with the Au22 kernel. The small Stokes shift of 1 indicates that it has a very small excited state structural distortion, leading to high radiative decay rate (kr) probability. The emission of cluster 1 is a mixture of phosphorescence and thermally activated delayed fluorescence(TADF), and the enhancement of the NIR emission is mainly due to the promotion of kr rather than the inhibition of knr. This work demonstrates that the metal kernel and the surface structure are both very important for cluster-based NIR luminescence materials.},

note = {Gold nanoclusters with strong emissions in the near-infrared are challenging to attain. Here, the authors show that for rod-shaped nanoclusters, both the shape of the kernel and the rigid surface structure are important to increase the NIR emissions.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Nanocrystalline copper for direct copper-to-copper bonding with improved cross-interface formation at low thermal budget},

author = {Chuan He and Jingzhuo Zhou and Rui Zhou and Cong Chen and Siyi Jing and Kaiyu Mu and Yu-Ting Huang and Chih-Chun Chung and Sheng-Jye Cherng and Yang Lu and King-Ning Tu and Shien-Ping Feng },

url = {https://www.nature.com/articles/s41467-024-51510-7.pdf},

doi = {10.1038/s41467-024-51510-7},

year  = {2024},

date = {2024-08-17},

journal = {Nature Communications},

volume = {15},

number = {7095},

abstract = {Direct copper-to-copper (Cu-Cu) bonding is a promising technology for advanced electronic packaging. Nanocrystalline (NC) Cu receives increasing attention due to its unique ability to promote grain growth across the bonding interface. However, achieving sufficient grain growth still requires a high thermal budget. This study explores how reducing grain size and controlling impurity concentration in NC Cu leads to substantial grain growth at low temperatures. The fabricated NC Cu has a uniform nanograin size of around 50 nm and a low impurity level of 300 ppm. To prevent ungrown NC and void formation caused by impurity aggregation, we propose a double-layer (DL) structure comprising a normal coarse-grained (CG) layer underneath the NC layer. The CG layer, with a grain size of 1 μm and an impurity level of 3 ppm, acts as a sink, facilitating impurity diffusion from the NC layer to the CG layer. Thanks to sufficient grain growth throughout the entire NC layer, cross-interface Cu-Cu bonding becomes possible under a low thermal budget, either at 100 °C for 60 min or at 200 °C for only 5 min.},

note = {Direct copper-to-copper bonding is crucial for advanced electronic packaging. Here, the authors demonstrate Cu-Cu bonding with low thermal budget using nanocrystalline Cu with a double-layer structure.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Chiral 3D structures through multi-dimensional transfer printing of multilayer quantum dot patterns},

author = {Geon Yeong Kim and Shinho Kim and Ki Hyun Park and Hanhwi Jang and Moohyun Kim and Tae Won Nam and Kyeong Min Song and Hongjoo Shin and Yemin Park and Yeongin Cho and Jihyeon Yeom and Min-Jae Choi and Min Seok Jang and Yeon Sik Jung },

url = {https://www.nature.com/articles/s41467-024-51179-y.pdf},

doi = {10.1038/s41467-024-51179-y},

year  = {2024},

date = {2024-08-14},

journal = {Nature Communications},

volume = {15},

number = {6996},

abstract = {Three-dimensional optical nanostructures have garnered significant interest in photonics due to their extraordinary capabilities to manipulate the amplitude, phase, and polarization states of light. However, achieving complex three-dimensional optical nanostructures with bottom-up fabrication has remained challenging, despite its nanoscale precision and cost-effectiveness, mainly due to inherent limitations in structural controllability. Here, we report the optical characteristics of intricate two- and three-dimensional nanoarchitectures made of colloidal quantum dots fabricated with multi-dimensional transfer printing. Our customizable fabrication platform, directed by tailored interface polarity, enables flexible geometric control over a variety of one-, two-, and three-dimensional quantum dot architectures, achieving tunable and advanced optical features. For example, we demonstrate a two-dimensional quantum dot nanomesh with tuned subwavelength square perforations designed by finite-difference time-domain calculations, achieving an 8-fold enhanced photoluminescence due to the maximized optical resonance. Furthermore, a three-dimensional quantum dot chiral structure is also created via asymmetric stacking of one-dimensional quantum dot layers, realizing a pronounced circular dichroism intensity exceeding 20°.},

note = {3D photonic nanostructures can manipulate the amplitude, phase, and polarization of light, but their bottom-up fabrication is hindered by limited structural control. Here, the authors present chiral 3D structures through multi-dimensional transfer printing of multilayer quantum dot patterns.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Nacre-like surface nanolaminates enhance fatigue resistance of pure titanium},

author = {Yong Zhang and Chenyun He and Qin Yu and Xiao Li and Xiaogang Wang and Yin Zhang and Ji Wang and Chao Jiang and Yunfei Jia and Xian-Cheng Zhang and Binhan Sun and Robert O. Ritchie and Shan-Tung Tu },

url = {https://www.nature.com/articles/s41467-024-51423-5.pdf},

doi = {10.1038/s41467-024-51423-5},

year  = {2024},

date = {2024-08-13},

journal = {Nature Communications},

volume = {15},

number = {6917},

abstract = {Fatigue failure is invariably the most crucial failure mode for metallic structural components. Most microstructural strategies for enhancing fatigue resistance are effective in suppressing either crack initiation or propagation, but often do not work for both synergistically. Here, we demonstrate that this challenge can be overcome by architecting a gradient structure featuring a surface layer of nacre-like nanolaminates followed by multi-variant twinned structure in pure titanium. The polarized accommodation of highly regulated grain boundaries in the nanolaminated layer to cyclic loading enhances the structural stability against lamellar thickening and microstructure softening, thereby delaying surface roughening and thus crack nucleation. The decohesion of the nanolaminated grains along horizonal high-angle grain boundaries gives rise to an extraordinarily high frequency (≈1.7 × 103 times per mm) of fatigue crack deflection, effectively reducing fatigue crack propagation rate (by 2 orders of magnitude lower than the homogeneous coarse-grained counterpart). These intriguing features of the surface nanolaminates, along with the various toughening mechanisms activated in the subsurface twinned structure, result in a fatigue resistance that significantly exceeds those of the homogeneous and gradient structures with equiaxed grains. Our work on architecting the surface nanolaminates in gradient structure provides a scalable and sustainable strategy for designing more fatigue-resistant alloys.},

note = {Most strategies to improve fatigue resistance address either crack initiation or growth. Here, the authors design a gradient-structured Ti with nacre-like surface nanolaminates that increase fatigue performance by suppressing both stages of cracking},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {An order-disorder core-shell strategy for enhanced work-hardening capability and ductility in nanostructured alloys},

author = {Fenghui Duan and Qian Li and Zhihao Jiang and Lin Zhou and Junhua Luan and Zheling Shen and Weihua Zhou and Shiyuan Zhang and Jie Pan and Xin Zhou and Tao Yang and Jian Lu },

url = {https://www.nature.com/articles/s41467-024-50984-9.pdf},

doi = {10.1038/s41467-024-50984-9},

year  = {2024},

date = {2024-08-09},

journal = {Nature Communications},

volume = {15},

number = {6832},

abstract = {Nanocrystalline metallic materials have the merit of high strength but usually suffer from poor ductility and rapid grain coarsening, limiting their practical application. Here, we introduce a core-shell nanostructure in a multicomponent alloy to address these challenges simultaneously, achieving a high tensile strength of 2.65 GPa, a large uniform elongation of 17%, and a high thermal stability of 1173 K. Our strategy relies on an ordered superlattice structure that excels in dislocation accumulation, encased by a ≈3 nm disordered face-centered-cubic nanolayer acting as dislocation sources. The ordered superlattice with high anti-phase boundary energy retards dislocation motions, promoting their interaction and storage within the nanograins. The disordered interfacial nanolayer promotes dislocation emission and effectively accommodates the plastic strain at grain boundaries, preventing intergranular cracking. Consequently, the order-disorder core-shell nanostructure exhibits enhanced work-hardening capability and large ductility. Moreover, such core-shell nanostructure exhibits high coarsening resistance at elevated temperatures, enabling it high thermal stability. Such a design strategy holds promise for developing high-performance materials.},

note = {Nanocrystalline metallic materials have the merit of high strength, but usually suffer from poor ductility and rapid grain coarsening. Here, the authors develop a nanocrystalline core-shell alloy to overcome these challenges.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Continuous polyamorphic transition in high-entropy metallic glass},

author = {Yihuan Cao and Ming Yang and Qing Du and Fu-Kuo Chiang and Yingjie Zhang and Shi-Wei Chen and Yubin Ke and Hongbo Lou and Fei Zhang and Yuan Wu and Hui Wang and Suihe Jiang and Xiaobin Zhang and Qiaoshi Zeng and Xiongjun Liu and Zhaoping Lu },

url = {https://www.nature.com/articles/s41467-024-51080-8.pdf},

doi = {10.1038/s41467-024-51080-8},

year  = {2024},

date = {2024-08-07},

journal = {Nature Communications},

number = {6702},

abstract = {Polyamorphic transition (PT) is a compelling and pivotal physical phenomenon in the field of glass and materials science. Understanding this transition is of scientific and technological significance, as it offers an important pathway for effectively tuning the structure and property of glasses. In contrast to the PT observed in conventional metallic glasses (MGs), which typically exhibit a pronounced first-order nature, herein we report a continuous PT (CPT) without first-order characteristics in high-entropy MGs (HEMGs) upon heating. This CPT behavior is featured by the continuous structural evolution at the atomic level and an increasing chemical concentration gradient with temperature, but no abrupt reduction in volume and energy. The continuous transformation is associated with the absence of local favorable structures and chemical heterogeneity caused by the high configurational entropy, which limits the distance and frequency of atomic diffusion. As a result of the CPT, numerous glass states can be generated, which provides an opportunity to understand the nature, atomic packing, formability, and properties of MGs. Moreover, this discovery highlights the implication of configurational entropy in exploring polyamorphic glasses with an identical composition but highly tunable structures and properties.},

note = {The understanding of polyamorphic transitions is of scientific and technological importance. Here, the authors report a continuous polyamorphic transition without first-order transition characteristics in high-entropy metallic glasses.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Restructuring dynamics of surface species in bimetallic nanoparticles probed by modulation excitation spectroscopy},

author = {Prahlad K. Routh and Evgeniy Redekop and Sebastian Prodinger and Jessi E. S. van der Hoeven and Kang Rui Garrick Lim and Joanna Aizenberg and Maarten Nachtegaal and Adam H. Clark and Anatoly I. Frenkel },

url = {https://www.nature.com/articles/s41467-024-51068-4.pdf},

doi = {10.1038/s41467-024-51068-4},

year  = {2024},

date = {2024-08-07},

journal = {Nature Communications},

volume = {15},

number = {6734},

abstract = {Restructuring of metal components on bimetallic nanoparticle surfaces in response to the changes in reactive environment is a ubiquitous phenomenon whose potential for the design of tunable catalysts is underexplored. The main challenge is the lack of knowledge of the structure, composition, and evolution of species on the nanoparticle surfaces during reaction. We apply a modulation excitation approach to the X-ray absorption spectroscopy of the 30 atomic % Pd in Au supported nanocatalysts via the gas (H2 and O2) concentration modulation. For interpreting restructuring kinetics, we correlate the phase-sensitive detection with the time-domain analysis aided by a denoising algorithm. Here we show that the surface and near-surface species such as Pd oxides and atomically dispersed Pd restructured periodically, featuring different time delays. We propose a model that Pd oxide formation is preceded by the build-up of Pd regions caused by oxygen-driven segregation of Pd atoms towards the surface. During the H2 pulse, rapid reduction and dissolution of Pd follows an induction period which we attribute to H2 dissociation. Periodic perturbations of nanocatalysts by gases can, therefore, enable variations in the stoichiometry of the surface and near-surface oxides and dynamically tune the degree of oxidation/reduction of metals at/near the catalyst surface.},

note = {Nanocatalysts can restructure during reactions. Here, the authors dynamically varied the stoichiometry of the surface species in 30 % Pd-in-Au nanoparticles by modulating H2 and O2 gases and quantified the formation kinetics of Pd regions and oxides.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Capillary trapping of various nanomaterials on additively manufactured scaffolds for 3D micro-/nanofabrication},

author = {Xianglong Lyu and Zhiqiang Zheng and Anitha Shiva and Mertcan Han and Cem Balda Dayan and Mingchao Zhang and Metin Sitti },

url = {https://www.nature.com/articles/s41467-024-51086-2.pdf},

doi = {10.1038/s41467-024-51086-2},

year  = {2024},

date = {2024-08-06},

journal = {Nature Communications},

volume = {15},

number = {6693},

abstract = {High-precision additive manufacturing technologies, such as two-photon polymerization, are mainly limited to photo-curable polymers and currently lacks the possibility to produce multimaterial components. Herein, we report a physically bottom-up assembly strategy that leverages capillary force to trap various nanomaterials and assemble them onto three-dimensional (3D) microscaffolds. This capillary-trapping strategy enables precise and uniform assembly of nanomaterials into versatile 3D microstructures with high uniformity and mass loading. Our approach applies to diverse materials irrespective of their physiochemical properties, including polymers, metals, metal oxides, and others. It can integrate at least four different material types into a single 3D microstructure in a sequential, layer-by-layer manner, opening immense possibilities for tailored functionalities on demand. Furthermore, the 3D microscaffolds are removable, facilitating the creation of pure material-based 3D microstructures. This universal 3D micro-/nanofabrication technique with various nanomaterials enables the creation of advanced miniature devices with potential applications in multifunctional microrobots and smart micromachines.},

note = {High-precision 3D micro-/nanofabrication technologies such as two-photon polymerization are limited to photocurable polymers. Here, the authors report a “capillary-trapping” strategy to fabricate various 3D micro-scaffolds composed of different nanomaterials.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Accelerated proton dissociation in an excited state induces superacidic microenvironments around graphene quantum dots},

author = {Yongqiang Li and Siwei Yang and Wancheng Bao and Quan Tao and Xiuyun Jiang and Jipeng Li and Peng He and Gang Wang and Kai Qi and Hui Dong and Guqiao Ding and Xiaoming Xie },

url = {https://www.nature.com/articles/s41467-024-50982-x.pdf},

doi = {10.1038/s41467-024-50982-x},

year  = {2024},

date = {2024-08-05},

journal = {Nature Communications},

volume = {15},

number = {6634},

abstract = {Investigating proton transport at the interface in an excited state facilitates the mechanistic investigation and utilization of nanomaterials. However, there is a lack of suitable tools for in-situ and interfacial analysis. Here we addresses this gap by in-situ observing the proton transport of graphene quantum dots (GQDs) in an excited state through reduction of magnetic resonance relaxation time. Experimental results, utilizing 0.1 mT ultra-low-field nuclear magnetic resonance relaxometry compatible with a light source, reveal the light-induced proton dissociation and acidity of GQDs’ microenvironment in the excited state (Hammett acidity function: –13.40). Theoretical calculations demonstrate significant acidity enhancement in –OH functionalized GQDs with light induction (pKa* = –4.62, stronger than that of H2SO4). Simulations highlight the contributions of edge and phenolic –OH groups to proton dissociation. The light-induced superacidic microenvironment of GQDs benefits functionalization and improves the catalytic performances of GQDs. Importantly, this work advances the understanding of interfacial properties of light-induced sp2–sp3 carbon nanostructure and provides a valuable tool for exploring catalyst interfaces in photocatalysis.},

note = {Understanding interfacial proton transport in an excited state is crucial for catalytic and diagnostic applications of nanomaterials. Here, the authors combine ultra-low-field NMR relaxometry with a light source to study the light-induced proton dissociation of graphene quantum dots.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Probing charge redistribution at the interface of self-assembled cyclo-P5 pentamers on Ag(111)},

author = {Outhmane Chahib and Yuling Yin and Jung-Ching Liu and Chao Li and Thilo Glatzel and Feng Ding and Qinghong Yuan and Ernst Meyer and Rémy Pawlak },

url = {https://www.nature.com/articles/s41467-024-50862-4.pdf},

doi = {10.1038/s41467-024-50862-4},

year  = {2024},

date = {2024-08-02},

urldate = {2024-08-02},

journal = {Nature Communications},

volume = {15},

number = {6542},

abstract = {Phosphorus pentamers (cyclo-P5) are unstable in nature but can be synthesized at the Ag(111) surface. Unlike monolayer black phosphorous, little is known about their electronic properties when in contact with metal electrodes, although this is crucial for future applications. Here, we characterize the atomic structure of cyclo-P5 assembled on Ag(111) using atomic force microscopy with functionalized tips and density functional theory. Combining force and tunneling spectroscopy, we find that a strong charge transfer induces an inward dipole moment at the cyclo-P5/Ag interface as well as the formation of an interface state. We probe the image potential states by field-effect resonant tunneling and quantify the increase of the local change of work function of 0.46 eV at the cyclo-P5 assembly. Our experimental approach suggest that the cyclo-P5/Ag interface has the characteristic ingredients of a p-type semiconductor-metal Schottky junction with potential applications in field-effect transistors, diodes, or solar cells.},

note = {Although unstable in nature, phosphorus pentamers (cyclo-P5) can be synthesized on a silver surface. Here, the authors use scanning probe microscopy to probe charge redistribution at the P5/Ag interface offering potential applications in transistors or solar cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Quantifying the conductivity of a single polyene chain by lifting with an STM tip},

author = {Sifan You and Cuiju Yu and Yixuan Gao and Xuechao Li and Guyue Peng and Kaifeng Niu and Jiahao Xi and Chaojie Xu and Shixuan Du and Xingxing Li and Jinlong Yang and Lifeng Chi },

url = {https://www.nature.com/articles/s41467-024-50915-8.pdf},

doi = {10.1038/s41467-024-50915-8},

year  = {2024},

date = {2024-08-01},

urldate = {2024-08-01},

journal = {Nature Communications},

volume = {15},

number = {6475},

abstract = {Conjugated polymers are promising candidates for molecular wires in nanoelectronics, with flexibility in mechanics, stability in chemistry and variety in electrical conductivity. Polyene, as a segment of polyacetylene, is a typical conjugated polymer with straightforward structure and wide-range adjustable conductance. To obtain atomic scale understanding of charge transfer in polyene, we have measured the conductance of a single polyene-based molecular chain via lifting it up with scanning tunneling microscopy tip. Different from semiconducting characters in pristine polyene (polyacetylene), high conductance and low decay constant are obtained, along with an electronic state around Fermi level and characteristic vibrational mode. These observed phenomena result from pinned molecular orbital owing to molecule-electrode coupling at the interface, and weakened bond length alternation due to electron-phonon coupling inside single molecular chain. Our findings emphasize the interfacial characteristics in molecular junctions and promising properties of polyene, with single molecular conductance as a vital tool for bringing insights into the design and construction of nanodevices.},

note = {Polyene is a segment of polyacetylene, a conductive polymer. Here, the authors measured the conductance of single molecular chain of trans-polyene and found a high conductivity and low decay constant, attributed to the alignment of the energy levels.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Quantitative 3D structural analysis of small colloidal assemblies under native conditions by liquid-cell fast electron tomography},

author = {Daniel Arenas Esteban and Da Wang and Ajinkya Kadu and Noa Olluyn and Ana Sánchez-Iglesias and Alejandro Gomez-Perez and Jesús González-Casablanca and Stavros Nicolopoulos and Luis M. Liz-Marzán and Sara Bals },

url = {https://www.nature.com/articles/s41467-024-50652-y.pdf},

doi = {10.1038/s41467-024-50652-y},

year  = {2024},

date = {2024-07-30},

urldate = {2024-07-30},

journal = {Nature Communications},

volume = {15},

number = {6399},

abstract = {Electron tomography has become a commonly used tool to investigate the three-dimensional (3D) structure of nanomaterials, including colloidal nanoparticle assemblies. However, electron microscopy is typically done under high-vacuum conditions, requiring sample preparation for assemblies obtained by wet colloid chemistry methods. This involves solvent evaporation and deposition on a solid support, which consistently alters the nanoparticle organization. Here, we suggest using electron tomography to study nanoparticle assemblies in their original colloidal liquid environment. To address the challenges related to electron tomography in liquid, we devise a method that combines fast data acquisition in a commercial liquid-cell with a dedicated alignment and reconstruction workflow. We present the advantages of this methodology in accurately characterizing two different systems. 3D reconstructions of assemblies comprising polystyrene-capped Au nanoparticles encapsulated in polymeric shells reveal less compact and more distorted configurations for experiments performed in a liquid medium compared to their dried counterparts. A similar expansion can be observed in quantitative analysis of the surface-to-surface distances of self-assembled Au nanorods in water rather than in a vacuum, in agreement with bulk measurements. This study, therefore, emphasizes the importance of developing high-resolution characterization tools that preserve the native environment of colloidal nanostructures.},

note = {Drying force-induced deformation complicates the characterization of the 3D structure of colloidal assemblies. Here, the authors develop a liquid electron tomography method for unravelling the 3D structures of small colloidal assemblies under native conditions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Slow vibrational relaxation drives ultrafast formation of photoexcited polaron pair states in glycolated conjugated polymers},

author = {Katia Pagano and Jin Gwan Kim and Joel Luke and Ellasia Tan and Katherine Stewart and Igor V. Sazanovich and Gabriel Karras and Hristo Ivov Gonev and Adam V. Marsh and Na Yeong Kim and Sooncheol Kwon and Young Yong Kim and M. Isabel Alonso and Bernhard Dörling and Mariano Campoy-Quiles and Anthony W. Parker and Tracey M. Clarke and Yun-Hi Kim and Ji-Seon Kim },

url = {https://www.nature.com/articles/s41467-024-50530-7.pdf},

doi = {10.1038/s41467-024-50530-7},

year  = {2024},

date = {2024-07-22},

urldate = {2024-07-22},

journal = {Nature Communications},

volume = {15},

number = {6153},

abstract = {Glycol sidechains are often used to enhance the performance of organic photoconversion and electrochemical devices. Herein, we study their effects on electronic states and electronic properties. We find that polymer glycolation not only induces more disordered packing, but also results in a higher reorganisation energy due to more localised π-electron density. Transient absorption spectroscopy and femtosecond stimulated Raman spectroscopy are utilised to monitor the structural relaxation dynamics coupled to the excited state formation upon photoexcitation. Singlet excitons are initially formed, followed by polaron pair formation. The associated structural relaxation slows down in glycolated polymers (5 ps vs. 1.25 ps for alkylated), consistent with larger reorganisation energy. This slower vibrational relaxation is found to drive ultrafast formation of the polaron pair state (5 ps vs. 10 ps for alkylated). These results provide key experimental evidence demonstrating the impact of molecular structure on electronic state formation driven by strong vibrational coupling.},

note = {Glycol sidechains are often used to enhance the performance of organic photoconversion and electrochemical devices. Here, the authors provide photophysical insight into the role of glycol sidechains for the formation of polaron pairs induced by strong vibrational coupling.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Constrained patterning of orientated metal chalcogenide nanowires and their growth mechanism},

author = {Qishuo Yang and Yun-Peng Wang and Xiao-Lei Shi and XingXing Li and Erding Zhao and Zhi-Gang Chen and Jin Zou and Kai Leng and Yongqing Cai and Liang Zhu and Sokrates T. Pantelides and Junhao Lin },

url = {https://www.nature.com/articles/s41467-024-50525-4.pdf},

doi = {10.1038/s41467-024-50525-4},

year  = {2024},

date = {2024-07-18},

urldate = {2024-07-18},

journal = {Nature Communications},

volume = {15},

number = {6074},

abstract = {One-dimensional metallic transition-metal chalcogenide nanowires (TMC-NWs) hold promise for interconnecting devices built on two-dimensional (2D) transition-metal dichalcogenides, but only isotropic growth has so far been demonstrated. Here we show the direct patterning of highly oriented Mo6Te6 NWs in 2D molybdenum ditelluride (MoTe2) using graphite as confined encapsulation layers under external stimuli. The atomic structural transition is studied through in-situ electrical biasing the fabricated heterostructure in a scanning transmission electron microscope. Atomic resolution high-angle annular dark-field STEM images reveal that the conversion of Mo6Te6 NWs from MoTe2 occurs only along specific directions. Combined with first-principles calculations, we attribute the oriented growth to the local Joule-heating induced by electrical bias near the interface of the graphite-MoTe2 heterostructure and the confinement effect generated by graphite. Using the same strategy, we fabricate oriented NWs confined in graphite as lateral contact electrodes in the 2H-MoTe2 FET, achieving a low Schottky barrier of 11.5 meV, and low contact resistance of 43.7 Ω µm at the metal-NW interface. Our work introduces possible approaches to fabricate oriented NWs for interconnections in flexible 2D nanoelectronics through direct metal phase patterning.},

note = {Nanowires made of transition metal chalcogenides are promising as connecting elements in devices, but so far only isotropic growth is feasible. Here, the authors regulate the growth orientation of nanowires by introducing external stimuli into graphite-confined MoTe2 heterostructures.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Wide-energy programmable microwave plasma-ionization for high-coverage mass spectrometry analysis},

author = {Fengjian Chu and Gaosheng Zhao and Wei Wei and Nazifi Sani Shuaibu and Hongru Feng and Yuanjiang Pan and Xiaozhi Wang },

url = {https://www.nature.com/articles/s41467-024-50322-z.pdf},

doi = {10.1038/s41467-024-50322-z},

year  = {2024},

date = {2024-07-18},

urldate = {2024-07-18},

journal = {Nature Communications},

volume = {15},

number = {6075},

abstract = {Although numerous ambient ionization mass spectroscopy technologies have been developed over the past 20 years to address diverse analytical circumstances, a single-ion source technique that can handle all analyte types is still lacking. Here, a wide-energy programmable microwave plasma-ionization mass spectrometry (WPMPI-MS) system is presented, through which MS analysis can achieve high coverage of substances with various characteristics by digitally regulating the microwave energy. In addition, ionization energy can be rapidly scanned using programmable waveforms, enabling the simultaneous detection of biomolecules, heavy metals, non-polar molecules, etc., in seconds. WPMPI-MS performs well in analyzing real samples, rapidly analyzing nine toxicological standards in one drop of serum, and demonstrating good quantification and liquid chromatography coupling capability. The WPMPI-MS has also been used to detect soil extracts, solid pharmaceuticals, and landfill leachate, further demonstrating its robust analytical capabilities for real samples. The prospective uses of the technology in biological and chemical analysis are extensive, and it is anticipated to emerge as a viable alternative to commercially available ion sources.},

note = {Ion source technology in mass spectrometry still has limitations in analyte coverage. Here, the authors present a wide-energy programmable microwave plasma ionization mass spectrometry system that enables MS analysis with high coverage.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Diameter-dependent phase selectivity in 1D-confined tungsten phosphides},

author = {Gangtae Jin and Christian D. Multunas and James L. Hart and Mehrdad T. Kiani and Nghiep Khoan Duong and Quynh P. Sam and Han Wang and Yeryun Cheon and David J. Hynek and Hyeuk Jin Han and Ravishankar Sundararaman and Judy J. Cha },

url = {https://www.nature.com/articles/s41467-024-50323-y.pdf},

doi = {10.1038/s41467-024-50323-y},

year  = {2024},

date = {2024-07-13},

urldate = {2024-07-13},

journal = {Nature Communications},

volume = {15},

number = {5889},

abstract = {Topological materials confined in 1D can transform computing technologies, such as 1D topological semimetals for nanoscale interconnects and 1D topological superconductors for fault-tolerant quantum computing. As such, understanding crystallization of 1D-confined topological materials is critical. Here, we demonstrate 1D template-assisted nanowire synthesis where we observe diameter-dependent phase selectivity for tungsten phosphides. A phase bifurcation occurs to produce tungsten monophosphide and tungsten diphosphide at the cross-over nanowire diameter regime of 35–70 nm. Four-dimensional scanning transmission electron microscopy is used to identify the two phases and to map crystallographic orientations of grains at a few nm resolution. The 1D-confined phase selectivity is attributed to the minimization of the total surface energy, which depends on the nanowire diameter and chemical potentials of precursors. Theoretical calculations are carried out to construct the diameter-dependent phase diagram, which agrees with experimental observations. Our findings suggest a crystallization route to stabilize topological materials confined in 1D},

note = {Topological materials confined in 1D could transform computing technology, but their crystallization is poorly understood. Here, the authors demonstrate template-based synthesis of 1D nanowires, revealing diameter-dependent phase selectivity.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Plasmonic trimers designed as SERS-active chemical traps for subtyping of lung tumors},

author = {Xing Zhao and Xiaojing Liu and Dexiang Chen and Guodong Shi and Guoqun Li and Xiao Tang and Xiangnan Zhu and Mingze Li and Lei Yao and Yunjia Wei and Wenzhe Song and Zixuan Sun and Xingce Fan and Zhixin Zhou and Teng Qiu and Qi Hao },

url = {https://www.nature.com/articles/s41467-024-50321-0.pdf},

doi = {10.1038/s41467-024-50321-0},

year  = {2024},

date = {2024-07-12},

urldate = {2024-07-12},

journal = {Nature Communications},

volume = {15},

number = {5855},

abstract = {Plasmonic materials can generate strong electromagnetic fields to boost the Raman scattering of surrounding molecules, known as surface-enhanced Raman scattering. However, these electromagnetic fields are heterogeneous, with only molecules located at the ‘hotspots’, which account for ≈ 1% of the surface area, experiencing efficient enhancement. Herein, we propose patterned plasmonic trimers, consisting of a pair of plasmonic dimers at the bilateral sides and a trap particle positioned in between, to address this challenge. The trimer configuration selectively directs probe molecules to the central traps where ‘hotspots’ are located through chemical affinity, ensuring a precise spatial overlap between the probes and the location of maximum field enhancement. We investigate the Raman enhancement of the Au@Al2O3-Au-Au@Al2O3 trimers, achieving a detection limit of 10−14 M of 4-methylbenzenethiol, 4-mercaptopyridine, and 4-aminothiophenol. Moreover, single-molecule SERS sensitivity is demonstrated by a bi-analyte method. Benefiting from this sensitivity, our approach is employed for the early detection of lung tumors using fresh tissues. Our findings suggest that this approach is sensitive to adenocarcinoma but not to squamous carcinoma or benign cases, offering insights into the differentiation between lung tumor subtypes.},

note = {SERS spectroscopy critically relies on the accumulation of analyte molecules in electromagnetic ‘hotspots’. Here, the authors demonstrate plasmonic trimers with central particles that act as chemical traps, enabling the subtyping of lung tumors using fresh tissue samples.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In-situ and wavelength-dependent photocatalytic strain evolution of a single Au nanoparticle on a TiO2 film},

author = {Sung Hyun Park and Sukyoung Kim and Jae Whan Park and Seunghee Kim and Wonsuk Cha and Joonseok Lee },

url = {https://www.nature.com/articles/s41467-024-49862-1.pdf},

doi = {10.1038/s41467-024-49862-1},

year  = {2024},

date = {2024-06-27},

urldate = {2024-06-27},

journal = {Nature Communications},

volume = {15},

number = {5416},

abstract = {Photocatalysis is a promising technique due to its capacity to efficiently harvest solar energy and its potential to address the global energy crisis. However, the structure–activity relationships of photocatalyst during wavelength-dependent photocatalytic reactions remains largely unexplored because it is difficult to measure under operating conditions. Here we show the photocatalytic strain evolution of a single Au nanoparticle (AuNP) supported on a TiO2 film by combining three-dimensional (3D) Bragg coherent X-ray diffraction imaging with an external light source. The wavelength-dependent generation of reactive oxygen species (ROS) has significant effects on the structural deformation of the AuNP, leading to its strain evolution. Density functional theory (DFT) calculations are employed to rationalize the induced strain caused by the adsorption of ROS on the AuNP surface. These observations provide insights of how the photocatalytic activity impacts on the structural deformation of AuNP, contributing to the general understanding of the atomic-level catalytic adsorption process.},

note = {The wavelength-dependent structural deformations of nanoparticles during photocatalysis are poorly understood. Here, the authors present the photocatalytic strain evolution of a single Au nanoparticle using 3D Bragg coherent X-ray diffraction imaging.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Efficient removal of nanoplastics from industrial wastewater through synergetic electrophoretic deposition and particle-stabilized foam formation},

author = {Amna Abdeljaoued and Beatriz López Ruiz and Yikalo-Eyob Tecle and Marie Langner and Natalie Bonakdar and Gudrun Bleyer and Patrik Stenner and Nicolas Vogel },

url = {https://www.nature.com/articles/s41467-024-48142-2.pdf},

doi = {10.1038/s41467-024-48142-2},

year  = {2024},

date = {2024-06-27},

urldate = {2024-06-27},

journal = {Nature Communications},

volume = {15},

number = {5437},

abstract = {Microplastic particles have been discovered in virtually all ecosystems worldwide, yet they may only represent the surface of a much larger issue. Nanoplastics, with dimensions well below 1 µm, pose an even greater environmental concern. Due to their size, they can infiltrate and disrupt individual cells within organisms, potentially exacerbating ecological impacts. Moreover, their minute dimensions present several hurdles for removal, setting them apart from microplastics. Here, we describe a process to remove colloidally stable nanoplastics from wastewater, which synergistically combines electrophoretic deposition and the formation of particle-stabilized foam. This approach capitalizes on localized changes in particle hydrophilicity induced by pH fluctuations resulting from water electrolysis at the electrode surface. By leveraging these pH shifts to enhance particle attachment to nascent bubbles proximal to the electrode, separation of colloidal particles from aqueous dispersions is achieved. Using poly(methyl methacrylate) (PMMA) colloidal particles as a model, we gain insights into the separation mechanisms, which are subsequently applied to alternative model systems with varying surface properties and materials, as well as to real-world industrial wastewaters from dispersion paints and PMMA fabrication processes. Our investigations demonstrate removal efficiencies surpassing 90%.},

note = {Nanoplastics represent a significant environmental challenge due to their minute size, which complicates removal efforts. Here, the authors present a method to effectively extract colloidally stable nanoplastic particles from industrial wastewater.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fluorescence resonance energy transfer in atomically precise metal nanoclusters by cocrystallization-induced spatial confinement},

author = {Hao Li and Tian Wang and Jiaojiao Han and Ying Xu and Xi Kang and Xiaosong Li and Manzhou Zhu },

url = {https://www.nature.com/articles/s41467-024-49735-7.pdf},

doi = {10.1038/s41467-024-49735-7},

year  = {2024},

date = {2024-06-24},

journal = {Nature Communications},

volume = {15},

number = {5351},

abstract = {Understanding the fluorescence resonance energy transfer (FRET) of metal nanoparticles at the atomic level has long been a challenge due to the lack of accurate systems with definite distance and orientation of molecules. Here we present the realization of achieving FRET between two atomically precise copper nanoclusters through cocrystallization-induced spatial confinement. In this study, we demonstrate the establishment of FRET in a cocrystallized Cu8(p-MBT)8(PPh3)4@Cu10(p-MBT)10(PPh3)4 system by exploiting the overlapping spectra between the excitation of the Cu10(p-MBT)10(PPh3)4 cluster and the emission of the Cu8(p-MBT)8(PPh3)4 cluster, combined with accurate control over the confined space between the two nanoclusters. Density functional theory is employed to provide deeper insights into the role of the distance and dipole orientations of molecules to illustrate the FRET procedure between two cluster molecules at the electronic structure level.},

note = {Understanding FRET of metal nanoparticles at the atomic level has long been a challenge. Here, the authors have achieved FRET activity with atomically precise Cu clusters by using a cocrystallisation-induced spatial confinement strategy.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Bulk-suppressed and surface-sensitive Raman scattering by transferable plasmonic membranes with irregular slot-shaped nanopores},

author = {Roman M. Wyss and Günter Kewes and Pietro Marabotti and Stefan M. Koepfli and Karl-Philipp Schlichting and Markus Parzefall and Eric Bonvin and Martin F. Sarott and Morgan Trassin and Maximilian Oezkent and Chen-Hsun Lu and Kevin-P. Gradwohl and Thomas Perrault and Lala Habibova and Giorgia Marcelli and Marcela Giraldo and Jan Vermant and Lukas Novotny and Martin Frimmer and Mads C. Weber and Sebastian Heeg },

url = {https://www.nature.com/articles/s41467-024-49130-2.pdf},

doi = {10.1038/s41467-024-49130-2},

year  = {2024},

date = {2024-06-19},

urldate = {2024-06-19},

journal = {Nature Communications},

volume = {15},

number = {5236},

abstract = {Raman spectroscopy enables the non-destructive characterization of chemical composition, crystallinity, defects, or strain in countless materials. However, the Raman response of surfaces or thin films is often weak and obscured by dominant bulk signals. Here we overcome this limitation by placing a transferable porous gold membrane, (PAuM) on the surface of interest. Slot-shaped nanopores in the membrane act as plasmonic antennas and enhance the Raman response of the surface or thin film underneath. Simultaneously, the PAuM suppresses the penetration of the excitation laser into the bulk, efficiently blocking its Raman signal. Using graphene as a model surface, we show that this method increases the surface-to-bulk Raman signal ratio by three orders of magnitude. We find that 90% of the Raman enhancement occurs within the top 2.5 nm of the material, demonstrating truly surface-sensitive Raman scattering. To validate our approach, we quantify the strain in a 12.5 nm thin Silicon film and analyze the surface of a LaNiO3 thin film. We observe a Raman mode splitting for the LaNiO3 surface-layer, which is spectroscopic evidence that the surface structure differs from the bulk. These results validate that PAuM gives direct access to Raman signatures of thin films and surfaces.},

note = {Characterizing surfaces by Raman spectroscopy is limited by the competition of surface and bulk Raman responses. Here the authors use nanoporous plasmonic membranes to enhance surface Raman signals while suppressing bulk contributions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Single-gold etching at the hypercarbon atom of C-centred hexagold(I) clusters protected by chiral N-heterocyclic carbenes},

author = {Xiao-Li Pei and Pei Zhao and Hitoshi Ube and Zhen Lei and Masahiro Ehara and Mitsuhiko Shionoya},

url = {https://www.nature.com/articles/s41467-024-49295-w.pdf},

doi = {10.1038/s41467-024-49295-w},

year  = {2024},

date = {2024-06-12},

urldate = {2024-06-12},

journal = {Nature Communications},

volume = {15},

number = {5024},

abstract = {Chemical etching of nano-sized metal clusters at the atomic level has a high potential for creating metal number-specific structures and functions that are difficult to achieve with bottom-up synthesis methods. In particular, precisely etching metal atoms one by one from nonmetallic element-centred metal clusters and elucidating the relationship between their well-defined structures, and chemical and physical properties will facilitate future materials design for metal clusters. Here we report the single-gold etching at a hypercarbon centre in gold(I) clusters. Specifically, C-centred hexagold(I) clusters protected by chiral N-heterocyclic carbenes are etched with bisphosphine to yield C-centred pentagold(I) (CAuI5) clusters. The CAuI5 clusters exhibit an unusually large bathochromic shift in luminescence, which is reproduced theoretically. The etching mechanism is experimentally and theoretically suggested to be a tandem dissociation-association-elimination pathway. Furthermore, the vacant site of the central carbon of the CAuI5 cluster can accommodate AuCl, allowing for post-functionalisation of the C-centred gold(I) clusters.},

note = {The control of atomically precise etching of nano-sized metal clusters is important for understanding their structure-specific properties. Here, the authors report the etching of a single gold atom on a hypercarbon centre of gold(I) clusters.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Waning-and-waxing shape changes in ionic nanoplates upon cation exchange},

author = {Zhanzhao Li and Masaki Saruyama and Toru Asaka and Toshiharu Teranishi },

url = {https://www.nature.com/articles/s41467-024-49294-x.pdf},

doi = {10.1038/s41467-024-49294-x},

year  = {2024},

date = {2024-06-08},

urldate = {2024-06-08},

journal = {Nature Communications},

volume = {15},

number = {4899},

abstract = {Flexible control of the composition and morphology of nanocrystals (NCs) over a wide range is an essential technology for the creation of functional nanomaterials. Cation exchange (CE) is a facile method by which to finely tune the compositions of ionic NCs, providing an opportunity to obtain complex nanostructures that are difficult to form using conventional chemical synthesis procedures. However, due to their robust anion frameworks, CE cannot typically be used to modify the original morphology of the host NCs. In this study, we report an anisotropic morphological transformation of Cu1.8S NCs during CE. Upon partial CE of Cu1.8S nanoplates (NPLs) with Mn2+, the hexagonal NPLs are transformed into crescent-shaped Cu1.8S–MnS NPLs. Upon further CE, these crescent-shaped NPLs evolve back into completely hexagonal MnS NPLs. Comprehensive characterization of the intermediates reveals that this waxing-and-waning shape-evolution process is due to dissolution, redeposition, and intraparticle migration of Cu+ and S2−. Furthermore, in addition to Mn2+, this CE-induced transformation process occurs with Zn2+, Cd2+ and Fe3+. This finding presents a strategy by which to create heterostructured NCs with various morphologies and compositions under mild conditions.},

note = {The robust anion framework of ionic nanocrystals impedes shape change by cation exchange. Here, the authors report an anisotropic, regenerative transformation of Cu1.8S nanoplates during cation exchange.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Collective chiroptical activity through the interplay of excitonic and charge-transfer effects in localized plasmonic fields},

author = {Huacheng Li and Xin Xu and Rongcheng Guan and Artur Movsesyan and Zhenni Lu and Qiliang Xu and Ziyun Jiang and Yurong Yang and Majid Khan and Jin Wen and Hongwei Wu and Santiago de la Moya and Gil Markovich and Huatian Hu and Zhiming Wang and Qiang Guo and Tao Yi and Alexander O. Govorov and Zhiyong Tang and Xiang Lan },

url = {https://www.nature.com/articles/s41467-024-49086-3.pdf},

doi = {10.1038/s41467-024-49086-3},

year  = {2024},

date = {2024-06-06},

urldate = {2024-06-06},

journal = {Nature Communications},

volume = {15},

number = {4846},

abstract = {The collective light-matter interaction of chiral supramolecular aggregates or molecular ensembles with confined light fields remains a mystery beyond the current theoretical description. Here, we programmably and accurately build models of chiral plasmonic complexes, aiming to uncover the entangled effects of excitonic correlations, intra- and intermolecular charge transfer, and localized surface plasmon resonances. The intricate interplay of multiple chirality origins has proven to be strongly dependent on the site-specificity of chiral molecules on plasmonic nanoparticle surfaces spanning the nanometer to sub-nanometer scale. This dependence is manifested as a distinct circular dichroism response that varies in spectral asymmetry/splitting, signal intensity, and internal ratio of intensity. The inhomogeneity of the surface-localized plasmonic field is revealed to affect excitonic and charge-transfer mixed intermolecular couplings, which are inherent to chirality generation and amplification. Our findings contribute to the development of hybrid classical-quantum theoretical frameworks and the harnessing of spin-charge transport for emergent applications.},

note = {Chiral interaction of molecular ensembles with confined light fields is elusive. Here, the authors report collective chiroptical effects through coupling of exciton and charge-transfer mixed molecular assemblies with plasmonic nanoparticles.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Pretreatment-free SERS sensing of microplastics using a self-attention-based neural network on hierarchically porous Ag foams},

author = {Olga Guselnikova and Andrii Trelin and Yunqing Kang and Pavel Postnikov and Makoto Kobashi and Asuka Suzuki and Lok Kumar Shrestha and Joel Henzie and Yusuke Yamauchi },

url = {https://www.nature.com/articles/s41467-024-48148-w.pdf},

doi = {10.1038/s41467-024-48148-w},

year  = {2024},

date = {2024-05-28},

urldate = {2024-05-28},

journal = {Nature Communications},

volume = {15},

number = {4351},

abstract = {Low-cost detection systems are needed for the identification of microplastics (MPs) in environmental samples. However, their rapid identification is hindered by the need for complex isolation and pre-treatment methods. This study describes a comprehensive sensing platform to identify MPs in environmental samples without requiring independent separation or pre-treatment protocols. It leverages the physicochemical properties of macroporous-mesoporous silver (Ag) substrates templated with self-assembled polymeric micelles to concurrently separate and analyze multiple MP targets using surface-enhanced Raman spectroscopy (SERS). The hydrophobic layer on Ag aids in stabilizing the nanostructures in the environment and mitigates biofouling. To monitor complex samples with multiple MPs and to demultiplex numerous overlapping patterns, we develop a neural network (NN) algorithm called SpecATNet that employs a self-attention mechanism to resolve the complex dependencies and patterns in SERS data to identify six common types of MPs: polystyrene, polyethylene, polymethylmethacrylate, polytetrafluoroethylene, nylon, and polyethylene terephthalate. SpecATNet uses multi-label classification to analyze multi-component mixtures even in the presence of various interference agents. The combination of macroporous-mesoporous Ag substrates and self-attention-based NN technology holds potential to enable field monitoring of MPs by generating rich datasets that machines can interpret and analyze.},

note = {Detection and identification of microplastics (MPs) in environmental samples is hampered by the need for isolation and pretreatment methods. Here, the authors combine porous Ag substrates with self-attention neural networks to directly identify six types of MPs in environmental samples.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Narrowband room temperature phosphorescence of closed-loop molecules through the multiple resonance effect},

author = {Xiaokang Yao and Yuxin Li and Huifang Shi and Ze Yu and Beishen Wu and Zixing Zhou and Chifeng Zhou and Xifang Zheng and Mengting Tang and Xiao Wang and Huili Ma and Zhengong Meng and Wei Huang and Zhongfu An },

url = {https://www.nature.com/articles/s41467-024-48856-3.pdf},

doi = {10.1038/s41467-024-48856-3},

year  = {2024},

date = {2024-05-28},

urldate = {2024-05-28},

journal = {Nature Communications},

volume = {15},

number = {4520},

abstract = {Luminescent materials with narrowband emission show great potential for diverse applications in optoelectronics. Purely organic phosphors with room-temperature phosphorescence (RTP) have made significant success in rationally manipulating quantum efficiency, lifetimes, and colour gamut in the past years, but there is limited attention on the purity of the RTP colours. Herein we report a series of closed-loop molecules with narrowband phosphorescence by multiple resonance effect, which significantly improves the colour purity of RTP. Phosphors show narrowband phosphorescence with full width at half maxima (FWHM) of 30 nm after doping into a rigid benzophenone matrix under ambient conditions, of which the RTP efficiency reaches 51.8%. At 77 K, the FWHM of phosphorescence is only 11 nm. Meanwhile, the colour of narrowband RTP can be tuned from sky blue to green with the modification of methyl groups. Additionally, the potential applications in X-ray imaging and display are demonstrated. This work not only outlines a design principle for developing narrowband RTP materials but also makes a major step forward extending the potential applications of narrowband luminescent materials in optoelectronics.},

note = {Luminescent materials with narrowband emissions are vital for optoelectronic applications. Here, the authors achieve room temperature phosphorescence with a FWHM of 30 nm through the multiple resonance effect and showcase its practical application in X-ray imaging.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Self-assembly of nanocrystal checkerboard patterns via non-specific interactions},

author = {Yufei Wang and Yilong Zhou and Quanpeng Yang and Rourav Basak and Yu Xie and Dong Le and Alexander D. Fuqua and Wade Shipley and Zachary Yam and Alex Frano and Gaurav Arya and Andrea R. Tao },

url = {https://www.nature.com/articles/s41467-024-47572-2.pdf},

doi = {10.1038/s41467-024-47572-2},

year  = {2024},

date = {2024-05-09},

urldate = {2024-05-09},

journal = {Nature Communications},

volume = {15},

number = {3913},

abstract = {Checkerboard lattices—where the resulting structure is open, porous, and highly symmetric—are difficult to create by self-assembly. Synthetic systems that adopt such structures typically rely on shape complementarity and site-specific chemical interactions that are only available to biomolecular systems (e.g., protein, DNA). Here we show the assembly of checkerboard lattices from colloidal nanocrystals that harness the effects of multiple, coupled physical forces at disparate length scales (interfacial, interparticle, and intermolecular) and that do not rely on chemical binding. Colloidal Ag nanocubes were bi-functionalized with mixtures of hydrophilic and hydrophobic surface ligands and subsequently assembled at an air–water interface. Using feedback between molecular dynamics simulations and interfacial assembly experiments, we achieve a periodic checkerboard mesostructure that represents a tiny fraction of the phase space associated with the polymer-grafted nanocrystals used in these experiments. In a broader context, this work expands our knowledge of non-specific nanocrystal interactions and presents a computation-guided strategy for designing self-assembling materials.},

note = {The self-assembly of nanocrystals into checkerboard lattice patterns is difficult to control. Here, the authors investigate the formation of such patterns from hydrophilic/hydrophobic bifunctionalized Ag nanocubes and use multiscale simulations to understand the effects of physical forces.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Synthetic molecular switches driven by DNA-modifying enzymes},

author = {Hong Kang and Yuexuan Yang and Bryan Wei },

url = {https://www.nature.com/articles/s41467-024-47742-2.pdf},

doi = {10.1038/s41467-024-47742-2},

year  = {2024},

date = {2024-05-06},

urldate = {2024-05-06},

journal = {Nature Communications},

volume = {15},

number = {3781},

abstract = {Taking inspiration from natural systems, in which molecular switches are ubiquitous in the biochemistry regulatory network, we aim to design and construct synthetic molecular switches driven by DNA-modifying enzymes, such as DNA polymerase and nicking endonuclease. The enzymatic treatments on our synthetic DNA constructs controllably switch ON or OFF the sticky end cohesion and in turn cascade to the structural association or disassociation. Here we showcase the concept in multiple DNA nanostructure systems with robust assembly/disassembly performance. The switch mechanisms are first illustrated in minimalist systems with a few DNA strands. Then the ON/OFF switches are realized in complex DNA lattice and origami systems with designated morphological changes responsive to the specific enzymatic treatments.},

note = {Molecular switches are ubiquitous in the biochemistry regulatory network. Here, the authors construct synthetic molecular switches controlled by DNA-modifying enzymes such as DNA polymerase and nicking endonuclease to control and cascade assembly and disassembly.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Low-index mesoscopic surface reconstructions of Au surfaces using Bayesian force fields},

author = {Cameron J. Owen and Yu Xie and Anders Johansson and Lixin Sun and Boris Kozinsky },

url = {https://www.nature.com/articles/s41467-024-48192-6.pdf},

doi = {10.1038/s41467-024-48192-6},

year  = {2024},

date = {2024-05-06},

urldate = {2024-05-06},

journal = {Nature Communications},

volume = {15},

number = {3790},

abstract = {Metal surfaces have long been known to reconstruct, significantly influencing their structural and catalytic properties. Many key mechanistic aspects of these subtle transformations remain poorly understood due to limitations of previous simulation approaches. Using active learning of Bayesian machine-learned force fields trained from ab initio calculations, we enable large-scale molecular dynamics simulations to describe the thermodynamics and time evolution of the low-index mesoscopic surface reconstructions of Au (e.g., the Au(111)-‘Herringbone,’ Au(110)-(1 × 2)-‘Missing-Row,’ and Au(100)-‘Quasi-Hexagonal’ reconstructions). This capability yields direct atomistic understanding of the dynamic emergence of these surface states from their initial facets, providing previously inaccessible information such as nucleation kinetics and a complete mechanistic interpretation of reconstruction under the effects of strain and local deviations from the original stoichiometry. We successfully reproduce previous experimental observations of reconstructions on pristine surfaces and provide quantitative predictions of the emergence of spinodal decomposition and localized reconstruction in response to strain at non-ideal stoichiometries. A unified mechanistic explanation is presented of the kinetic and thermodynamic factors driving surface reconstruction. Furthermore, we study surface reconstructions on Au nanoparticles, where characteristic (111) and (100) reconstructions spontaneously appear on a variety of high-symmetry particle morphologies.},

note = {Metal surfaces have long been known to reconstruct, but key mechanistic aspects are poorly understood. Here, the authors use Bayesian force fields to gain insights into gold surface reconstructions that are crucial for material science and catalysis.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Optofluidic crystallithography for directed growth of single-crystalline halide perovskites},

author = {Xue-Guang Chen and Linhan Lin and Guan-Yao Huang and Xiao-Mei Chen and Xiao-Ze Li and Yun-Ke Zhou and Yixuan Zou and Tairan Fu and Peng Li and Zhengcao Li and Hong-Bo Sun },

url = {https://www.nature.com/articles/s41467-024-48110-w.pdf},

doi = {10.1038/s41467-024-48110-w},

year  = {2024},

date = {2024-05-01},

urldate = {2024-05-01},

journal = {Nature Communications},

volume = {15},

number = {3677},

abstract = {Crystallization is a fundamental phenomenon which describes how the atomic building blocks such as atoms and molecules are arranged into ordered or quasi-ordered structure and form solid-state materials. While numerous studies have focused on the nucleation behavior, the precise and spatiotemporal control of growth kinetics, which dictates the defect density, the micromorphology, as well as the properties of the grown materials, remains elusive so far. Herein, we propose an optical strategy, termed optofluidic crystallithography (OCL), to solve this fundamental problem. Taking halide perovskites as an example, we use a laser beam to manipulate the molecular motion in the native precursor environment and create inhomogeneous spatial distribution of the molecular species. Harnessing the coordinated effect of laser-controlled local supersaturation and interfacial energy, we precisely steer the ionic reaction at the growth interface and directly print arbitrary single crystals of halide perovskites of high surface quality, crystallinity, and uniformity at a high printing speed of 102 μm s−1. The OCL technique can be potentially extended to the fabrication of single-crystal structures beyond halide perovskites, once crystallization can be triggered under the laser-directed local supersaturation.},

note = {Precise and spatio-temporal control of crystallization kinetics is important but challenging. Here, the authors propose an optical strategy called optofluidic crystallithography to steer the growth of single-crystalline halide perovskites.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Visible-light-excited robust room-temperature phosphorescence of dimeric single-component luminophores in the amorphous state},

author = {Danman Guo and Wen Wang and Kaimin Zhang and Jinzheng Chen and Yuyuan Wang and Tianyi Wang and Wangmeng Hou and Zhen Zhang and Huahua Huang and Zhenguo Chi and Zhiyong Yang },

url = {https://www.nature.com/articles/s41467-024-47937-7.pdf},

doi = {10.1038/s41467-024-47937-7},

year  = {2024},

date = {2024-04-27},

urldate = {2024-04-27},

journal = {Nature Communications},

volume = {15},

number = {3598},

abstract = {Organic room temperature phosphorescence (RTP) has significant potential in various applications of information storage, anti-counterfeiting, and bio-imaging. However, achieving robust organic RTP emission of the single-component system is challenging to overcome the restriction of the crystalline state or other rigid environments with cautious treatment. Herein, we report a single-component system with robust persistent RTP emission in various aggregated forms, such as crystal, fine powder, and even amorphous states. Our experimental data reveal that the vigorous RTP emissions rely on their tight dimers based on strong and large-overlap π-π interactions between polycyclic aromatic hydrocarbon (PAH) groups. The dimer structure can offer not only excitons in low energy levels for visible-light excited red long-lived RTP but also suppression of the nonradiative decays even in an amorphous state for good resistance of RTP to heat (up to 70 °C) or water. Furthermore, we demonstrate the water-dispersible nanoparticle with persistent RTP over 600 nm and a lifetime of 0.22 s for visible-light excited cellular and in-vivo imaging, prepared through the common microemulsion approach without overcaution for nanocrystal formation.},

note = {Organic room-temperature phosphorescence (RTP) is limited to rigid environments. Here, the authors report a single-component system with robust persistent RTP emissions in various aggregation states, such as crystalline, fine powder, and amorphous.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Collapse of carbon nanotubes due to local high-pressure from van der Waals encapsulation},

author = {Cheng Hu and Jiajun Chen and Xianliang Zhou and Yufeng Xie and Xinyue Huang and Zhenghan Wu and Saiqun Ma and Zhichun Zhang and Kunqi Xu and Neng Wan and Yueheng Zhang and Qi Liang and Zhiwen Shi },

url = {https://www.nature.com/articles/s41467-024-47903-3.pdf},

doi = {10.1038/s41467-024-47903-3},

year  = {2024},

date = {2024-04-25},

urldate = {2024-04-25},

journal = {Nature Communications},

volume = {15},

number = {3486},

abstract = {Van der Waals (vdW) assembly of low-dimensional materials has proven the capability of creating structures with on-demand properties. It is predicted that the vdW encapsulation can induce a local high-pressure of a few GPa, which will strongly modify the structure and property of trapped materials. Here, we report on the structural collapse of carbon nanotubes (CNTs) induced by the vdW encapsulation. By simply covering CNTs with a hexagonal boron nitride flake, most of the CNTs (≈77%) convert from a tubular structure to a collapsed flat structure. Regardless of their original diameters, all the collapsed CNTs exhibit a uniform height of ≈0.7 nm, which is roughly the thickness of bilayer graphene. Such structural collapse is further confirmed by Raman spectroscopy, which shows a prominent broadening and blue shift in the Raman G-peak. The vdW encapsulation-induced collapse of CNTs is fully captured by molecular dynamics simulations of the local vdW pressure. Further near-field optical characterization reveals a metal-semiconductor transition in accompany with the CNT structural collapse. Our study provides not only a convenient approach to generate local high-pressure for fundamental research, but also a collapsed-CNT semiconductor for nanoelectronic applications.},

note = {Van der Waals (vdW) assembly of low-dimensional materials has proven the capability of creating structures with on-demand properties. Here, the authors report on the structural collapse of CNTs in conjunction with a metal-semiconductor junction induced by the VdW encapsulation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Flower-shaped 2D crystals grown in curved fluid vesicle membranes},

author = {Hao Wan and Geunwoong Jeon and Weiyue Xin and Gregory M. Grason and Maria M. Santore },

url = {https://www.nature.com/articles/s41467-024-47844-x.pdf},

doi = {10.1038/s41467-024-47844-x},

year  = {2024},

date = {2024-04-24},

urldate = {2024-04-24},

journal = {Nature Communications},

volume = {15},

number = {3442},

abstract = {The morphologies of two-dimensional (2D) crystals, nucleated, grown, and integrated within 2D elastic fluids, for instance in giant vesicle membranes, are dictated by an interplay of mechanics, permeability, and thermal contraction. Mitigation of solid strain drives the formation of crystals with vanishing Gaussian curvature (i.e., developable domain shapes) and, correspondingly, enhanced Gaussian curvature in the surrounding 2D fluid. However, upon cooling to grow the crystals, large vesicles sustain greater inflation and tension because their small area-to-volume ratio slows water permeation. As a result, more elaborate shapes, for instance, flowers with bendable but inextensible petals, form on large vesicles despite their more gradual curvature, while small vesicles harbor compact planar crystals. This size dependence runs counter to the known cumulative growth of strain energy of 2D colloidal crystals on rigid spherical templates. This interplay of intra-membrane mechanics and processing points to the scalable production of flexible molecular crystals of controllable complex shape.},

note = {Thin crystals grown on rigid spherical templates of increasing curvature exhibit increased protrusions. Here, the authors demonstrate the opposite curvature effect on the morphology of molecularly thin crystals grown within elastic fluid membranes, like those of biological cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Topology selectivity of a conformationally flexible precursor through selenium doping},

author = {Liangliang Cai and Tianhao Gao and Andrew T. S. Wee },

url = {https://www.nature.com/articles/s41467-024-47614-9.pdf},

doi = {10.1038/s41467-024-47614-9},

year  = {2024},

date = {2024-04-15},

urldate = {2024-04-15},

journal = {Nature Communications},

volume = {15},

number = {3235},

abstract = {Conformational arrangements within nanostructures play a crucial role in shaping the overall configuration and determining the properties, for example in covalent/metal organic frameworks. In on-surface synthesis, conformational diversity often leads to uncontrollable or disordered structures. Therefore, the exploration of controlling and directing the conformational arrangements is significant in achieving desired nanoarchitectures. Herein, a conformationally flexible precursor 2,4,6-tris(3-bromophenyl)−1,3,5-triazine is employed, and a random phase consisting of C3h and Cs conformers is firstly obtained after deposition of the precursor on Cu(111) at room temperature to 365 K. At low coverage (0.01 ML) selenium doping, we achieve the selectivity of the C3h conformer and improve the nanopore structural homogeneity. The ordered two-dimensional metal organic nanostructure can be fulfilled by selenium doping from room temperature to 365 K. The formation of the conformationally flexible precursor on Cu(111) is explored through the combination of high-resolution scanning tunneling microscopy and non-contact atomic force microscopy. The regulation of energy diagrams in the absence or presence of the Se atom is revealed by density functional theory calculations. These results can enrich the on-surface synthesis toolbox of conformationally flexible precursors, for the design of complex nanoarchitectures, and for future development of engineered nanomaterials.},

note = {Research into the control of conformational arrangements is of great importance for achieving bespoke nanoarchitectures. Here, the authors achieve topology selectivity of a conformationally flexible precursor by Se doping.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Stress-induced ordering evolution of 1D segmented heteronanostructures and their chemical post-transformations},

author = {Qing-Xia Chen and Yu-Yang Lu and Yang Yang and Li-Ge Chang and Yi Li and Yuan Yang and Zhen He and Jian-Wei Liu and Yong Ni and Shu-Hong Yu },

url = {https://www.nature.com/articles/s41467-024-47446-7.pdf},

doi = {10.1038/s41467-024-47446-7},

year  = {2024},

date = {2024-04-13},

urldate = {2024-04-13},

journal = {Nature Communications},

volume = {15},

number = {3208},

abstract = {Investigations of one-dimensional segmented heteronanostructures (1D-SHs) have recently attracted much attention due to their potentials for applications resulting from their structure and synergistic effects between compositions and interfaces. Unfortunately, developing a simple, versatile and controlled synthetic method to fabricate 1D-SHs is still a challenge. Here we demonstrate a stress-induced axial ordering mechanism to describe the synthesis of 1D-SHs by a general under-stoichiometric reaction strategy. Using the continuum phase-field simulations, we elaborate a three-stage evolution process of the regular segment alternations. This strategy, accompanied by easy chemical post-transformations, enables to synthesize 25 1D-SHs, including 17 nanowire-nanowire and 8 nanowire-nanotube nanostructures with 13 elements (Ag, Te, Cu, Pt, Pb, Cd, Sb, Se, Bi, Rh, Ir, Ru, Zn) involved. This ordering evolution-driven synthesis will help to investigate the ordering reconstruction and potential applications of 1D-SHs.},

note = {The formation mechanisms for periodic heterostructures are still poorly understood. Here, the authors propose a versatile approach to synthesize one-dimensional segmented heterostructures and reveal a stress-induced ordering mechanism through phase-field simulations.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Dynamic multicolor emissions of multimodal phosphors by Mn2+ trace doping in self-activated CaGa4O7},

author = {Yiqian Tang and Yiyu Cai and Kunpeng Dou and Jianqing Chang and Wei Li and Shanshan Wang and Mingzi Sun and Bolong Huang and Xiaofeng Liu and Jianrong Qiu and Lei Zhou and Mingmei Wu and Jun-Cheng Zhang },

url = {https://www.nature.com/articles/s41467-024-47431-0.pdf},

doi = {10.1038/s41467-024-47431-0},

year  = {2024},

date = {2024-04-13},

urldate = {2024-04-13},

journal = {Nature Communications},

volume = {15},

number = {3209},

abstract = {The manipulation of excitation modes and resultant emission colors in luminescent materials holds pivotal importance for encrypting information in anti-counterfeiting applications. Despite considerable achievements in multimodal and multicolor luminescent materials, existing options generally suffer from static monocolor emission under fixed external stimulation, rendering them vulnerability to replication. Achieving dynamic multimodal luminescence within a single material presents a promising yet challenging solution. Here, we report the development of a phosphor exhibiting dynamic multicolor photoluminescence (PL) and photo-thermo-mechanically responsive multimodal emissions through the incorporation of trace Mn2+ ions into a self-activated CaGa4O7 host. The resulting phosphor offers adjustable emission-color changing rates, controllable via re-excitation intervals and photoexcitation powers. Additionally, it demonstrates temperature-induced color reversal and anti-thermal-quenched emission, alongside reproducible elastic mechanoluminescence (ML) characterized by high mechanical durability. Theoretical calculations elucidate electron transfer pathways dominated by intrinsic interstitial defects and vacancies for dynamic multicolor emission. Mn2+ dopants serve a dual role in stabilizing nearby defects and introducing additional defect levels, enabling flexible multi-responsive luminescence. This developed phosphor facilitates evolutionary color/pattern displays in both temporal and spatial dimensions using readily available tools, offering significant promise for dynamic anticounterfeiting displays and multimode sensing applications.},

note = {Achieving dynamic multimodal luminescence in a single material is promising but challenging. Here, the authors engineer a phosphor with dynamic multicolor luminescence and photo-thermomechanically responsive emissions by adding Mn2+ to a self-activated CaGa4O7 host.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Spiral packing and chiral selectivity in model membranes probed by phase-resolved sum-frequency generation microscopy},

author = {Alexander P. Fellows and Ben John and Martin Wolf and Martin Thämer },

url = {https://www.nature.com/articles/s41467-024-47573-1.pdf},

doi = {10.1038/s41467-024-47573-1},

year  = {2024},

date = {2024-04-11},

urldate = {2024-04-11},

journal = {Nature Communications},

volume = {15},

number = {3161},

abstract = {Since the lipid raft model was developed at the end of the last century, it became clear that the specific molecular arrangements of phospholipid assemblies within a membrane have profound implications in a vast range of physiological functions. Studies of such condensed lipid islands in model systems using fluorescence and Brewster angle microscopies have shown a wide range of sizes and morphologies, with suggestions of substantial in-plane molecular anisotropy and mesoscopic structural chirality. Whilst these variations can significantly alter many membrane properties including its fluidity, permeability and molecular recognition, the details of the in-plane molecular orientations underlying these traits remain largely unknown. Here, we use phase-resolved sum-frequency generation microscopy on model membranes of mixed chirality phospholipid monolayers to fully determine the three-dimensional molecular structure of the constituent micron-scale condensed domains. We find that the domains possess curved molecular directionality with spiralling mesoscopic packing, where both the molecular and spiral turning directions depend on the lipid chirality, but form structures clearly deviating from mirror symmetry for different enantiomeric mixtures. This demonstrates strong enantioselectivity in the domain growth process and indicates fundamental thermodynamic differences between homo- and heterochiral membranes, which may be relevant in the evolution of homochirality in all living organisms.},

note = {The properties of lipid membranes are intimately controlled by their complex heterogeneous structure. Here, the authors use phase-resolved sum-frequency generation microscopy to fully determine the hierarchical lipid packing from the molecular to the mesoscopic scale.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Controlled condensation by liquid contact-induced adaptations of molecular conformations in self-assembled monolayers},

author = {Guoying Bai and Haiyan Zhang and Dong Gao and Houguo Fei and Cunlan Guo and Mingxia Ren and Yufeng Liu },

url = {https://www.nature.com/articles/s41467-024-47507-x.pdf},

doi = {10.1038/s41467-024-47507-x},

year  = {2024},

date = {2024-04-11},

urldate = {2024-04-11},

journal = {Nature Communications},

volume = {2024},

number = {3132},

abstract = {Surface condensation control strategies are crucial but commonly require relatively tedious, time-consuming, and expensive techniques for surface-chemical and topographical engineering. Here we report a strategy to alter surface condensation behavior without resorting to any molecule-type or topographical transmutations. After ultrafast contact of liquids with and removal from surfaces, the condensation rate and density of water droplets on the surfaces decrease, the extent of which is positively correlated with the polarity of the liquid and the duration of contact. The liquid contact-induced condensation rate/density decrease (LCICD) can be attributed to the decrease of nucleation site density resulted from the liquid contact-induced adaption of surface molecular conformation. Based on this, we find that LCICD is applicable to various surfaces, on condition that there are flexible segments capable of shielding at least part of nucleation sites through changing the conformation under liquid contact induction. Leveraging the LCICD effect, we achieve erasable information storage on diverse substrates. Furthermore, our strategy holds promise for controlling condensation of other substances since LCICD is not specific to the water condensation process.},

note = {Surface condensation is predetermined and is typically adjusted by chemical or topographical surface modification. Here, the authors report on a strategy to control the surface condensation behavior by adjusting molecular conformations in self-assembled monolayers.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Impact of molecular symmetry on crystallization pathways in highly supersaturated KH2PO4 solutions},

author = {Yong Chan Cho and Sooheyong Lee and Lei Wang and Yun-Hee Lee and Seongheun Kim and Hyun-Hwi Lee and John Jonghyun Lee and Geun Woo Lee },

url = {https://www.nature.com/articles/s41467-024-47503-1.pdf},

doi = {10.1038/s41467-024-47503-1},

year  = {2024},

date = {2024-04-10},

urldate = {2024-04-10},

journal = {Nature Communications},

volume = {15},

number = {3117},

abstract = {Solute structure and its evolution in supersaturated aqueous solutions are key clues to understand Ostwald’s step rule. Here, we measure the structural evolution of solute molecules in highly supersaturated solutions of KH2PO4 (KDP) and NH4H2PO4 (ADP) using a combination of electrostatic levitation and synchrotron X-ray scattering. The measurement reveals the existence of a solution-solution transition in KDP solution, caused by changing molecular symmetries and structural evolution of the solution with supersaturation. Moreover, we find that the molecular symmetry of H2PO4- impacts on phase selection. These findings manifest that molecular symmetry and its structural evolution can govern the crystallization pathways in aqueous solutions, explaining the microscopic origin of Ostwald’s step rule.},

note = {The molecular symmetry of solute structure in aqueous solutions is a key clue to understand Ostwald’s step rule. Here, the authors show that molecular symmetry and its structural evolution can govern the crystallization pathways in aqueous solutions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Kinetically controlled metal-elastomer nanophases for environmentally resilient stretchable electronics},

author = {Soosang Chae and Won Jin Choi and Lisa Julia Nebel and Chang Hee Cho and Quinn A. Besford and André Knapp and Pavlo Makushko and Yevhen Zabila and Oleksandr Pylypovskyi and Min Woo Jeong and Stanislav Avdoshenko and Oliver Sander and Denys Makarov and Yoon Jang Chung and Andreas Fery and Jin Young Oh and Tae Il Lee },

url = {https://www.nature.com/articles/s41467-024-47223-6.pdf},

doi = {10.1038/s41467-024-47223-6},

year  = {2024},

date = {2024-04-09},

urldate = {2024-04-09},

journal = {Nature Communications},

volume = {15},

number = {3071},

abstract = {Nanophase mixtures, leveraging the complementary strengths of each component, are vital for composites to overcome limitations posed by single elemental materials. Among these, metal-elastomer nanophases are particularly important, holding various practical applications for stretchable electronics. However, the methodology and understanding of nanophase mixing metals and elastomers are limited due to difficulties in blending caused by thermodynamic incompatibility. Here, we present a controlled method using kinetics to mix metal atoms with elastomeric chains on the nanoscale. We find that the chain migration flux and metal deposition rate are key factors, allowing the formation of reticular nanophases when kinetically in-phase. Moreover, we observe spontaneous structural evolution, resulting in gyrified structures akin to the human brain. The hybridized gyrified reticular nanophases exhibit strain-invariant metallic electrical conductivity up to 156% areal strain, unparalleled durability in organic solvents and aqueous environments with pH 2–13, and high mechanical robustness, a prerequisite for environmentally resilient devices.},

note = {Metal-elastomer nanophases are critical for stretchable electronics but face mixing challenges. This study introduces a kinetic method for precise mixing, yielding gyrified nanophases with improved durability and strain-invariant conductivity, which holds promise for resilient stretchable devices.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Wang2024,

title = {Universal inter-molecular radical transfer reactions on metal surfaces},

author = {Junbo Wang and Kaifeng Niu and Huaming Zhu and Chaojie Xu and Chuan Deng and Wenchao Zhao and Peipei Huang and Haiping Lin and Dengyuan Li and Johanna Rosen and Peinian Liu and Francesco Allegretti and Johannes V. Barth and Biao Yang and Jonas Björk and Qing Li and Lifeng Chi },

url = {https://www.nature.com/articles/s41467-024-47252-1.pdf},

doi = {10.1038/s41467-024-47252-1},

year  = {2024},

date = {2024-04-08},

urldate = {2024-04-08},

journal = {Nature Communications},

volume = {15},

number = {3030},

abstract = {On-surface synthesis provides tools to prepare low-dimensional supramolecular structures. Traditionally, reactive radicals are a class of single-electron species, serving as exceptional electron-withdrawing groups. On metal surfaces, however, such species are affected by conduction band screening effects that may even quench their unpaired electron characteristics. As a result, radicals are expected to be less active, and reactions catalyzed by surface-stabilized radicals are rarely reported. Herein, we describe a class of inter-molecular radical transfer reactions on metal surfaces. With the assistance of aryl halide precursors, the coupling of terminal alkynes is steered from non-dehydrogenated to dehydrogenated products, resulting in alkynyl-Ag-alkynyl bonds. Dehalogenated molecules are fully passivated by detached hydrogen atoms. The reaction mechanism is unraveled by various surface-sensitive technologies and density functional theory calculations. Moreover, we reveal the universality of this mechanism on metal surfaces. Our studies enrich the on-surface synthesis toolbox and develop a pathway for producing low-dimensional organic materials.},

note = {Radicals are expected to be inactive on metal surfaces. Here the authors describe general intermolecular radical transfer reactions on Ag and Cu surfaces and confirm the reaction mechanism by extensive control experiments.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Crosslinking-induced patterning of MOFs by direct photo- and electron-beam lithography},

author = {Xiaoli Tian and Fu Li and Zhenyuan Tang and Song Wang and Kangkang Weng and Dan Liu and Shaoyong Lu and Wangyu Liu and Zhong Fu and Wenjun Li and Hengwei Qiu and Min Tu and Hao Zhang and Jinghong Li },

url = {https://www.nature.com/articles/s41467-024-47293-6.pdf},

doi = {10.1038/s41467-024-47293-6},

year  = {2024},

date = {2024-04-04},

urldate = {2024-04-04},

journal = {Nature Communications},

volume = {15},

number = {2920},

abstract = {Metal-organic frameworks (MOFs) with diverse chemistry, structures, and properties have emerged as appealing materials for miniaturized solid-state devices. The incorporation of MOF films in these devices, such as the integrated microelectronics and nanophotonics, requires robust patterning methods. However, existing MOF patterning methods suffer from some combinations of limited material adaptability, compromised patterning resolution and scalability, and degraded properties. Here we report a universal, crosslinking-induced patterning approach for various MOFs, termed as CLIP-MOF. Via resist-free, direct photo- and electron-beam (e-beam) lithography, the ligand crosslinking chemistry leads to drastically reduced solubility of colloidal MOFs, permitting selective removal of unexposed MOF films with developer solvents. This enables scalable, micro-/nanoscale (≈70 nm resolution), and multimaterial patterning of MOFs on large-area, rigid or flexible substrates. Patterned MOF films preserve their crystallinity, porosity, and other properties tailored for targeted applications, such as diffractive gas sensors and electrochromic pixels. The combined features of CLIP-MOF create more possibilities in the system-level integration of MOFs in various electronic, photonic, and biomedical devices.},

note = {Precise and scalable patterning is essential for the use of metal-organic frameworks (MOFs) in solid-state electronics and photonics. Here, the authors report on resistance-free, direct photo- and electron-beam lithography of MOF films using crosslinking chemistry.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Direct observation of phase transitions in truncated tetrahedral microparticles under quasi-2D confinement},

author = {David Doan and John Kulikowski and X. Wendy Gu },

url = {https://www.nature.com/articles/s41467-024-46230-x.pdf},

doi = {10.1038/s41467-024-46230-x},

year  = {2024},

date = {2024-03-25},

urldate = {2024-03-25},

journal = {Nature Communications},

volume = {15},

number = {1954},

abstract = {Colloidal crystals are used to understand fundamentals of atomic rearrangements in condensed matter and build complex metamaterials with unique functionalities. Simulations predict a multitude of self-assembled crystal structures from anisotropic colloids, but these shapes have been challenging to fabricate. Here, we use two-photon lithography to fabricate Archimedean truncated tetrahedrons and self-assemble them under quasi-2D confinement. These particles self-assemble into a hexagonal phase under an in-plane gravitational potential. Under additional gravitational potential, the hexagonal phase transitions into a quasi-diamond two-unit basis. In-situ imaging reveal this phase transition is initiated by an out-of-plane rotation of a particle at a crystalline defect and causes a chain reaction of neighboring particle rotations. Our results provide a framework of studying different structures from hard-particle self-assembly and demonstrates the ability to use confinement to induce unusual phases.},

note = {Boundary conditions can give rise to new types of phases during self-assembly. Here the authors show that tetrahedral particles can form a hexagonal phase on a surface, that can transform into a quasi-diamond phase under a gravitational field.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Forward-predictive SERS-based chemical taxonomy for untargeted structural elucidation of epimeric cerebrosides},

author = {Emily Xi Tan and Shi Xuan Leong and Wei An Liew and In Yee Phang and Jie Ying Ng and Nguan Soon Tan and Yie Hou Lee and Xing Yi Ling 

},

url = {https://www.nature.com/articles/s41467-024-46838-z.pdf},

doi = {10.1038/s41467-024-46838-z},

year  = {2024},

date = {2024-03-22},

urldate = {2024-03-22},

journal = {Nature Communications},

volume = {15},

number = {2582},

abstract = {Achieving untargeted chemical identification, isomeric differentiation, and quantification is critical to most scientific and technological problems but remains challenging. Here, we demonstrate an integrated SERS-based chemical taxonomy machine learning framework for untargeted structural elucidation of 11 epimeric cerebrosides, attaining >90% accuracy and robust single epimer and multiplex quantification with <10% errors. First, we utilize 4-mercaptophenylboronic acid to selectively capture the epimers at molecular sites of isomerism to form epimer-specific SERS fingerprints. Corroborating with in-silico experiments, we establish five spectral features, each corresponding to a structural characteristic: (1) presence/absence of epimers, (2) monosaccharide/cerebroside, (3) saturated/unsaturated cerebroside, (4) glucosyl/galactosyl, and (5) GlcCer or GalCer’s carbon chain lengths. Leveraging these insights, we create a fully generalizable framework to identify and quantify cerebrosides at concentrations between 10−4 to 10−10 M and achieve multiplex quantification of binary mixtures containing biomarkers GlcCer24:1, and GalCer24:1 using their untrained spectra in the models},

note = {SERS-based chemical taxonomy is attractive for practical SERS applications where the identity and concentration of analytes are unknown. Here, the authors demonstrate a machine learning framework for classifying “unknown” molecules that lie outside the boundaries of the models used.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Toward sub-second solution exchange dynamics in flow reactors for liquid-phase transmission electron microscopy},

author = {Stefan Merkens and Christopher Tollan and Giuseppe De Salvo and Katarzyna Bejtka and Marco Fontana and Angelica Chiodoni and Joscha Kruse and Maiara Aime Iriarte-Alonso and Marek Grzelczak and Andreas Seifert and Andrey Chuvilin },

url = {https://www.nature.com/articles/s41467-024-46842-3.pdf},

doi = {10.1038/s41467-024-46842-3},

year  = {2024},

date = {2024-03-21},

urldate = {2024-03-21},

journal = {Nature Communications},

volume = {15},

number = {2522},

abstract = {Liquid-phase transmission electron microscopy is a burgeoning experimental technique for monitoring nanoscale dynamics in a liquid environment, increasingly employing microfluidic reactors to control the composition of the sample solution. Current challenges comprise fast mass transport dynamics inside the central nanochannel of the liquid cell, typically flow cells, and reliable fixation of the specimen in the limited imaging area. In this work, we present a liquid cell concept – the diffusion cell – that satisfies these seemingly contradictory requirements by providing additional on-chip bypasses to allow high convective transport around the nanochannel in which diffusive transport predominates. Diffusion cell prototypes are developed using numerical mass transport models and fabricated on the basis of existing two-chip setups. Important hydrodynamic parameters, i.e., the total flow resistance, the flow velocity in the imaging area, and the time constants of mixing, are improved by 2-3 orders of magnitude compared to existing setups. The solution replacement dynamics achieved within seconds already match the mixing timescales of many ex-situ scenarios, and further improvements are possible. Diffusion cells can be easily integrated into existing liquid-phase transmission electron microscopy workflows, provide correlation of results with ex-situ experiments, and can create additional research directions addressing fast nanoscale processes.},

note = {In liquid-phase TEM, microfluidic reactors are used to monitor nanoscale (electro)chemical dynamics in liquid environments. Here, the authors develop a reactor design with accelerated mass transport, facilitating quantitative in-situ and in-operando studies.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Controlled dissolution of a single ion from a salt interface},

author = {Huijun Han and Yunjae Park and Yohan Kim and Feng Ding and Hyung-Joon Shin },

url = {https://www.nature.com/articles/s41467-024-46704-y.pdf},

doi = {10.1038/s41467-024-46704-y},

year  = {2024},

date = {2024-03-16},

urldate = {2024-03-16},

journal = {Nature Communications},

volume = {15},

number = {2401},

abstract = {Interactions between monatomic ions and water molecules are fundamental to understanding the hydration of complex polyatomic ions and ionic process. Among the simplest and well-established ion-related reactions is dissolution of salt in water, which is an endothermic process requiring an increase in entropy. Extensive efforts have been made to date; however, most studies at single-ion level have been limited to theoretical approaches. Here, we demonstrate the salt dissolution process by manipulating a single water molecule at an under-coordinated site of a sodium chloride film. Manipulation of molecule in a controlled manner enables us to understand ion–water interaction as well as dynamics of water molecules at NaCl interfaces, which are responsible for the selective dissolution of anions. The water dipole polarizes the anion in the NaCl ionic crystal, resulting in strong anion–water interaction and weakening of the ionic bonds. Our results provide insights into a simple but important elementary step of the single-ion chemistry, which may be useful in ion-related sciences and technologies.

},

note = {The strong ionic bond in salt is broken by electrostatic interactions with water, but direct observation at the level of a single ion is challenging. Here, the authors have visualized the preferential dissolution of an anion by manipulating a single water molecule.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Electrostatic potentials of atomic nanostructures at metal surfaces quantified by scanning quantum dot microscopy},

author = {Rustem Bolat and Jose M. Guevara and Philipp Leinen and Marvin Knol and Hadi H. Arefi and Michael Maiworm and Rolf Findeisen and Ruslan Temirov and Oliver T. Hofmann and Reinhard J. Maurer and F. Stefan Tautz and Christian Wagner },

url = {https://www.nature.com/articles/s41467-024-46423-4.pdf},

doi = {10.1038/s41467-024-46423-4},

year  = {2024},

date = {2024-03-13},

urldate = {2024-03-13},

journal = {Nature Communications},

volume = {15},

number = {2259},

abstract = {The discrete and charge-separated nature of matter — electrons and nuclei — results in local electrostatic fields that are ubiquitous in nanoscale structures and relevant in catalysis, nanoelectronics and quantum nanoscience. Surface-averaging techniques provide only limited experimental access to these potentials, which are determined by the shape, material, and environment of the nanostructure. Here, we image the potential over adatoms, chains, and clusters of Ag and Au atoms assembled on Ag(111) and quantify their surface dipole moments. By focusing on the total charge density, these data establish a benchmark for theory. Our density functional theory calculations show a very good agreement with experiment and allow a deeper analysis of the dipole formation mechanisms, their dependence on fundamental atomic properties and on the shape of the nanostructures. We formulate an intuitive picture of the basic mechanisms behind dipole formation, allowing better design choices for future nanoscale systems such as single-atom catalysts.},

note = {Surface averaging techniques offer only limited access to the electrostatic potentials of nanostructures, which are determined by shape, material, and environment. Here, the authors quantify these potentials for gold and silver adatom chains, explaining the mechanisms of dipole formation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In situ electrochemical regeneration of nanogap hotspots for continuously reusable ultrathin SERS sensors},

author = {Sarah May Sibug-Torres and David-Benjamin Grys and Gyeongwon Kang and Marika Niihori and Elle Wyatt and Nicolas Spiesshofer and Ashleigh Ruane and Bart de Nijs and Jeremy J. Baumberg },

url = {https://www.nature.com/articles/s41467-024-46097-y.pdf},

doi = {10.1038/s41467-024-46097-y},

year  = {2024},

date = {2024-03-06},

urldate = {2024-03-06},

journal = {Nature Communications},

volume = {15},

number = {2022},

abstract = {Surface-enhanced Raman spectroscopy (SERS) harnesses the confinement of light into metallic nanoscale hotspots to achieve highly sensitive label-free molecular detection that can be applied for a broad range of sensing applications. However, challenges related to irreversible analyte binding, substrate reproducibility, fouling, and degradation hinder its widespread adoption. Here we show how in-situ electrochemical regeneration can rapidly and precisely reform the nanogap hotspots to enable the continuous reuse of gold nanoparticle monolayers for SERS. Applying an oxidising potential of +1.5 V (vs Ag/AgCl) for 10 s strips a broad range of adsorbates from the nanogaps and forms a metastable oxide layer of few-monolayer thickness. Subsequent application of a reducing potential of −0.80 V for 5 s in the presence of a nanogap-stabilising molecular scaffold, cucurbit[5]uril, reproducibly regenerates the optimal plasmonic properties with SERS enhancement factors ≈106. The regeneration of the nanogap hotspots allows these SERS substrates to be reused over multiple cycles, demonstrating ≈5% relative standard deviation over at least 30 cycles of analyte detection and regeneration. Such continuous and reliable SERS-based flow analysis accesses diverse applications from environmental monitoring to medical diagnostics.},

note = {SERS is a powerful analytical technique, but achieving reproducibility for continuous analysis a challenge. Here, the authors report a SERS substrate recycling method that enables direct analysis of complex samples without substrate contamination.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Reversible chirality inversion of an AuAgx-cysteine coordination polymer by pH change},

author = {Bing Ni and Dustin Vivod and Jonathan Avaro and Haoyuan Qi and Dirk Zahn and Xun Wang and Helmut Cölfen },

url = {https://www.nature.com/articles/s41467-024-45935-3.pdf},

doi = {10.1038/s41467-024-45935-3},

year  = {2024},

date = {2024-03-06},

urldate = {2024-03-06},

journal = {Nature Communications},

volume = {15},

number = {2042},

abstract = {Responsive chiral systems have attracted considerable attention, given their potential for diverse applications in biology, optoelectronics, photonics, and related fields. Here we show the reversible chirality inversion of an AuAgx-cysteine (AuAgx-cys) coordination polymer (CP) by pH changes. The polymer can be obtained by mixing HAuCl4 and AgNO3 with L-cysteine (or D-cysteine) in appropriate proportions in H2O (or other surfactant solutions). Circular dichroism (CD) spectrum is used to record the strong optical activity of the AuAg0.06-L-cys enantiomer (denoted as L0.06), which can be switched to that of the corresponding D0.06 enantiomer by alkalization (final dispersion pH > 13) and can be switched back after neutralization (final dispersion pH <8). Multiple structural changes at different pH values (≈9.6, ≈13) are observed through UV-Vis and CD spectral measurements, as well as other controlled experiments. Exploration of the CP synthesis kinetics suggests that the covalent bond formation is rapid and then the conformation of the CP materials would continuously evolve. The reaction stoichiometry investigation shows that the formation of CP materials with chirality inversion behavior requires the balancing between different coordination and polymerization processes. This study provides insights into the potential of inorganic stereochemistry in developing promising functional materials.},

note = {Reactive chiral systems have attracted much attention in biology, optoelectronics, and photonics; however, a comprehensive understanding of these systems remains incomplete. Here the authors show the reversible chirality of AuAgx-cys coordination polymers induced by pH changes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Guo2024,

title = {Extensive photochemical restructuring of molecule-metal surfaces under room light},

author = {Chenyang Guo and Philip Benzie and Shu Hu and Bart de Nijs and Ermanno Miele and Eoin Elliott and Rakesh Arul and Helen Benjamin and Grzegorz Dziechciarczyk and Reshma R. Rao and Mary P. Ryan and Jeremy J. Baumberg },

url = {https://www.nature.com/articles/s41467-024-46125-x.pdf},

doi = {10.1038/s41467-024-46125-x},

year  = {2024},

date = {2024-03-02},

urldate = {2024-03-02},

journal = {Nature Communications},

volume = {15},

number = {1928},

abstract = {The molecule-metal interface is of paramount importance for many devices and processes, and directly involved in photocatalysis, molecular electronics, nanophotonics, and molecular (bio-)sensing. Here the photostability of this interface is shown to be sensitive even to room light levels for specific molecules and metals. Optical spectroscopy is used to track photoinduced migration of gold atoms when functionalised with different thiolated molecules that form uniform monolayers on Au. Nucleation and growth of characteristic surface metal nanostructures is observed from the light-driven adatoms. By watching the spectral shifts of optical modes from nanoparticles used to precoat these surfaces, we identify processes involved in the photo-migration mechanism and the chemical groups that facilitate it. This photosensitivity of the molecule-metal interface highlights the significance of optically induced surface reconstruction. In some catalytic contexts this can enhance activity, especially utilising atomically dispersed gold. Conversely, in electronic device applications such reconstructions introduce problematic aging effects.},

note = {The nature of the molecule-metal interface is crucial for many technological applications. Here, the authors show that the photostability of the material can be sensitive to room light when coated with a single molecular layer, with implications for devices and processes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Yan2024,

title = {Spatiotemporal control of photochromic upconversion through interfacial energy transfer},

author = {Long Yan and Jinshu Huang and Zhengce An and Qinyuan Zhang and Bo Zhou },

url = {https://www.nature.com/articles/s41467-024-46228-5.pdf},

doi = {10.1038/s41467-024-46228-5},

year  = {2024},

date = {2024-03-01},

urldate = {2024-03-01},

journal = {Nature Communications},

volume = {15},

number = {1923},

abstract = {Dynamic control of multi-photon upconversion with rich and tunable emission colors is stimulating extensive interest in both fundamental research and frontier applications of lanthanide based materials. However, manipulating photochromic upconversion towards color-switchable emissions of a single lanthanide emitter is still challenging. Here, we report a conceptual model to realize the spatiotemporal control of upconversion dynamics and photochromic evolution of Er3+ through interfacial energy transfer (IET) in a core-shell nanostructure. The design of Yb sublattice sensitization interlayer, instead of regular Yb3+ doping, is able to raise the absorption capability of excitation energy and enhance the upconversion. We find that a nanoscale spatial manipulation of interfacial interactions between Er and Yb sublattices can further contribute to upconversion. Moreover, the red/green color-switchable upconversion of Er3+ is achieved through using the temporal modulation ways of non-steady-state excitation and time-gating technique. Our results allow for versatile designs and dynamic management of emission colors from luminescent materials and provide more chances for their frontier photonic applications such as optical anti-counterfeiting and speed monitoring.},

note = {Achieving spatiotemporal control of photochromic upconversion from a single lanthanide emitter remains challenging. Here, the authors present a conceptual model enabling such control of Er3+ photochromic upconversion via interfacial energy transfer in a core-shell nanostructure.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Otsuka2024,

title = {Transient chemical and structural changes in graphene oxide during ripening},

author = {Hayato Otsuka and Koki Urita and Nobutaka Honma and Takashi Kimuro and Yasushi Amako and Radovan Kukobat and Teresa J. Bandosz and Junzo Ukai and Isamu Moriguchi and Katsumi Kaneko },

url = {https://www.nature.com/articles/s41467-024-46083-4.pdf},

doi = {10.1038/s41467-024-46083-4},

year  = {2024},

date = {2024-02-24},

urldate = {2024-02-24},

journal = {Nature Communications},

volume = {15},

number = {1708},

abstract = {Graphene oxide (GO)—the oxidized form of graphene—is actively studied in various fields, such as energy, electronic devices, separation of water, materials engineering, and medical technologies, owing to its fascinating physicochemical properties. One major drawback of GO is its instability, which leads to the difficulties in product management. A physicochemical understanding of the ever-changing nature of GO can remove the barrier for its growing applications. Here, we evidencde the presence of intrinsic, metastable and transient GO states upon ripening. The three GO states are identified using a pi-pi* transition peak of ultraviolet–visible absorption spectra and exhibit inherent magnetic and electrical properties. The presence of three states of GO is supported by the compositional changes of oxygen functional groups detected via X-ray photoelectron spectroscopy and structural information from X-ray diffraction analysis and transmission electron microscopy. Although intrinsic GO having a pi-pi* transition at 230.5 ± 0.5 nm is stable only for 5 days at 298 K, the intrinsic state can be stabilized by either storing GO dispersions below 255 K or by adding ammonium peroxydisulfate.},

note = {Graphene oxide is in demand for various applications - however, this is complicated by changing physicochemical properties over time. Here, the authors show the intrinsic, metastable, and transient states of graphene oxide colloids upon ripening.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Baek2024,

title = {Insights into structural defect formation in individual InP/ZnSe/ZnS quantum dots under UV oxidation},

author = {Hayeon Baek and Sungsu Kang and Junyoung Heo and Soonmi Choi and Ran Kim and Kihyun Kim and Nari Ahn and Yeo-Geon Yoon and Taekjoon Lee and Jae Bok Chang and Kyung Sig Lee and Young-Gil Park and Jungwon Park },

url = {https://www.nature.com/articles/s41467-024-45944-2.pdf},

doi = {10.1038/s41467-024-45944-2},

year  = {2024},

date = {2024-02-23},

urldate = {2024-02-23},

journal = {Nature Communications},

volume = {15},

number = {1671},

abstract = {InP/ZnSe/ZnS quantum dots (QDs) stand as promising candidates for advancing QD-organic light-emitting diodes (QLED), but low emission efficiency due to their susceptibility to oxidation impedes applications. Structural defects play important roles in the emission efficiency degradation of QDs, but the formation mechanism of defects in oxidized QDs has been less investigated. Here, we investigated the impact of diverse structural defects formation on individual QDs and propagation during UV-facilitated oxidation using high-resolution (scanning) transmission electron microscopy. UV-facilitated oxidation of the QDs alters shell morphology by the formation of surface oxides, leaving ZnSe surfaces poorly passivated. Further oxidation leads to the formation of structural defects, such as dislocations, and induces strain at the oxide-QD interfaces, facilitating In diffusion from the QD core. These changes in the QD structures result in emission quenching. This study provides insight into the formation of structural defects through photo-oxidation, and their effects on emission properties of QDs.},

note = {InP/ZnSe/ZnS quantum dots (QDs) are promising candidates for advanced light-emitting diodes, but low emission efficiency due to oxidation hampers applications. Here, the authors provide insight into the structural defects that form on individual QDs during UV-facilitated oxidation. },

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Yuan2024,

title = {Direct in-situ insights into the asymmetric surface reconstruction of rutile TiO2 (110)},

author = {Wentao Yuan and Bingwei Chen and Zhong-Kang Han and Ruiyang You and Ying Jiang and Rui Qi and Guanxing Li and Hanglong Wu and Maria Veronica Ganduglia-Pirovano and Yong Wang },

url = {https://www.nature.com/articles/s41467-024-46011-6.pdf},

doi = {10.1038/s41467-024-46011-6},

year  = {2024},

date = {2024-02-22},

urldate = {2024-02-22},

journal = {Nature Communications},

volume = {15},

number = {1616},

abstract = {The reconstruction of rutile TiO2 (110) holds significant importance as it profoundly influences the surface chemistry and catalytic properties of this widely used material in various applications, from photocatalysis to solar energy conversion. Here, we directly observe the asymmetric surface reconstruction of rutile TiO2 (110)-(1×2) with atomic-resolution using in situ spherical aberration-corrected scanning transmission electron microscopy. Density functional theory calculations were employed to complement the experimental observations. Our findings highlight the pivotal role played by repulsive electrostatic interaction among the small polarons −formed by excess electrons following the removal of neutral oxygen atoms− and the subsequent surface relaxations induced by these polarons. The emergence and disappearance of these asymmetric structures can be controlled by adjusting the oxygen partial pressure. This research provides a deeper understanding, prediction, and manipulation of the surface reconstructions of rutile TiO2 (110), holding implications for a diverse range of applications and technological advancements involving rutile-based materials.

},

note = {The reconstruction of rutile TiO2 (110) impacts its surface chemistry and catalytic properties. Here, the authors offer a detailed understanding of the asymmetric surface reconstruction of TiO2 (110)-(1×2) through a combination of STEM and DFT calculations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Zhang2024,

title = {Spontaneous crystallization of strongly confined CsSnxPb1-xI3 perovskite colloidal quantum dots at room temperature},

author = {Louwen Zhang and Hai Zhou and Yibo Chen and Zhimiao Zheng and Lishuai Huang and Chen Wang and Kailian Dong and Zhongqiang Hu and Weijun Ke and Guojia Fang },

url = {https://www.nature.com/articles/s41467-024-45945-1.pdf},

doi = {10.1038/s41467-024-45945-1},

year  = {2024},

date = {2024-02-21},

urldate = {2024-02-21},

journal = {Nature Communications},

volume = {15},

number = {1609},

abstract = {The scalable and low-cost room temperature (RT) synthesis for pure-iodine all-inorganic perovskite colloidal quantum dots (QDs) is a challenge due to the phase transition induced by thermal unequilibrium. Here, we introduce a direct RT strongly confined spontaneous crystallization strategy in a Cs-deficient reaction system without polar solvents for synthesizing stable pure-iodine all-inorganic tin-lead (Sn-Pb) alloyed perovskite colloidal QDs, which exhibit bright yellow luminescence. By tuning the ratio of Cs/Pb precursors, the size confinement effect and optical band gap of the resultant CsSnxPb1-xI3 perovskite QDs can be well controlled. This strongly confined RT approach is universal for wider bandgap bromine- and chlorine-based all-inorganic and iodine-based hybrid perovskite QDs. The alloyed CsSn0.09Pb0.91I3 QDs show superior yellow emission properties with prolonged carrier lifetime and significantly increased colloidal stability compared to the pristine CsPbI3 QDs, which is enabled by strong size confinement, Sn2+ passivation and enhanced formation energy. These findings provide a RT size-stabilized synthesis pathway to achieve high-performance pure-iodine all-inorganic Sn-Pb mixed perovskite colloidal QDs for optoelectronic applications.},

note = {Photoactive pure-iodine all-inorganic colloidal perovskite quantum dots (QDs) are attractive for optoelectronic applications, however their synthesis at room temperature is challenging. Here the authors report a room temperature strongly confined strategy to synthesize  CsSnxPb1-xI3 QDs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Lei2024,

title = {Dual heterogeneous interfaces enhance X-ray excited persistent luminescence for low-dose 3D imaging},

author = {Lei Lei and Minghao Yi and Yubin Wang and Youjie Hua and Junjie Zhang and Paras N. Prasad and Shiqing Xu },

url = {https://www.nature.com/articles/s41467-024-45390-0.pdf},

doi = {10.1038/s41467-024-45390-0},

year  = {2024},

date = {2024-02-07},

urldate = {2024-02-07},

journal = {Nature Communications},

volume = {15},

number = {1140},

abstract = {Lanthanide-doped fluoride nanoparticles (NPs) showcase adjustable X-ray-excited persistent luminescence (XEPL), holding significant promise for applications in three-dimensional (3D) imaging through the creation of flexible X-ray detectors. However, a dangerous high X-ray irradiation dose rate and complicated heating procedure are required to generate efficient XEPL for high-resolution 3D imaging, which is attributed to a lack of strategies to significantly enhance the XEPL intensity. Here we report that the XEPL intensity of a series of lanthanide activators (Dy, Pr, Er, Tm, Gd, Tb) is greatly improved by constructing dual heterogeneous interfaces in a double-shell nanostructure. Mechanistic studies indicate that the employed core@shell@shell structure could not only passivate the surface quenchers to lower the non-radiative relaxation possibility, but also reduce the interfacial Frenkel defect formation energy leading to increase the trap concentration. By employing a NPs containing flexible film as the scintillation screen, the inside 3D electrical structure of a watch was clearly achieved based on the delayed XEPL imaging and 3D reconstruction procedure. We foresee that these findings will promote the development of advanced X-ray activated persistent fluoride NPs and offer opportunities for safer and more efficient X-ray imaging techniques in a number of scientific and practical areas.},

note = {High-resolution X-ray imaging requires a high radiation dose. Here, the authors achieve low-dose 3D imaging by increasing the XEPL intensity using a double-shell nanostructure with two heterogeneous interfaces.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Sun2024,

title = {Rapid synthesis of phosphor-glass composites in seconds based on particle self-stabilization},

author = {Yongsheng Sun and Yuzhen Wang and Weibin Chen and Qingquan Jiang and Dongdan Chen and Guoping Dong and Zhiguo Xia },

url = {https://www.nature.com/articles/s41467-024-45293-0.pdf},

doi = {10.1038/s41467-024-45293-0},

year  = {2024},

date = {2024-02-05},

urldate = {2024-02-05},

journal = {Nature Communications},

volume = {15},

number = {1033},

abstract = {Phosphor-glass composites (PGC) are excellent candidates for highly efficient and stable photonic converters; however, their synthesis generally requires harsh procedures and long time, resulting in additional performance loss and energy consumption. Here we develop a rapid synthetic route to PGC within about 10 seconds, which enables uniform dispersion of Y3Al5O12:Ce3+ (YAG:Ce) phosphor particles through a particle self-stabilization model in molten tellurite glass. Thanks for good wettability between YAG:Ce micro-particles and tellurite glass melt, it creates an energy barrier of 6.94 × 105 zJ to prevent atomic-scale contact and sintering of particles in the melt. This in turn allows the generation of YAG:Ce-based PGC as attractive emitters with high quantum efficiency (98.4%) and absorption coefficient (86.8%) that can produce bright white light with luminous flux of 1227 lm and luminous efficiency of 276 lm W−1 under blue laser driving. This work shows a generalizable synthetic strategy for the development of functional glass composites.},

note = {Phosphor-glass composites can serve as efficient and stable photonic converters, but their synthesis generally requires harsh and time-consuming procedures. Here, the authors report an alternative synthesis route that requires only a few seconds and is based on particle self-stabilization.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Piquero-Zulaica2024,

title = {Deceptive orbital confinement at edges and pores of carbon-based 1D and 2D nanoarchitectures},

author = {Ignacio Piquero-Zulaica and Eduardo Corral-Rascón and Xabier Diaz de Cerio and Alexander Riss and Biao Yang and Aran Garcia-Lekue and Mohammad A. Kher-Elden and Zakaria M. Abd El-Fattah and Shunpei Nobusue and Takahiro Kojima and Knud Seufert and Hiroshi Sakaguchi and Willi Auwärter and Johannes V. Barth},

url = {https://www.nature.com/articles/s41467-024-45138-w.pdf},

doi = {10.1038/s41467-024-45138-w},

year  = {2024},

date = {2024-02-05},

urldate = {2024-02-05},

journal = {Nature Communications},

volume = {15},

number = {1062},

abstract = {The electronic structure defines the properties of graphene-based nanomaterials. Scanning tunneling microscopy/spectroscopy (STM/STS) experiments on graphene nanoribbons (GNRs), nanographenes, and nanoporous graphene (NPG) often determine an apparent electronic orbital confinement into the edges and nanopores, leading to dubious interpretations such as image potential states or super-atom molecular orbitals. We show that these measurements are subject to a wave function decay into the vacuum that masks the undisturbed electronic orbital shape. We use Au(111)-supported semiconducting gulf-type GNRs and NPGs as model systems fostering frontier orbitals that appear confined along the edges and nanopores in STS measurements. DFT calculations confirm that these states originate from valence and conduction bands. The deceptive electronic orbital confinement observed is caused by a loss of Fourier components, corresponding to states of high momentum. This effect can be generalized to other 1D and 2D carbon-based nanoarchitectures and is important for their use in catalysis and sensing applications.},

note = {The apparent electronic confinement at nanographene boundaries in scanning tunneling microscopy/spectroscopy is often misinterpreted. Here, the authors explain this phenomenon in terms of the decay of frontier orbitals and confinement at the edges of graphene nanoribbons and pores in nanoporous graphene.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Nominally identical microplastic models differ greatly in their particle-cell interactions},

author = {Simon Wieland and Anja F. R. M. Ramsperger and Wolfgang Gross and Moritz Lehmann and Thomas Witzmann and Anja Caspari and Martin Obst and Stephan Gekle and Günter K. Auernhammer and Andreas Fery and Christian Laforsch and Holger Kress},

url = {https://www.nature.com/articles/s41467-024-45281-4.pdf},

doi = {10.1038/s41467-024-45281-4},

year  = {2024},

date = {2024-01-31},

urldate = {2024-01-31},

journal = {Nature Communications},

volume = {15},

number = {922},

abstract = {Due to the abundance of microplastics in the environment, research about its possible adverse effects is increasing exponentially. Most studies investigating the effect of microplastics on cells still rely on commercially available polystyrene microspheres. However, the choice of these model microplastic particles can affect the outcome of the studies, as even nominally identical model microplastics may interact differently with cells due to different surface properties such as the surface charge. Here, we show that nominally identical polystyrene microspheres from eight different manufacturers significantly differ in their ζ-potential, which is the electrical potential of a particle in a medium at its slipping plane. The ζ-potential of the polystyrene particles is additionally altered after environmental exposure. We developed a microfluidic microscopy platform to demonstrate that the ζ-potential determines particle-cell adhesion strength. Furthermore, we find that due to this effect, the ζ-potential also strongly determines the internalization of the microplastic particles into cells. Therefore, the ζ-potential can act as a proxy of microplastic-cell interactions and may govern adverse effects reported in various organisms exposed to microplastics.},

note = {Microplastics research is often based on commercial model particles. Here, the authors show that nominally identical particles may differ significantly in their properties and thus in their interactions with cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{Dai2024,

title = {Switchable unidirectional emissions from hydrogel gratings with integrated carbon quantum dots},

author = {Chenjie Dai and Shuai Wan and Zhe Li and Yangyang Shi and Shuang Zhang and Zhongyang Li },

url = {https://www.nature.com/articles/s41467-024-45284-1.pdf},

doi = {10.1038/s41467-024-45284-1},

year  = {2024},

date = {2024-01-29},

urldate = {2024-01-29},

journal = {Nature Communications},

volume = {15},

number = {845},

abstract = {Directional emission of photoluminescence despite its incoherence is an attractive technique for light-emitting fields and nanophotonics. Optical metasurfaces provide a promising route for wavefront engineering at the subwavelength scale, enabling the feasibility of unidirectional emission. However, current directional emission strategies are mostly based on static metasurfaces, and it remains a challenge to achieve unidirectional emissions tuning with high performance. Here, we demonstrate quantum dots-hydrogel integrated gratings for actively switchable unidirectional emission with simultaneously a narrow divergence angle less than 1.5° and a large diffraction angle greater than 45°. We further demonstrate that the grating efficiency alteration leads to a more than 7-fold tuning of emission intensity at diffraction order due to the variation of hydrogel morphology subject to change in ambient humidity. Our proposed switchable emission strategy can promote technologies of active light-emitting devices for radiation control and optical imaging.},

note = {Directional emission of photoluminescence is an emerging technique for light-emitting fields and nanophotonics. Here, the authors demonstrate a hydrogel grating with integrated quantum dots for switchable unidirectional emission tuning.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Accurate prediction of the optical properties of nanoalloys with both plasmonic and magnetic elements},

author = {Vito Coviello and Denis Badocco and Paolo Pastore and Martina Fracchia and Paolo Ghigna and Alessandro Martucci and Daniel Forrer and Vincenzo Amendola },

url = {https://www.nature.com/articles/s41467-024-45137-x.pdf},

doi = {10.1038/s41467-024-45137-x},

year  = {2024},

date = {2024-01-27},

urldate = {2024-01-27},

journal = {Nature Communications},

volume = {15},

number = {834},

abstract = {The alloying process plays a pivotal role in the development of advanced multifunctional plasmonic materials within the realm of modern nanotechnology. However, accurate in silico predictions are only available for metal clusters of just a few nanometers, while the support of modelling is required to navigate the broad landscape of components, structures and stoichiometry of plasmonic nanoalloys regardless of their size. Here we report on the accurate calculation and conceptual understanding of the optical properties of metastable alloys of both plasmonic (Au) and magnetic (Co) elements obtained through a tailored laser synthesis procedure. The model is based on the density functional theory calculation of the dielectric function with the Hubbard-corrected local density approximation, the correction for intrinsic size effects and use of classical electrodynamics. This approach is built to manage critical aspects in modelling of real samples, as spin polarization effects due to magnetic elements, short-range order variability, and size heterogeneity. The method provides accurate results also for other magnetic-plasmonic (Au-Fe) and typical plasmonic (Au-Ag) nanoalloys, thus being available for the investigation of several other nanomaterials waiting for assessment and exploitation in fundamental sectors such as quantum optics, magneto-optics, magneto-plasmonics, metamaterials, chiral catalysis and plasmon-enhanced catalysis.},

note = {The optical properties of nanoalloys are complex and difficult to describe. Here, the authors use density functional and Mie theory to calculate the extinction of Au-Co and other nanoalloys of interest for quantum optics, magnetooptics, catalysis, and metamaterials.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ratiometric fluorescent sensing of pyrophosphate with sp³-functionalized single-walled carbon nanotubes},

author = {Simon Settele and C. Alexander Schrage and Sebastian Jung and Elena Michel and Han Li and Benjamin S. Flavel and A. Stephen K. Hashmi and Sebastian Kruss and Jana Zaumseil },

url = {https://www.nature.com/articles/s41467-024-45052-1.pdf},

doi = {10.1038/s41467-024-45052-1},

year  = {2024},

date = {2024-01-24},

urldate = {2024-01-24},

journal = {Nature Communications},

volume = {14},

number = {706},

abstract = {Inorganic pyrophosphate is a key molecule in many biological processes from DNA synthesis to cell metabolism. Here we introduce sp3-functionalized (6,5) single-walled carbon nanotubes (SWNTs) with red-shifted defect emission as near-infrared luminescent probes for the optical detection and quantification of inorganic pyrophosphate. The sensing scheme is based on the immobilization of Cu2+ ions on the SWNT surface promoted by coordination to covalently attached aryl alkyne groups and a triazole complex. The presence of Cu2+ ions on the SWNT surface causes fluorescence quenching via photoinduced electron transfer, which is reversed by copper-complexing analytes such as pyrophosphate. The differences in the fluorescence response of sp3-defect to pristine nanotube emission enables reproducible ratiometric measurements in a wide concentration window. Biocompatible, phospholipid-polyethylene glycol-coated SWNTs with such sp3 defects are employed for the detection of pyrophosphate in cell lysate and for monitoring the progress of DNA synthesis in a polymerase chain reaction. This robust ratiometric and near-infrared luminescent probe for pyrophosphate may serve as a starting point for the rational design of nanotube-based biosensors.},

note = {Inorganic pyrophosphate is a key molecule in many biological processes. Here, the authors develop an optical sensor that enables its ratiometric detection in the near infrared with functionalized single-walled carbon nanotubes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Synthesis of inter-[60]fullerene conjugates with inherent chirality},

author = {Yoshifumi Hashikawa and Shu Okamoto and Yasujiro Murata },

url = {https://www.nature.com/articles/s41467-024-44834-x.pdf},

doi = {10.1038/s41467-024-44834-x},

year  = {2024},

date = {2024-01-15},

urldate = {2024-01-15},

journal = {Nature Communications},

volume = {15},

number = {514},

abstract = {Coalescence of [60]fullerenes potentially produces hypothetical nanocarbon assemblies with non-naturally occurring topologies. Since the discovery of [60]fullerene in 1985, coalesced [60]fullerene oligomers have only been observed as transient species by transmission electron microscopy during an oligomerization process under a high electron acceleration voltage. Herein, we showcase the rational synthesis of covalent assemblies consisting of inherently chiral open-[60]fullerenes. The crystallographic analyses unveiled double-caged structures of non-conjugated and conjugated inter-[60]fullerene hybrids, in which the two [60]fullerene cages are bounds to each other through a covalent linkage. The former one further assembles via a heterochiral recognition so that four carbon cages are arranged in a tetrahedral manner both in solution and solid state. Reflecting radially-conjugated double π-surface nature, the inter-[60]fullerene conjugate exhibits strong electronic communication in its reduced states, intense absorption behavior, and chiroptical activity with a dissymmetry factor of 0.21 (at 674 nm) which breaks the record for known chiral organic molecules.},

note = {Inter-fullerene conjugates are non-naturally occurring carbon allotropes. Here the authors report on the chemical synthesis and solid-state structure of three inter-[60]fullerene hybrids with inherent chirality.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Quantitative analysis of printed nanostructured networks using high-resolution 3D FIB-SEM nanotomography},

author = {Cian Gabbett and Luke Doolan and Kevin Synnatschke and Laura Gambini and Emmet Coleman and Adam G. Kelly and Shixin Liu and Eoin Caffrey and Jose Munuera and Catriona Murphy and Stefano Sanvito and Lewys Jones and Jonathan N. Coleman 

},

url = {https://www.nature.com/articles/s41467-023-44450-1.pdf},

doi = {10.1038/s41467-023-44450-1},

year  = {2024},

date = {2024-01-04},

urldate = {2024-01-04},

journal = {Nature Communications},

volume = {15},

number = {278},

abstract = {Networks of solution-processed nanomaterials are becoming increasingly important across applications in electronics, sensing and energy storage/generation. Although the physical properties of these devices are often completely dominated by network morphology, the network structure itself remains difficult to interrogate. Here, we utilise focused ion beam – scanning electron microscopy nanotomography (FIB-SEM-NT) to quantitatively characterise the morphology of printed nanostructured networks and their devices using nanometre-resolution 3D images. The influence of nanosheet/nanowire size on network structure in printed films of graphene, WS2 and silver nanosheets (AgNSs), as well as networks of silver nanowires (AgNWs), is investigated. We present a comprehensive toolkit to extract morphological characteristics including network porosity, tortuosity, specific surface area, pore dimensions and nanosheet orientation, which we link to network resistivity. By extending this technique to interrogate the structure and interfaces within printed vertical heterostacks, we demonstrate the potential of this technique for device characterisation and optimisation.},

note = {The physical properties of devices made of printed nanosheets and nanowires are determined by their intrinsic nanostructured network morphology. Here, the authors use FIB-SEM nanotomography to quantitatively analyze printed nanostructured networks via 3D reconstructions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Probing the critical nucleus size in tetrahydrofuran clathrate hydrate formation using surface-anchored nanoparticles},

author = {Han Xue and Linhai Li and Yiqun Wang and Youhua Lu and Kai Cui and Zhiyuan He and Guoying Bai and Jie Liu and Xin Zhou and Jianjun Wang },

url = {https://www.nature.com/articles/s41467-023-44378-6.pdf},

doi = {10.1038/s41467-023-44378-6},

year  = {2024},

date = {2024-01-02},

urldate = {2024-01-02},

journal = {Nature Communications},

volume = {15},

number = {157},

abstract = {Controlling the formation of clathrate hydrates is crucial for advancing hydrate-based technologies. However, the microscopic mechanism underlying clathrate hydrate formation through nucleation remains poorly elucidated. Specifically, the critical nucleus, theorized as a pivotal step in nucleation, lacks empirical validation. Here, we report uniform nanoparticles, e.g., graphene oxide (GO) nanosheets and gold or silver nanocubes with controlled sizes, as nanoprobes to experimentally measure the size of the critical nucleus of tetrahydrofuran (THF) clathrate hydrate formation. The capability of the nanoparticles in facilitating THF clathrate hydrate nucleation displays generally an abrupt change at a nanoparticle-size-determined specific supercooling. It is revealed that the free-energy barrier shows an abrupt change when the nanoparticles have an approximately the same size as that of the critical nucleus. Thus, it is inferred that THF clathrate hydrate nucleation involves the creation of a critical nucleus with its size being inversely proportional to the supercooling. By proving the existence and determining the supercooling-dependent size of the critical nucleus of the THF clathrate hydrates, this work brings insights in the microscopic pictures of the clathrate hydrate nucleation.},

note = {The critical nucleus, which considered a key step in the formation of clathrate hydrates, has not yet been empirically confirmed. Here, the authors probe the critical nucleus size in clathrate formation of tetrahydrofuran and thus provide mechanistic insights.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fast free energy estimates from λ-dynamics with bias-updated Gibbs sampling},

author = {Michael T. Robo and Ryan L. Hayes and Xinqiang Ding and Brian Pulawski and Jonah Z. Vilseck },

url = {https://www.nature.com/articles/s41467-023-44208-9.pdf},

doi = {10.1038/s41467-023-44208-9},

year  = {2023},

date = {2023-12-21},

urldate = {2023-12-21},

journal = {Nature Communications},

volume = {14},

number = {8515},

abstract = {Relative binding free energy calculations have become an integral computational tool for lead optimization in structure-based drug design. Classical alchemical methods, including free energy perturbation or thermodynamic integration, compute relative free energy differences by transforming one molecule into another. However, these methods have high operational costs due to the need to perform many pairwise perturbations independently. To reduce costs and accelerate molecular design workflows, we present a method called λ-dynamics with bias-updated Gibbs sampling. This method uses dynamic biases to continuously sample between multiple ligand analogues collectively within a single simulation. We show that many relative binding free energies can be determined quickly with this approach without compromising accuracy. For five benchmark systems, agreement to experiment is high, with root mean square errors near or below 1.0 kcal mol−1. Free energy results are consistent with other computational approaches and within statistical noise of both methods (0.4 kcal mol−1 or less). Notably, large efficiency gains over thermodynamic integration of 18–66-fold for small perturbations and 100–200-fold for whole aromatic ring substitutions are observed. The rapid determination of relative binding free energies will enable larger chemical spaces to be more readily explored and structure-based drug design to be accelerated.},

note = {Calculations of relative binding free energy are crucial for lead optimization in structure-based drug design, but classical methods are computationally expensive. Here, the authors describe a more efficient method for calculating the free energy that is as accurate as thermodynamic integration.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Janus particles with tunable patch symmetry and their assembly into chiral colloidal clusters},

author = {Tianran Zhang and Dengping Lyu and Wei Xu and Xuan Feng and Ran Ni and Yufeng Wang },

url = {https://www.nature.com/articles/s41467-023-44154-6.pdf},

doi = {10.1038/s41467-023-44154-6},

year  = {2023},

date = {2023-12-20},

urldate = {2023-12-20},

journal = {Nature Communications},

volume = {14},

number = {8494},

abstract = {Janus particles, which have an attractive patch on the otherwise repulsive surface, have been commonly employed for anisotropic colloidal assembly. While current methods of particle synthesis allow for control over the patch size, they are generally limited to producing dome-shaped patches with a high symmetry (C∞). Here, we report on the synthesis of Janus particles with patches of various tunable shapes, having reduced symmetries ranging from C2v to C3v and C4v. The Janus particles are synthesized by partial encapsulation of an octahedral metal-organic framework particle (UiO-66) in a polymer matrix. The extent of encapsulation is precisely regulated by a stepwise, asymmetric dewetting process that exposes selected facets of the UiO-66 particle. With depletion interaction, the Janus particles spontaneously assemble into colloidal clusters reflecting the particles’ shapes and patch symmetries. We observe the formation of chiral structures, whereby chirality emerges from achiral building blocks. With the ability to encode symmetry and directional bonding information, our strategy could give access to more complex colloidal superstructures through assembly.},

note = {Janus particles commonly exhibit a high-symmetry patch, constraining the range of possible assemblies. Here, the authors devise a synthetic approach to fine-tune the patch symmetry in Janus particles and showcase the assembly of these particles into chiral colloidal clusters.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Mechanically tunable organogels from highly charged polyoxometalate clusters loaded with fluorescent dyes},

author = {Fenghua Zhang and Zhong Li and Xun Wang },

url = {https://www.nature.com/articles/s41467-023-43989-3.pdf},

doi = {10.1038/s41467-023-43989-3},

year  = {2023},

date = {2023-12-14},

urldate = {2023-12-14},

journal = {Nature Communications},

volume = {14},

number = {8327},

abstract = {Inorganic nanowires-based organogel, a class of emerging organogel with convenient preparation, recyclability, and excellent mechanical properties, is in its infancy. Solidifying and functionalizing nanowires-based organogels by designing the gelator structure remains challenging. Here, we fabricate Ca2-P2W16 and Ca2-P2W15M nanowires utilizing highly charged [Ca2P2W16O60]10− and [Ca2P2W15MO60]14−/13− cluster units, respectively, which are then employed for preparing organogels. The mechanical performance and stability of prepared organogels are improved due to the enhanced interactions between nanowires and locked organic molecules. Compressive stress and tensile stress of Ca2-P2W16 nanowires-based organogel reach 34.5 and 29.0 kPa, respectively. The critical gel concentration of Ca2-P2W16 nanowires is as low as 0.28%. Single-molecule force spectroscopy confirms that the connections between cluster units and linkers can regulate the flexibility of nanowires. Furthermore, the incorporation of fluorophores into the organogels adds fluorescence properties. This work reveals the relationships between the microstructures of inorganic gelators and the properties of organogels, guiding the synthesis of high-performance and functional organogels.},

note = {Functionalizing inorganic organogels is a challenge and can have a negative impact on their mechanical properties. Here, the authors present nanowire-based organogels based on highly charged polyoxometalate cluster units that are mechanically tuned and loaded with fluorescent dyes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Hot luminescence from single-molecule chromophores electrically and mechanically self-decoupled by tripodal scaffolds},

author = {Vibhuti Rai and Nico Balzer and Gabriel Derenbach and Christof Holzer and Marcel Mayor and Wulf Wulfhekel and Lukas Gerhard and Michal Valášek },

url = {https://www.nature.com/articles/s41467-023-43948-y.pdf},

doi = {10.1038/s41467-023-43948-y},

year  = {2023},

date = {2023-12-12},

urldate = {2023-12-12},

journal = {Nature Communications},

volume = {14},

number = {8253},

abstract = {Control over the electrical contact to an individual molecule is one of the biggest challenges in molecular optoelectronics. The mounting of individual chromophores on extended tripodal scaffolds enables both efficient electrical and mechanical decoupling of individual chromophores from metallic leads. Core-substituted naphthalene diimides fixed perpendicular to a gold substrate by a covalently attached extended tripod display high stability with well-defined and efficient electroluminescence down to the single-molecule level. The molecularly controlled spatial arrangement balances the electric conduction for electroluminescence and the insulation to avoid non-radiative carrier recombination, enabling the spectrally and spatially resolved electroluminescence of individual self-decoupled chromophores in a scanning tunneling microscope. Hot luminescence bands are even visible in single self-decoupled chromophores, documenting the mechanical decoupling between the vibrons of the chromophore and the substrate.},

note = {A fundamental challenge for molecular electronics is the change in photophysical properties of molecules upon direct electrical contact. Here, the authors observe hot luminescence emitted by single-molecule chromophores that are electrically and mechanically self-decoupled by a tripodal scaffold.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Plasmonic metasurfaces of cellulose nanocrystal matrices with quadrants of aligned gold nanorods for photothermal anti-icing},

author = {Jeongsu Pyeon and Soon Mo Park and Juri Kim and Jeong-Hwan Kim and Yong-Jin Yoon and Dong Ki Yoon and Hyoungsoo Kim },

url = {https://www.nature.com/articles/s41467-023-43511-9.pdf},

doi = {10.1038/s41467-023-43511-9},

year  = {2023},

date = {2023-12-08},

urldate = {2023-12-08},

journal = {Nature Communications},

volume = {14},

number = {8096},

abstract = {Cellulose nanocrystals (CNCs) are intriguing as a matrix for plasmonic metasurfaces made of gold nanorods (GNRs) because of their distinctive properties, including renewability, biodegradability, non-toxicity, and low cost. Nevertheless, it is very difficult to precisely regulate the positioning and orientation of CNCs on the substrate in a consistent pattern. In this study, CNCs and GNRs, which exhibit tunable optical and anti-icing capabilities, are employed to manufacture a uniform plasmonic metasurface using a drop-casting technique. Two physical phenomena—(i) spontaneous and rapid self-dewetting and (ii) evaporation-induced self-assembly—are used to accomplish this. Additionally, we improve the CNC-GNR ink composition and determine the crucial coating parameters necessary to balance the two physical mechanisms in order to produce thin films without coffee rings. The final homogeneous CNC-GNR film has consistent annular ring patterns with plasmonic quadrant hues that are properly aligned, which enhances plasmonic photothermal effects. The CNC-GNR multi-array platform offers above-zero temperatures on a substrate that is subcooled below the freezing point. The current study presents a physicochemical approach for functional nanomaterial-based CNC control.},

note = {Cellulose nanocrystals are very attractive as a matrix material for plasmonic nanoparticles, but controlling particle orientation for patterning is challenging. Here, the authors prepare annular ring patterns with quadrants of aligned gold nanorods for photothermal applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Direct probing of single-molecule chemiluminescent reaction dynamics under catalytic conditions in solution},

author = {Ziqing Zhang and Jinrun Dong and Yibo Yang and Yuan Zhou and Yuang Chen and Yang Xu and Jiandong Feng},

url = {https://www.nature.com/articles/s41467-023-43640-1.pdf},

doi = {10.1038/s41467-023-43640-1},

year  = {2023},

date = {2023-12-02},

urldate = {2023-12-02},

journal = {Nature Communications},

volume = {14},

number = {7993},

abstract = {Chemical reaction kinetics can be evaluated by probing dynamic changes of chemical substrates or physical phenomena accompanied during the reaction process. Chemiluminescence, a light emitting exoenergetic process, involves random reaction positions and kinetics in solution that are typically characterized by ensemble measurements with nonnegligible average effects. Chemiluminescent reaction dynamics at the single-molecule level remains elusive. Here we report direct imaging of single-molecule chemiluminescent reactions in solution and probing of their reaction dynamics under catalytic conditions. Double-substrate Michaelis–Menten type of catalytic kinetics is found to govern the single-molecule reaction dynamics in solution, and a heterogeneity is found among different catalyst particles and different catalytic sites on a single particle. We further show that single-molecule chemiluminescence imaging can be used to evaluate the thermodynamics of the catalytic system, resolving activation energy at the single-particle level. Our work provides fundamental insights into chemiluminescent reactions and offers an efficient approach for evaluating catalysts.},

note = {Research into the dynamics of chemical reactions at the single-molecule level is a pivotal undertaking. Here, the authors present a direct investigation of the chemiluminescent reaction dynamics of single molecules in solution, providing spatiotemporally resolved insights into chemical reactions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Local probe-induced structural isomerization in a one-dimensional molecular array},

author = {Shigeki Kawai and Orlando J. Silveira and Lauri Kurki and Zhangyu Yuan and Tomohiko Nishiuchi and Takuya Kodama and Kewei Sun and Oscar Custance and Jose L. Lado and Takashi Kubo and Adam S. Foster },

url = {https://www.nature.com/articles/s41467-023-43659-4.pdf},

doi = {10.1038/s41467-023-43659-4},

year  = {2023},

date = {2023-11-25},

urldate = {2023-11-25},

journal = {Nature Communications},

volume = {14},

number = {7741},

abstract = {Synthesis of one-dimensional molecular arrays with tailored stereoisomers is challenging yet has great potential for application in molecular opto-, electronic- and magnetic-devices, where the local array structure plays a decisive role in the functional properties. Here, we demonstrate the construction and characterization of dehydroazulene isomer and diradical units in three-dimensional organometallic compounds on Ag(111) with a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. Tip-induced voltage pulses firstly result in the formation of a diradical species via successive homolytic fission of two C-Br bonds in the naphthyl groups, which are subsequently transformed into chiral dehydroazulene moieties. The delicate balance of the reaction rates among the diradical and two stereoisomers, arising from an in-line configuration of tip and molecular unit, allows directional azulene-to-azulene and azulene-to-diradical local probe structural isomerization in a controlled manner. Furthermore, our theoretical calculations suggest that the diradical moiety hosts an open-shell singlet with antiferromagnetic coupling between the unpaired electrons, which can undergo an inelastic spin transition of 91 meV to the ferromagnetically coupled triplet state.},

note = {Achieving unit-by-unit isomerization within a molecular array poses a significant challenge in chemistry. Here, the authors demonstrate tip-induced stereoisomerization of dehydroazulene and diradical units in three-dimensional organometallic compounds on Ag(111).},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The role of halogens in Au–S bond cleavage for energy-differentiated catalysis at the single-bond limit},

author = {Peihui Li and Songjun Hou and Qingqing Wu and Yijian Chen and Boyu Wang and Haiyang Ren and Jinying Wang and Zhaoyi Zhai and Zhongbo Yu and Colin J. Lambert and Chuancheng Jia and Xuefeng Guo },

url = {https://www.nature.com/articles/s41467-023-43639-8.pdf},

doi = {10.1038/s41467-023-43639-8},

year  = {2023},

date = {2023-11-24},

urldate = {2023-11-24},

journal = {Nature Communications},

volume = {14},

number = {7695},

abstract = {The transformation from one compound to another involves the breaking and formation of chemical bonds at the single-bond level, especially during catalytic reactions that are of great significance in broad fields such as energy conversion, environmental science, life science and chemical synthesis. The study of the reaction process at the single-bond limit is the key to understanding the catalytic reaction mechanism and further rationally designing catalysts. Here, we develop a method to monitor the catalytic process from the perspective of the single-bond energy using high-resolution scanning tunneling microscopy single-molecule junctions. Experimental and theoretical studies consistently reveal that the attack of a halogen atom on an Au atom can reduce the breaking energy of Au−S bonds, thereby accelerating the bond cleavage reaction and shortening the plateau length during the single-molecule junction breaking. Furthermore, the distinction in catalytic activity between different halogen atoms can be compared as well. This study establishes the intrinsic relationship among the reaction activation energy, the chemical bond breaking energy and the single-molecule junction breaking process, strengthening our mastery of catalytic reactions towards precise chemistry.},

note = {Investigation of the reaction process at the single-bond interface is key to understanding the catalytic reaction mechanism. Here, the authors develop a STM-BJ method to monitor the catalytic process from the perspective of single-bond energy.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Engineering chirality at wafer scale with ordered carbon nanotube architectures},

author = {Jacques Doumani and Minhan Lou and Oliver Dewey and Nina Hong and Jichao Fan and Andrey Baydin and Keshav Zahn and Yohei Yomogida and Kazuhiro Yanagi and Matteo Pasquali and Riichiro Saito and Junichiro Kono and Weilu Gao },

url = {https://www.nature.com/articles/s41467-023-43199-x.pdf},

doi = {10.1038/s41467-023-43199-x},

year  = {2023},

date = {2023-11-15},

urldate = {2023-11-15},

journal = {Nature Communications},

volume = {14},

number = {7380},

abstract = {Creating artificial matter with controllable chirality in a simple and scalable manner brings new opportunities to diverse areas. Here we show two such methods based on controlled vacuum filtration - twist stacking and mechanical rotation - for fabricating wafer-scale chiral architectures of ordered carbon nanotubes (CNTs) with tunable and large circular dichroism (CD). By controlling the stacking angle and handedness in the twist-stacking approach, we maximize the CD response and achieve a high deep-ultraviolet ellipticity of 40 ± 1 mdeg nm−1. Our theoretical simulations using the transfer matrix method reproduce the experimentally observed CD spectra and further predict that an optimized film of twist-stacked CNTs can exhibit an ellipticity as high as 150 mdeg nm−1, corresponding to a g factor of 0.22. Furthermore, the mechanical rotation method not only accelerates the fabrication of twisted structures but also produces both chiralities simultaneously in a single sample, in a single run, and in a controllable manner. The created wafer-scale objects represent an alternative type of synthetic chiral matter consisting of ordered quantum wires whose macroscopic properties are governed by nanoscopic electronic signatures and can be used to explore chiral phenomena and develop chiral photonic and optoelectronic devices.},

note = {Methods for generating macroscopic chiral matter struggle with limited scalability. Here, the authors show two vacuum filtration methods - twist stacking and mechanical rotation - to align carbon nanotubes into chiral structures at wafer scale with tunable circular dichroism.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Accessible hotspots for single-protein SERS in DNA-origami assembled gold nanorod dimers with tip-to-tip alignment},

author = {Francis Schuknecht and Karol Kołątaj and Michael Steinberger and Tim Liedl and Theobald Lohmueller },

url = {https://www.nature.com/articles/s41467-023-42943-7.pdf},

doi = {10.1038/s41467-023-42943-7},

year  = {2023},

date = {2023-11-08},

urldate = {2023-11-08},

journal = {Nature Communications},

volume = {14},

number = {7192},

abstract = {The label-free identification of individual proteins from liquid samples by surface-enhanced Raman scattering (SERS) spectroscopy is a highly desirable goal in biomedical diagnostics. However, the small Raman scattering cross-section of most (bio-)molecules requires a means to strongly amplify their Raman signal for successful measurement, especially for single molecules. This amplification can be achieved in a plasmonic hotspot that forms between two adjacent gold nanospheres. However, the small (≈1−2 nm) gaps typically required for single-molecule measurements are not accessible for most proteins. A useful strategy would thus involve dimer structures with gaps large enough to accommodate single proteins, whilst providing sufficient field enhancement for single-molecule SERS. Here, we report on using a DNA origami scaffold for tip-to-tip alignment of gold nanorods with an average gap size of 8 nm. The gaps are accessible to streptavidin and thrombin, which are captured at the plasmonic hotspot by specific anchoring sites on the origami template. The field enhancement achieved for the nanorod dimers is sufficient for single-protein SERS spectroscopy with sub-second integration times. This design for SERS probes composed of DNA origami with accessible hotspots promotes future use for single-molecule biodiagnostics in the near-infrared range.},

note = {The identification of individual proteins is highly desirable in diagnostics. Here, the authors report on DNA-origami assembled dimers of gold nanorod with accessible hotspots to capture and identify single proteins from solution by SERS.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Real-time signal processing via chemical reactions for a microfluidic molecular communication system},

author = {Vivien Walter and Dadi Bi and Ali Salehi-Reyhani and Yansha Deng },

url = {https://www.nature.com/articles/s41467-023-42885-0.pdf},

doi = {10.1038/s41467-023-42885-0},

year  = {2023},

date = {2023-11-08},

urldate = {2023-11-08},

journal = {Nature Communications},

volume = {14},

number = {7188},

abstract = {Signal processing over the molecular domain is critical for analysing, modifying, and synthesising chemical signals in molecular communication systems. However, the lack of chemical signal processing blocks and the wide use of electronic devices to process electrical signals in existing molecular communication platforms can hardly meet the biocompatible, non-invasive, and size-miniaturised requirements of applications in various fields, e.g., medicine, biology, and environment sciences. To tackle this, here we design and construct a liquid-based microfluidic molecular communication platform for performing chemical concentration signal processing and digital signal transmission over distances. By specifically designing chemical reactions and microfluidic geometry, the transmitter of our platform is capable of shaping the emitted signals, and the receiver is able to threshold, amplify, and detect the chemical signals after propagation. By encoding bit information into the concentration of sodium hydroxide, we demonstrate that our platform can achieve molecular signal modulation and demodulation functionalities, and reliably transmit text messages over long distances. This platform is further optimised to maximise data rate while minimising communication error. The presented methodology for real-time chemical signal processing can enable the implementation of signal processing units in biological settings and then unleash its potential for interdisciplinary applications.},

note = {The use of electronic devices to process electrical signals in molecular communications can hardly realize its potential for various applications. Here, the authors report on chemical concentration signal processing in real time and digital signal transmission over distances.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {High-speed mapping of surface charge dynamics using sparse scanning Kelvin probe force microscopy},

author = {Marti Checa and Addis S. Fuhr and Changhyo Sun and Rama Vasudevan and Maxim Ziatdinov and Ilia Ivanov and Seok Joon Yun and Kai Xiao and Alp Sehirlioglu and Yunseok Kim and Pankaj Sharma and Kyle P. Kelley and Neus Domingo and Stephen Jesse and Liam Collins },

url = {https://www.nature.com/articles/s41467-023-42583-x.pdf},

doi = {10.1038/s41467-023-42583-x},

year  = {2023},

date = {2023-11-08},

urldate = {2023-11-08},

journal = {Nature Communications},

volume = {14},

number = {7196},

abstract = {Unraveling local dynamic charge processes is vital for progress in diverse fields, from microelectronics to energy storage. This relies on the ability to map charge carrier motion across multiple length- and timescales and understanding how these processes interact with the inherent material heterogeneities. Towards addressing this challenge, we introduce high-speed sparse scanning Kelvin probe force microscopy, which combines sparse scanning and image reconstruction. This approach is shown to enable sub-second imaging (>3 frames per second) of nanoscale charge dynamics, representing several orders of magnitude improvement over traditional Kelvin probe force microscopy imaging rates. Bridging this improved spatiotemporal resolution with macroscale device measurements, we successfully visualize electrochemically mediated diffusion of mobile surface ions on a LaAlO3/SrTiO3 planar device. Such processes are known to impact band-alignment and charge-transfer dynamics at these heterointerfaces. Furthermore, we monitor the diffusion of oxygen vacancies at the single grain level in polycrystalline TiO2. Through temperature-dependent measurements, we identify a charge diffusion activation energy of 0.18 eV, in good agreement with previously reported values and confirmed by DFT calculations. Together, these findings highlight the effectiveness and versatility of our method in understanding ionic charge carrier motion in microelectronics or nanoscale material systems.},

note = {Dynamic mapping of charge motion across multiple length- and timescales is essential for understanding a variety of phenomena. Here, the authors introduce sparse scanning KPFM, which enables fast nanoscale charge mapping at 3 frames per second to track ion migration.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Direct time-resolved observation of surface-bound carbon dioxide radical anions on metallic nanocatalysts},

author = {Zhiwen Jiang and Carine Clavaguéra and Changjiang Hu and Sergey A. Denisov and Shuning Shen and Feng Hu and Jun Ma and Mehran Mostafavi },

url = {https://www.nature.com/articles/s41467-023-42936-6.pdf},

doi = {10.1038/s41467-023-42936-6},

year  = {2023},

date = {2023-11-06},

urldate = {2023-11-06},

journal = {Nature Communications},

volume = {14},

number = {7116},

abstract = {Time-resolved identification of surface-bound intermediates on metallic nanocatalysts is imperative to develop an accurate understanding of the elementary steps of CO2 reduction. Direct observation on initial electron transfer to CO2 to form surface-bound CO2•− radicals is lacking due to the technical challenges. Here, we use picosecond pulse radiolysis to generate CO2•− via aqueous electron attachment and observe the stabilization processes toward well-defined nanoscale metallic sites. The time-resolved method combined with molecular simulations identifies surface-bound intermediates with characteristic transient absorption bands and distinct kinetics from nanosecond to the second timescale for three typical metallic nanocatalysts: Cu, Au, and Ni. The interfacial interactions are further investigated by varying the important factors, such as catalyst size and the presence of cation in the electrolyte. This work highlights fundamental ultrafast spectroscopy to clarify the critical initial step in the CO2 catalytic reduction mechanism.},

note = {Understanding the activity and selectivity of metal catalysts requires elucidating the dynamics of CO2•− radicals bound to the surface. Here, the authors use pulse radiolysis to directly observe the stabilization process of CO2•− radicals at nanoscale metallic sites from nanoseconds to seconds.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Recastable assemblies of carbon dots into mechanically robust macroscopic materials},

author = {Bowen Sui and Youliang Zhu and Xuemei Jiang and Yifan Wang and Niboqia Zhang and Zhongyuan Lu and Bai Yang and Yunfeng Li },

url = {https://www.nature.com/articles/s41467-023-42516-8.pdf},

doi = {10.1038/s41467-023-42516-8},

year  = {2023},

date = {2023-10-24},

urldate = {2023-10-24},

journal = {Nature Communications},

volume = {14},

number = {6782},

abstract = {Assembly of nanoparticles into macroscopic materials with mechanical robustness, green processability, and recastable ability is an important and challenging task in materials science and nanotechnology. As an emerging nanoparticle with superior properties, macroscopic materials assembled from carbon dots will inherit their properties and further offer collective properties; however, macroscopic materials assembled from carbon dots solely remain unexplored. Here we report macroscopic films assembled from carbon dots modified by ureido pyrimidinone. These films show tunable fluorescence inherited from carbon dots. More importantly, these films exhibit collective properties including self-healing, re-castability, and superior mechanical properties, with Young’s modulus over 490 MPa and breaking strength over 30 MPa. The macroscopic films maintain original mechanical properties after several cycles of recasting. Through scratch healing and welding experiments, these films show good self-healing properties under mild conditions. Moreover, the molecular dynamics simulation reveals that the interplay of interparticle and intraparticle hydrogen bonding controls mechanical properties of macroscopic films. Notably, these films are processed into diverse shapes by an eco-friendly hydrosetting method. The methodology and results in this work shed light on the exploration of functional macroscopic materials assembled from nanoparticles and will accelerate innovative developments of nanomaterials in practical applications.},

note = {The assembly of nanoparticles into macroscopic materials forms the basis for various advanced material applications. Here, the authors develop macroscopic materials that are both recastable and mechanically robust, despite being composed purely of carbon dots.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Liquid spherical shells are a non-equilibrium steady state of active droplets},

author = {Alexander M. Bergmann and Jonathan Bauermann and Giacomo Bartolucci and Carsten Donau and 

Michele Stasi and Anna-Lena Holtmannspötter and Frank Jülicher and Christoph A. Weber and Job Boekhoven},

url = {https://www.nature.com/articles/s41467-023-42344-w.pdf},

doi = {10.1038/s41467-023-42344-w},

year  = {2023},

date = {2023-10-17},

urldate = {2023-10-17},

journal = {Nature Communications},

volume = {14},

number = {6552},

abstract = {Liquid-liquid phase separation yields spherical droplets that eventually coarsen to one large, stable droplet governed by the principle of minimal free energy. In chemically fueled phase separation, the formation of phase-separating molecules is coupled to a fuel-driven, non-equilibrium reaction cycle. It thus yields dissipative structures sustained by a continuous fuel conversion. Such dissipative structures are ubiquitous in biology but are poorly understood as they are governed by non-equilibrium thermodynamics. Here, we bridge the gap between passive, close-to-equilibrium, and active, dissipative structures with chemically fueled phase separation. We observe that spherical, active droplets can undergo a morphological transition into a liquid, spherical shell. We demonstrate that the mechanism is related to gradients of short-lived droplet material. We characterize how far out of equilibrium the spherical shell state is and the chemical power necessary to sustain it. Our work suggests alternative avenues for assembling complex stable morphologies, which might already be exploited to form membraneless organelles by cells.},

note = {Dissipative structures are governed by non-equilibrium thermodynamics. Here, the authors describe a size-dependent transition from active droplets to active spherical shells—a dissipative structure that arises from reaction diffusion gradients. },

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tunable encapsulation of sessile droplets with solid and liquid shells},

author = {Rutvik Lathia and Satchit Nagpal and Chandantaru Dey Modak and Satyarthi Mishra and Deepak Sharma and Bheema Sankar Reddy and Pavan Nukala and Ramray Bhat and Prosenjit Sen },

url = {https://www.nature.com/articles/s41467-023-41977-1.pdf},

doi = {10.1038/s41467-023-41977-1},

year  = {2023},

date = {2023-10-13},

urldate = {2023-10-13},

journal = {Nature Communications},

volume = {14},

number = {6445},

abstract = {Droplet encapsulations using liquid or solid shells are of significant interest in microreactors, drug delivery, crystallization, and cell growth applications. Despite progress in droplet-related technologies, tuning micron-scale shell thickness over a large range of droplet sizes is still a major challenge. In this work, we report capillary force assisted cloaking using hydrophobic colloidal particles and liquid-infused surfaces. The technique produces uniform solid and liquid shell encapsulations over a broad range (5–200 μm shell thickness for droplet volume spanning over four orders of magnitude). Tunable liquid encapsulation is shown to reduce the evaporation rate of droplets by up to 200 times with a wide tunability in lifetime (1.5 h to 12 days). Further, we propose using the technique for single crystals and cell/spheroid culture platforms. Stimuli-responsive solid shells show hermetic encapsulation with tunable strength and dissolution time. Moreover, scalability, and versatility of the technique is demonstrated for on-chip applications.},

note = {Encapsulated liquids are important for several microreactor applications, including (bio)chemistry in confined spaces. Here, the authors report on oil-infused particle shells that allow control of shell thickness, stability, and permeability for applications in crystal growth and cell cultivation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Overcrowding induces fast colloidal solitons in a slowly rotating potential landscape},

author = {Eric Cereceda-López and Alexander P. Antonov and Artem Ryabov and Philipp Maass and Pietro Tierno },

url = {https://www.nature.com/articles/s41467-023-41989-x.pdf},

doi = {10.1038/s41467-023-41989-x},

year  = {2023},

date = {2023-10-13},

urldate = {2023-10-13},

journal = {Nature Communications},

volume = {14},

number = {6448},

abstract = {Collective particle transport across periodic energy landscapes is ubiquitously present in many condensed matter systems spanning from vortices in high-temperature superconductors, frictional atomic sliding, driven skyrmions to biological and active matter. Here we report the emergence of fast solitons propagating against a rotating optical landscape. These experimentally observed solitons are stable cluster waves that originate from a coordinated particle exchange process which occurs when the number of trapped microparticles exceeds the number of potential wells. The size and speed of individual solitons rapidly increase with the particle diameter as predicted by theory and confirmed by numerical simulations. We show that when several solitons coexist, an effective repulsive interaction can stabilize their propagation along the periodic potential. Our experiments demonstrate a generic mechanism for cluster-mediated transport with potential applications to condensed matter systems on different length scales.},

note = {Solitons are peculiar waves propagating without changing their shape. Here, the authors show that colloidal particles in a rotating optical landscape create rapidly propagating solitons, formed by particle clusters through many-body interactions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Chemo-mechanical forces modulate the topology dynamics of mesoscale DNA assemblies},

author = {Deepak Karna and Eriko Mano and Jiahao Ji and Ibuki Kawamata and Yuki Suzuki and Hanbin Mao },

url = {https://www.nature.com/articles/s41467-023-41604-z.pdf},

doi = {10.1038/s41467-023-41604-z},

year  = {2023},

date = {2023-10-13},

urldate = {2023-10-13},

journal = {Nature Communications},

volume = {14},

number = {6459},

abstract = {The intrinsic complexity of many mesoscale (10–100 nm) cellular machineries makes it challenging to elucidate their topological arrangement and transition dynamics. Here, we exploit DNA origami nanospring as a model system to demonstrate that tens of piconewton linear force can modulate higher-order conformation dynamics of mesoscale molecular assemblies. By switching between two chemical structures (i.e., duplex and tetraplex DNA) in the junctions of adjacent origami modules, the corresponding stretching or compressing chemo-mechanical stress reversibly flips the backbone orientations of the DNA nanosprings. Both coarse-grained molecular dynamics simulations and atomic force microscopy measurements reveal that such a backbone conformational switch does not alter the right-handed chirality of the nanospring helix. This result suggests that mesoscale helical handedness may be governed by the torque, rather than the achiral orientation, of nanospring backbones. It offers a topology-based caging/uncaging concept to present chemicals in response to environmental cues in solution.},

note = {Understanding the topological arrangement and transition dynamics of mesoscale assemblies is complicated by their molecular complexity. Here, the authors use DNA origami nanosprings to show that mesoscale helical handedness is dictated by backbone torque rather than achiral orientation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Light-driven nucleation, growth, and patterning of biorelevant crystals using resonant near-infrared laser heating},

author = {Marloes H. Bistervels and Balázs Antalicz and Marko Kamp and Hinco Schoenmaker and Willem L. Noorduin },

url = {https://www.nature.com/articles/s41467-023-42126-4.pdf},

doi = {10.1038/s41467-023-42126-4},

year  = {2023},

date = {2023-10-10},

urldate = {2023-10-10},

journal = {Nature Communications},

volume = {14},

number = {6350},

abstract = {Spatiotemporal control over crystal nucleation and growth is of fundamental interest for understanding how organisms assemble high-performance biominerals, and holds relevance for manufacturing of functional materials. Many methods have been developed towards static or global control, however gaining simultaneously dynamic and local control over crystallization remains challenging. Here, we show spatiotemporal control over crystallization of retrograde (inverse) soluble compounds induced by locally heating water using near-infrared (NIR) laser light. We modulate the NIR light intensity to start, steer, and stop crystallization of calcium carbonate and laser-write with micrometer precision. Tailoring the crystallization conditions overcomes the inherently stochastic crystallization behavior and enables positioning single crystals of vaterite, calcite, and aragonite. We demonstrate straightforward extension of these principles toward other biorelevant compounds by patterning barium-, strontium-, and calcium carbonate, as well as strontium sulfate and calcium phosphate. Since many important compounds exhibit retrograde solubility behavior, NIR-induced heating may enable light-controlled crystallization with precise spatiotemporal control.},

note = {Natural biominerals deposit with precise spatial and temporal control, but such control is difficult to replicate artificially. Here, the authors start, steer, and stop the crystallization of biorelevant minerals by user-defined light patterns.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Photothermally heated colloidal synthesis of nanoparticles driven by silica-encapsulated plasmonic heat sources},

author = {Aritra Biswas and Nir Lemcoff and Ofir Shelonchik and Doron Yesodi and Elad Yehezkel and Ella Yonit Finestone and Alexander Upcher and Yossi Weizmann },

url = {https://www.nature.com/articles/s41467-023-42167-9.pdf},

doi = {10.1038/s41467-023-42167-9},

year  = {2023},

date = {2023-10-10},

urldate = {2023-10-10},

journal = {Nature Communications},

volume = {14},

number = {6355},

abstract = {Using photons to drive chemical reactions has become an increasingly important field of chemistry. Plasmonic materials can provide a means to introduce the energy necessary for nucleation and growth of nanoparticles by efficiently converting visible and infrared light to heat. Moreover, the formation of crystalline nanoparticles has yet to be included in the extensive list of plasmonic photothermal processes. Herein, we establish a light-assisted colloidal synthesis of iron oxide, silver, and palladium nanoparticles by utilizing silica-encapsulated gold bipyramids as plasmonic heat sources. Our work shows that the silica surface chemistry and localized thermal hotspot generated by the plasmonic nanoparticles play crucial roles in the formation mechanism, enabling nucleation and growth at temperatures considerably lower than conventional heating. Additionally, the photothermal method is extended to anisotropic geometries and can be applied to obtain intricate assemblies inaccessible otherwise. This study enables photothermally heated nanoparticle synthesis in solution through the plasmonic effect and demonstrates the potential of this methodology.},

note = {Photothermal solution heating with nanoscale heat sources is an efficient alternative to conventional heating methods. Here, the authors use silica-encapsulated gold nanoparticles to drive the colloidal synthesis of iron oxide, silver, and palladium nanoparticles at lower temperatures.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Chirality-induced avalanche magnetization of magnetite by an RNA precursor},

author = {S. Furkan Ozturk and Deb Kumar Bhowmick and Yael Kapon and Yutao Sang and Anil Kumar and Yossi Paltiel and Ron Naaman and Dimitar D. Sasselov },

url = {https://www.nature.com/articles/s41467-023-42130-8.pdf},

doi = {10.1038/s41467-023-42130-8},

year  = {2023},

date = {2023-10-10},

urldate = {2023-10-10},

journal = {Nature Communications},

volume = {14},

number = {6351},

abstract = {Homochirality is a hallmark of life on Earth. To achieve and maintain homochirality within a prebiotic network, the presence of an environmental factor acting as a chiral agent and providing a persistent chiral bias to prebiotic chemistry is highly advantageous. Magnetized surfaces are prebiotically plausible chiral agents due to the chiral-induced spin selectivity (CISS) effect, and they were utilized to attain homochiral ribose-aminooxazoline (RAO), an RNA precursor. However, natural magnetic minerals are typically weakly magnetized, necessitating mechanisms to enhance their magnetization for their use as effective chiral agents. Here, we report the magnetization of magnetic surfaces by crystallizing enantiopure RAO, whereby chiral molecules induce a uniform surface magnetization due to the CISS effect, which spreads across the magnetic surface akin to an avalanche. Chirality-induced avalanche magnetization enables a feedback between chiral molecules and magnetic surfaces, which can amplify a weak magnetization and allow for highly efficient spin-selective processes on magnetic minerals.},

note = {Homochirality, a key feature of life, has unknown origins. Magnetic mineral surfaces can act as chiral agents, but are only weakly magnetized by nature. Here, the authors report the uniform magnetization of magnetite by an RNA precursor that spreads across the surface like an avalanche.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Surfactant-free interfacial growth of graphdiyne hollow microspheres and the mechanistic origin of their SERS activity},

author = {Lu Zhang and Wencai Yi and Junfang Li and Guoying Wei and Guangcheng Xi and Lanqun Mao},

url = {https://www.nature.com/articles/s41467-023-42038-3.pdf},

doi = {10.1038/s41467-023-42038-3},

year  = {2023},

date = {2023-10-09},

urldate = {2023-10-09},

journal = {Nature Communications},

volume = {14},

number = {6318},

abstract = {As a two-dimensional carbon allotrope, graphdiyne possesses a direct band gap, excellent charge carrier mobility, and uniformly distributed pores. Here, a surfactant-free growth method is developed to efficiently synthesize graphdiyne hollow microspheres at liquid‒liquid interfaces with a self-supporting structure, which avoids the influence of surfactants on product properties. We demonstrate that pristine graphdiyne hollow microspheres, without any additional functionalization, show a strong surface-enhanced Raman scattering effect with an enhancement factor of 3.7 × 10^7 and a detection limit of 1 × 10^−12 M for rhodamine 6 G, which is approximately 1000 times that of graphene. Experimental measurements and first-principles density functional theory simulations confirm the hypothesis that the surface-enhanced Raman scattering activity can be attributed to an efficiency interfacial charge transfer within the graphdiyne-molecule system.},

note = {The 2D carbon allotrope graphdiyne possesses a direct band gap, high charge carrier mobility, and uniformly distributed pores. Here, the authors report the surfactant-free growth of graphdiyne hollow microspheres and investigate the origin of their SERS activity.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Crystal dissolution by particle detachment},

author = {Guomin Zhu and Benjamin A. Legg and Michel Sassi and Xinran Liang and Meirong Zong and Kevin M. Rosso and James J. De Yoreo },

url = {https://www.nature.com/articles/s41467-023-41443-y.pdf},

doi = {10.1038/s41467-023-41443-y},

year  = {2023},

date = {2023-10-09},

urldate = {2023-10-09},

journal = {Nature Communications},

volume = {14},

number = {6300},

abstract = {Crystal dissolution, which is a fundamental process in both natural and technological settings, has been predominately viewed as a process of ion-by-ion detachment into a surrounding solvent. Here we report a mechanism of dissolution by particle detachment (DPD) that dominates in mesocrystals formed via crystallization by particle attachment (CPA). Using liquid phase electron microscopy to directly observe dissolution of hematite crystals — both compact rhombohedra and mesocrystals of coaligned nanoparticles — we find that the mesocrystals evolve into branched structures, which disintegrate as individual sub-particles detach. The resulting dissolution rates far exceed those for equivalent masses of compact single crystals. Applying a numerical generalization of the Gibbs-Thomson effect, we show that the physical drivers of DPD are curvature and strain inherently tied to the original CPA process. Based on the generality of the model, we anticipate that DPD is widespread for both natural minerals and synthetic crystals formed via CPA.},

note = {Crystal dissolution has been predominately viewed as a process of ion-by-ion detachment into a surrounding solvent. Here, the authors report an alternative mechanism of dissolution by particle detachment.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Controlling piezoresistance in single molecules through the isomerisation of bullvalenes},

author = {Jeffrey R. Reimers and Tiexin Li and André P. Birvé and Likun Yang and Albert C. Aragonès and Thomas Fallon and Daniel S. Kosov and Nadim Darwish},

url = {https://www.nature.com/articles/s41467-023-41674-z.pdf},

doi = {10.1038/s41467-023-41674-z},

year  = {2023},

date = {2023-10-03},

urldate = {2023-10-03},

journal = {Nature Communications},

volume = {14},

number = {6089 },

abstract = {Nanoscale electro-mechanical systems (NEMS) displaying piezoresistance offer unique measurement opportunities at the sub-cellular level, in detectors and sensors, and in emerging generations of integrated electronic devices. Here, we show a single-molecule NEMS piezoresistor that operates utilising constitutional and conformational isomerisation of individual diaryl-bullvalene molecules and can be switched at 850 Hz. Observations are made using scanning tunnelling microscopy break junction (STMBJ) techniques to characterise piezoresistance, combined with blinking (current-time) experiments that follow single-molecule reactions in real time. A kinetic Monte Carlo methodology (KMC) is developed to simulate isomerisation on the experimental timescale, parameterised using density-functional theory (DFT) combined with non-equilibrium Green’s function (NEGF) calculations. Results indicate that piezoresistance is controlled by both constitutional and conformational isomerisation, occurring at rates that are either fast (equilibrium) or slow (non-equilibrium) compared to the experimental timescale. Two different types of STMBJ traces are observed, one typical of traditional experiments that are interpreted in terms of intramolecular isomerisation occurring on stable tipped-shaped metal-contact junctions, and another attributed to arise from junction‒interface restructuring induced by bullvalene isomerisation.},

note = {The quest for miniaturization of electromechanical nanosystems requires the use of single molecules as active components. Here, the authors develop a piezoresistor based on a single bullvalene molecule that changes its shape by a Cope rearrangement. },

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Guided anisotropic oxygen transport in vacancy ordered oxides},

author = {Zhenzhong Yang and Le Wang and Jeffrey A. Dhas and Mark H. Engelhard and Mark E. Bowden and Wen Liu and Zihua Zhu and Chongmin Wang and Scott A. Chambers and Peter V. Sushko and Yingge Du },

url = {https://www.nature.com/articles/s41467-023-40746-4.pdf},

doi = {10.1038/s41467-023-40746-4},

year  = {2023},

date = {2023-09-28},

urldate = {2023-09-28},

journal = {Nature Communications},

volume = {14},

number = {6068},

abstract = {Anisotropic and efficient transport of ions under external stimuli governs the operation and failure mechanisms of energy-conversion systems and microelectronics devices. However, fundamental understanding of ion hopping processes is impeded by the lack of atomically precise materials and probes that allow for the monitoring and control at the appropriate time- and length- scales. In this work, using in-situ transmission electron microscopy, we directly show that oxygen ion migration in vacancy ordered, semiconducting SrFeO2.5 epitaxial thin films can be guided to proceed through two distinctly different diffusion pathways, each resulting in different polymorphs of SrFeO2.75 with different ground electronic properties before reaching a fully oxidized, metallic SrFeO3 phase. The diffusion steps and reaction intermediates are revealed by means of ab-initio calculations. The principles of controlling oxygen diffusion pathways and reaction intermediates demonstrated here may advance the rational design of structurally ordered oxides for tailored applications and provide insights for developing devices with multiple states of regulation.},

note = {Control of ion diffusion is instrumental in understanding the behavior and structural transformations of transition metal oxides. Here, the authors use in-situ TEM to reveal the atomic-scale evolution of the topotactic phase transition in BM-SFO triggered by the migration of oxygen ions under an external stimulus.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Strong signature of electron-vibration coupling in molecules on Ag(111) triggered by tip-gated discharging},

author = {Chao Li and Christoph Kaspar and Ping Zhou and Jung-Ching Liu and Outhmane Chahib and Thilo Glatzel and Robert Häner and Ulrich Aschauer and Silvio Decurtins and Shi-Xia Liu and Michael Thoss and Ernst Meyer and Rémy Pawlak },

url = {https://www.nature.com/articles/s41467-023-41601-2.pdf},

doi = {10.1038/s41467-023-41601-2},

year  = {2023},

date = {2023-09-25},

urldate = {2023-09-25},

journal = {Nature Communications},

volume = {14},

number = {5956},

abstract = {Electron-vibration coupling is of critical importance for the development of molecular electronics, spintronics, and quantum technologies, as it affects transport properties and spin dynamics. The control over charge-state transitions and subsequent molecular vibrations using scanning tunneling microscopy typically requires the use of a decoupling layer. Here we show the vibronic excitations of tetrabromotetraazapyrene (TBTAP) molecules directly adsorbed on Ag(111) into an orientational glassy phase. The electron-deficient TBTAP is singly-occupied by an electron donated from the substrate, resulting in a spin 1/2 state, which is confirmed by a Kondo resonance. The TBTAP•− discharge is controlled by tip-gating and leads to a series of peaks in scanning tunneling spectroscopy. These occurrences are explained by combining a double-barrier tunneling junction with a Franck-Condon model including molecular vibrational modes. This work demonstrates that suitable precursor design enables gate-dependent vibrational excitations of molecules on a metal, thereby providing a method to investigate electron-vibration coupling in molecular assemblies without a decoupling layer.},

note = {Electron-vibration coupling is driving advances in molecular electronics, spintronics, and quantum technology. Here, the authors succeeded in directly controlling vibronic excitations in tetrabromotetraazapyrene (TBTAP) molecules on the surface of Ag(111).},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Identification of a common ice nucleus on hydrophilic and hydrophobic close-packed metal surfaces},

author = {Pengcheng Chen and Qiuhao Xu and Zijing Ding and Qing Chen and Jiyu Xu and Zhihai Cheng and Xiaohui Qiu and Bingkai Yuan and Sheng Meng and Nan Yao },

url = {https://www.nature.com/articles/s41467-023-41436-x.pdf},

doi = {10.1038/s41467-023-41436-x},

year  = {2023},

date = {2023-09-19},

urldate = {2023-09-19},

journal = {Nature Communications},

volume = {14},

number = {5813},

abstract = {Establishing a general model of heterogeneous ice nucleation has long been challenging because of the surface water structures found on different substrates. Identifying common water clusters, regardless of the underlying substrate, is one of the key steps toward solving this problem. Here, we demonstrate the presence of a common water cluster found on both hydrophilic Pt(111) and hydrophobic Cu(111) surfaces using scanning tunneling microscopy and non-contact atomic force microscopy. Water molecules self-assemble into a structure with a central flat-lying hexagon and three fused pentagonal rings, forming a cluster consisting of 15 individual water molecules. This cluster serves as a critical nucleus during ice nucleation on both surfaces: ice growth beyond this cluster bifurcates to form two-dimensional (three-dimensional) layers on hydrophilic (hydrophobic) surfaces. Our results reveal the inherent similarity and distinction at the initial stage of ice growth on hydrophilic and hydrophobic close-packed metal surfaces; thus, these observations provide initial evidence toward a general model for water-substrate interaction.},

note = {One key challenge in water science is to create a universal model that can predict the arrangement of water/solid interfaces. Here, the authors use STM and noncontact-AFM to discover common water clusters during the initial growth on hydrophilic and hydrophobic close-packed metal surfaces.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Epitaxial growth of metal-organic framework nanosheets into single-crystalline orthogonal arrays},

author = {Yingying Zou and Chao Liu and Chaoqi Zhang and Ling Yuan and Jiaxin Li and Tong Bao and Guangfeng Wei and Jin Zou and Chengzhong Yu },

url = {https://www.nature.com/articles/s41467-023-41517-x.pdf},

doi = {10.1038/s41467-023-41517-x},

year  = {2023},

date = {2023-09-18},

urldate = {2023-09-18},

journal = {Nature Communications},

volume = {14},

number = {5780},

abstract = {Construction of two-dimensional nanosheets into three-dimensional regular structures facilitates the mass transfer and exploits the maximum potential of two-dimensional building blocks in applications such as catalysis. Here, we report the synthesis of metal-organic frameworks with an orthogonal nanosheet array. The assembly involves the epitaxial growth of single crystalline metal-organic framework nanosheets with a naturally non-preferred facet exposure as the shell on a cubic metal-organic framework as the core. The nanosheets, despite of two typical shapes and crystallographic orientations, also form a single crystalline orthogonally arrayed framework. The density and size of nanosheets in the core-shell-structured composite metal-organic frameworks can be well adjusted. Moreover, metal-organic frameworks with a single composition and hollow orthogonal nanosheet array morphology can be obtained. Benefiting from the unusual facet exposure and macroporous structure, the designed structure exhibits improved electrocatalytic oxygen evolution activity compared to conventional nanosheets.},

note = {Constructing regular 3D superstructures from 2D nanosheets is a challenge. Here, the authors report the epitaxial growth of MOF nanosheets into single-crystalline orthogonal arrays with enhanced functional properties.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Charge-state lifetimes of single molecules on few monolayers of NaCl},

author = {Katharina Kaiser and Leonard-Alexander Lieske and Jascha Repp and Leo Gross 

},

url = {https://www.nature.com/articles/s41467-023-40692-1.pdf},

doi = {10.1038/s41467-023-40692-1},

year  = {2023},

date = {2023-08-17},

urldate = {2023-08-17},

journal = {Nature Communications},

volume = {14},

number = {4988},

abstract = {In molecular tunnel junctions, where the molecule is decoupled from the electrodes by few-monolayers-thin insulating layers, resonant charge transport takes place by sequential charge transfer to and from the molecule which implies transient charging of the molecule. The corresponding charge state transitions, which involve tunneling through the insulating decoupling layers, are crucial for understanding electrically driven processes such as electroluminescence or photocurrent generation in such a geometry. Here, we use scanning tunneling microscopy to investigate the decharging of single ZnPc and H2Pc molecules through NaCl films of 3 to 5 monolayers thickness on Cu(111) and Au(111). To this end, we approach the tip to the molecule at resonant tunnel conditions up to a regime where charge transport is limited by tunneling through the NaCl film. The resulting saturation of the tunnel current is a direct measure of the lifetimes of the anionic and cationic states, i.e., the molecule’s charge-state lifetime, and thus provides a means to study charge dynamics and, thereby, exciton dynamics. Comparison of anion and cation lifetimes on different substrates reveals the critical role of the level alignment with the insulator’s conduction and valence band, and the metal-insulator interface state.},

note = {Resonant charge transport to and from molecules and their corresponding charge-state transitions are critical to understanding electrically driven processes. Here, the authors investigate the charge-state lifetimes of single molecules through NaCl films of 3 to 5 monolayers thickness.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Interplay of structure and photophysics of individualized rod-shaped graphene quantum dots with up to 132 sp² carbon atoms},

author = {Daniel Medina-Lopez and Thomas Liu and Silvio Osella and Hugo Levy-Falk and Nicolas Rolland and Christine Elias and Gaspard Huber and Pranav Ticku and Loïc Rondin and Bruno Jousselme and David Beljonne and Jean-Sébastien Lauret and Stephane Campidelli},

url = {https://www.nature.com/articles/s41467-023-40376-w.pdf},

doi = {10.1038/s41467-023-40376-w},

year  = {2023},

date = {2023-08-07},

urldate = {2023-08-07},

journal = {Nature Communications},

volume = {14},

number = {4728},

abstract = {Nanographene materials are promising building blocks for the growing field of low-dimensional materials for optics, electronics and biophotonics applications. In particular, bottom-up synthesized 0D graphene quantum dots show great potential as single quantum emitters. To fully exploit their exciting properties, the graphene quantum dots must be of high purity; the key parameter for efficient purification being the solubility of the starting materials. Here, we report the synthesis of a family of highly soluble and easily processable rod-shaped graphene quantum dots with fluorescence quantum yields up to 94%. This is uncommon for a red emission. The high solubility is directly related to the design of the structure, allowing for an accurate description of the photophysical properties of the graphene quantum dots both in solution and at the single molecule level. These photophysical properties were fully predicted by quantum-chemical calculations.},

note = {The use and characterization of graphene quantum dots is limited by their pronounced tendency to form aggregates. Here, the authors synthesize rod-shaped motifs of nanographenes with up to 132 

sp² carbon atoms that are fully individualized, which allows the precise description of their intrinsic photophysical properties.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Chirality control of a single carbene molecule by tip-induced van der Waals interactions},

author = {Yunjun Cao and Joel Mieres-Perez and Julien Frederic Rowen and Elsa Sanchez-Garcia and Wolfram Sander and Karina Morgenstern },

url = {https://www.nature.com/articles/s41467-023-39870-y.pdf},

doi = {10.1038/s41467-023-39870-y},

year  = {2023},

date = {2023-07-26},

urldate = {2023-07-26},

journal = {Nature Communications},

volume = {14},

number = {4500},

abstract = {Non-covalent interactions such as van der Waals interactions and hydrogen bonds are crucial for the chiral induction and control of molecules, but it remains difficult to study them at the single-molecule level. Here, we report a carbene molecule on a copper surface as a prototype of an anchored molecule with a facile chirality change. We examine the influence of the attractive van der Waals interactions on the chirality change by regulating the tip-molecule distance, resulting in an excess of a carbene enantiomer. Our model study provides insight into the change of molecular chirality controlled by van der Waals interactions, which is fundamental for understanding the mechanisms of chiral induction and amplification.},

note = {The control of molecular chirality is of great interest in stereochemistry and biochemistry. Here, the authors show how to alter the chirality dynamics of a single molecule through tip-induced van der Waals interactions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Atomically precise nanoclusters predominantly seed gold nanoparticle syntheses},

author = {Liang Qiao and Nia Pollard and Ravithree D. Senanayake and Zhi Yang and Minjung Kim and Arzeena S. Ali and Minh Tam Hoang and Nan Yao and Yimo Han and Rigoberto Hernandez and Andre Z. Clayborne and Matthew R. Jones },

url = {https://www.nature.com/articles/s41467-023-40016-3.pdf},

doi = {10.1038/s41467-023-40016-3},

year  = {2023},

date = {2023-07-21},

urldate = {2023-07-21},

journal = {Nature Communications},

volume = {14},

number = {4408},

abstract = {Seed-mediated synthesis strategies, in which small gold nanoparticle precursors are added to a growth solution to initiate heterogeneous nucleation, are among the most prevalent, simple, and productive methodologies for generating well-defined colloidal anisotropic nanostructures. However, the size, structure, and chemical properties of the seeds remain poorly understood, which partially explains the lack of mechanistic understanding of many particle growth reactions. Here, we identify the majority component in the seed solution as an atomically precise gold nanocluster, consisting of a 32-atom Au core with 8 halide ligands and 12 neutral ligands constituting a bound ion pair between a halide and the cationic surfactant: Au32X8[AQA+•X-]12 (X = Cl, Br; AQA = alkyl quaternary ammonium). Ligand exchange is dynamic and versatile, occurring on the order of minutes and allowing for the formation of 48 distinct Au32 clusters with AQAX (alkyl quaternary ammonium halide) ligands. Anisotropic nanoparticle syntheses seeded with solutions enriched in Au32X8[AQA+•X-]12 show narrower size distributions and fewer impurity particle shapes, indicating the importance of this cluster as a precursor to the growth of well-defined nanostructures.},

note = {In seed-mediated synthesis, small particulate precursors are added to a growth solution to initiate heterogeneous nucleation, allowing access to well-defined colloidal nanostructures. Here, the authors identify that one of the most commonly studied seed solutions is populated by atomically precise gold nanoclusters with 32 atoms.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Diaryl-hemiindigos as visible light, pH, and heat responsive four-state switches and application in photochromic transparent polymers},

author = {Maximilian Sacherer and Frank Hampel and Henry Dube },

url = {https://www.nature.com/articles/s41467-023-39944-x.pdf},

doi = {10.1038/s41467-023-39944-x},

year  = {2023},

date = {2023-07-20},

urldate = {2023-07-20},

journal = {Nature Communications},

volume = {14},

number = {4382},

abstract = {Photoswitches are indispensable tools for responsive chemical nanosystems and are used today in almost all areas of the natural sciences. Hemiindigo (HI) derivatives have recently been introduced as potent photoswitches, but their full applicability has been hampered by the limited possibilities of their functionalization and structural modification. Here we report on a short and easy to diversify synthesis yielding diaryl-HIs bearing one additional aromatic residue at the central double bond. The resulting chromophores offer an advantageous property profile combining red-light responsiveness, high thermal bistability, strong isomer accumulations in both switching directions, strong photochromism, tunable acid responsiveness, and acid gating. With this progress, a broader structural realm becomes accessible for HI photoswitches, which can now be synthetically tailored for advanced future applications, e.g., in research on molecular machines and switches, in studies of photoisomerization mechanisms, or in the generation of smart and addressable materials. To showcase the potential of these distinct light-responsive molecular tools, we demonstrate four-state switching, chemical fueling, and reversible inscription into transparent polymers using green and red light as well as acid/base stimuli, in addition to a comprehensive photochemical study of all compounds.},

note = {Hemiindigo derivatives can act as photoswitches, but their applicability is limited by synthetic challenges. Here, the authors report the synthesis of modified photoswitches and demonstrate four-state switching, chemical fueling, and reversible inscription into transparent polymers.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Macroscopic photonic single crystals via seeded growth of DNA-coated colloids},

author = {Alexander Hensley and Thomas E. Videbæk and Hunter Seyforth and William M. Jacobs and W. Benjamin Rogers },

url = {https://www.nature.com/articles/s41467-023-39992-3.pdf},

doi = {10.1038/s41467-023-39992-3},

year  = {2023},

date = {2023-07-15},

urldate = {2023-07-15},

journal = {Nature Communications},

volume = {14},

number = {4237},

abstract = {Photonic crystals—a class of materials whose optical properties derive from their structure in addition to their composition—can be created by self-assembling particles whose sizes are comparable to the wavelengths of visible light. Proof-of-principle studies have shown that DNA can be used to guide the self-assembly of micrometer-sized colloidal particles into fully programmable crystal structures with photonic properties in the visible spectrum. However, the extremely temperature-sensitive kinetics of micrometer-sized DNA-functionalized particles has frustrated attempts to grow large, monodisperse crystals that are required for photonic metamaterial applications. Here we describe a robust two-step protocol for self-assembling single-domain crystals that contain millions of optical-scale DNA-functionalized particles: Monodisperse crystals are initially assembled in monodisperse droplets made by microfluidics, after which they are grown to macroscopic dimensions via seeded diffusion-limited growth. We demonstrate the generality of our approach by assembling different macroscopic single-domain photonic crystals with metamaterial properties, like structural coloration, that depend on the underlying crystal structure. By circumventing the fundamental kinetic traps intrinsic to crystallization of optical-scale DNA-coated colloids, we eliminate a key barrier to engineering photonic devices from DNA-programmed materials},

note = {DNA-programmed colloidal assembly of macroscopic crystals for photonic applications remains elusive. Here, the authors use insights from studies of nucleation and seeded growth to develop a two-step method for assembling macroscopic photonic crystals.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Dynamic imaging of interfacial electrochemistry on single Ag nanowires by azimuth-modulated plasmonic scattering interferometry},

author = {Gang Wu and Chen Qian and Wen-Li Lv and Xiaona Zhao and Xian-Wei Liu },

url = {https://www.nature.com/articles/s41467-023-39866-8.pdf},

doi = {10.1038/s41467-023-39866-8},

year  = {2023},

date = {2023-07-13},

urldate = {2023-07-13},

journal = {Nature Communications},

volume = {14},

number = {4194},

abstract = {Direct visualization of surface chemical dynamics in solution is essential for understanding the mechanisms involved in nanocatalysis and electrochemistry; however, it is challenging to achieve high spatial and temporal resolution. Here, we present an azimuth-modulated plasmonic imaging technique capable of imaging dynamic interfacial changes. The method avoids strong interference from reflected light and consequently eliminates the parabolic-like interferometric patterns in the images, allowing for a 67-fold increase in the spatial resolution of plasmonic imaging. We demonstrate that this optical imaging approach enables comprehensive analyses of surface chemical dynamics and identification of previously unknown surface reaction heterogeneity by investigating electrochemical redox reactions over single silver nanowires as an example. This work provides a general strategy for high-resolution plasmonic imaging of surface electrochemical dynamics and other interfacial chemical reactions, complementing existing surface characterization methods.},

note = {Direct visualization of the chemical dynamics of surfaces in solution is essential to gain mechanistic insights into nanocatalysis and electrochemistry. Here, the authors demonstrate the imaging of dynamic interfacial changes on a single nanowire during chemical reactions using azimuthally modulated plasmonic scattering interferometry.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Mesoporous multimetallic nanospheres with exposed highly entropic alloy sites},

author = {Yunqing Kang and Ovidiu Cretu and Jun Kikkawa and Koji Kimoto and Hiroki Nara and Asep Sugih Nugraha and Hiroki Kawamoto and Miharu Eguchi and Ting Liao and Ziqi Sun and Toru Asahi and Yusuke Yamauchi },

url = {https://www.nature.com/articles/s41467-023-39157-2.pdf},

doi = {10.1038/s41467-023-39157-2},

year  = {2023},

date = {2023-07-12},

urldate = {2023-07-12},

journal = {Nature Communications},

volume = {14},

number = {4182},

abstract = {Multimetallic alloys (MMAs) with various compositions enrich the materials library with increasing diversity and have received much attention in catalysis applications. However, precisely shaping MMAs in mesoporous nanostructures and mapping the distributions of multiple elements remain big challenge due to the different reduction kinetics of various metal precursors and the complexity of crystal growth. Here we design a one-pot wet-chemical reduction approach to synthesize core–shell motif PtPdRhRuCu mesoporous nanospheres (PtPdRhRuCu MMNs) using a diblock copolymer as the soft template. The PtPdRhRuCu MMNs feature adjustable compositions and exposed porous structures rich in highly entropic alloy sites. The formation processes of the mesoporous structures and the reduction and growth kinetics of different metal precursors of PtPdRhRuCu MMNs are revealed. The PtPdRhRuCu MMNs exhibit robust electrocatalytic hydrogen evolution reaction (HER) activities and low overpotentials of 10, 13, and 28 mV at a current density of 10 mA cm−2 in alkaline (1.0 M KOH), acidic (0.5 M H2SO4), and neutral (1.0 M phosphate buffer solution (PBS)) electrolytes, respectively. The accelerated kinetics of the HER in PtPdRhRuCu MMNs are derived from multiple compositions with synergistic interactions among various metal sites and mesoporous structures with excellent mass/electron transportation characteristics.},

note = {Nanostructured materials made from multimetal alloys are attractive for catalytic applications. Here, the authors propose a soft-templating approach to prepare mesoporous PtPdRhRuCu nanospheres that feature exposed porous structures rich in highly entropic alloy sites.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Thermometry on individual nanoparticles highlights the impact of bimetallic interfaces},

author = {Marta Quintanilla},

url = {https://www.nature.com/articles/s41467-023-38983-8.pdf},

doi = {10.1038/s41467-023-38983-8},

year  = {2023},

date = {2023-06-27},

urldate = {2023-06-27},

journal = {Nature Communications},

volume = {14},

number = {3812},

abstract = {A new study sheds light on the impact of bimetallic interfaces in nanomaterials for heat generation using single-particle thermometry. Moving from nanoparticle ensembles to single particles is key to developing consistent knowledge of material performance and nanoscale processes, but also involves assumptions and definitions that require careful consideration.},

note = {A new study sheds light on the impact of bimetallic interfaces in nanomaterials for heat generation using single-particle thermometry. Moving from nanoparticle ensembles to single particles is key to developing consistent knowledge of material performance and nanoscale processes, but also involves assumptions and definitions that require careful consideration.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Impact of bimetallic interface design on heat generation in plasmonic Au/Pd nanostructures studied by single-particle thermometry},

author = {Julian Gargiulo and Matias Herran and Ianina L. Violi and Ana Sousa-Castillo and Luciana P. Martinez and Simone Ezendam and Mariano Barella and Helene Giesler and Roland Grzeschik and Sebastian Schlücker and Stefan A. Maier and Fernando D. Stefani and Emiliano Cortés },

url = {https://www.nature.com/articles/s41467-023-38982-9.pdf},

doi = {10.1038/s41467-023-38982-9},

year  = {2023},

date = {2023-06-26},

urldate = {2023-06-26},

journal = {Nature Communications},

volume = {14},

number = {3813},

abstract = {Localized surface plasmons are lossy and generate heat. However, accurate measurement of the temperature of metallic nanoparticles under illumination remains an open challenge, creating difficulties in the interpretation of results across plasmonic applications. Particularly, there is a quest for understanding the role of temperature in plasmon-assisted catalysis. Bimetallic nanoparticles combining plasmonic with catalytic metals are raising increasing interest in artificial photosynthesis and the production of solar fuels. Here, we perform single-particle thermometry measurements to investigate the link between morphology and light-to-heat conversion of colloidal Au/Pd nanoparticles with two different configurations: core–shell and core-satellite. It is observed that the inclusion of Pd as a shell strongly reduces the photothermal response in comparison to the bare cores, while the inclusion of Pd as satellites keeps photothermal properties almost unaffected. These results contribute to a better understanding of energy conversion processes in plasmon-assisted catalysis.},

note = {The conversion of light into heat is a key process for plasmonic-catalytic applications. Here, the authors investigate how the design of the bimetallic interface affects the photothermal heating properties in Au/Pd nanostructures by applying thermometry at the single-particle level.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Halide-assisted differential growth of chiral nanoparticles with threefold rotational symmetry},

author = {Jiapeng Zheng and Christina Boukouvala and George R. Lewis and Yicong Ma and Yang Chen and Emilie Ringe and Lei Shao and Zhifeng Huang and Jianfang Wang },

url = {https://www.nature.com/articles/s41467-023-39456-8.pdf},

doi = {10.1038/s41467-023-39456-8},

year  = {2023},

date = {2023-06-25},

urldate = {2023-06-25},

journal = {Nature Communications},

volume = {14},

number = {3783},

abstract = {Enriching the library of chiral plasmonic nanoparticles that can be chemically mass-produced will greatly facilitate the applications of chiral plasmonics in areas ranging from constructing optical metamaterials to sensing chiral molecules and activating immune cells. Here we report on a halide-assisted differential growth strategy that can direct the anisotropic growth of chiral Au nanoparticles with tunable sizes and diverse morphologies. Anisotropic Au nanodisks are employed as seeds to yield triskelion-shaped chiral nanoparticles with threefold rotational symmetry and high dissymmetry factors. The averaged scattering g-factors of the L- and D-nanotriskelions are as large as 0.57 and − 0.49 at 650 nm, respectively. The Au nanotriskelions have been applied in chiral optical switching devices and chiral nanoemitters. We also demonstrate that the manipulation of the directional growth rate enables the generation of a variety of chiral morphologies in the presence of homochiral ligands.



},

note = {Expanding the library of chiral plasmonic nanoparticles will foster the development of chiroptical applications. Here, the authors apply halide-assisted differential growth to convert Au nanodisks into triskelion-shaped chiral nanoparticles with threefold rotational symmetry.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Formation mechanism of high-index faceted Pt-Bi alloy nanoparticles by evaporation-induced growth from metal salts},

author = {Kunmo Koo and Bo Shen and Sung-Il Baik and Zugang Mao and Paul J. M. Smeets and Ivan Cheuk and Kun He and Roberto dos Reis and Liliang Huang and Zihao Ye and Xiaobing Hu and Chad A. Mirkin and Vinayak P. Dravid },

url = {https://www.nature.com/articles/s41467-023-39458-6.pdf},

doi = {10.1038/s41467-023-39458-6},

year  = {2023},

date = {2023-06-24},

urldate = {2023-06-24},

journal = {Nature Communications},

volume = {14},

number = {3790},

abstract = {Nanoparticles with high-index facets are intriguing because such facets can lend the structure useful functionality, including enhanced catalytic performance and wide-ranging optical tunability. Ligand-free solid-state syntheses of high index-facet nanoparticles, through an alloying-dealloying process with foreign volatile metals, are attractive owing to their materials generality and high yields. However, the role of foreign atoms in stabilizing the high-index facets and the dynamic nature of the transformation including the coarsening and facet regulation process are still poorly understood. Herein, the transformation of Pt salts to spherical seeds and then to tetrahexahedra, is studied in situ via gas-cell transmission electron microscopy. The dynamic behaviors of the alloying and dealloying process, which involves the coarsening of nanoparticles and consequent facet regulation stage are captured in the real time with a nanoscale spatial resolution. Based on additional direct evidence obtained using atom probe tomography and density functional theory calculations, the underlying mechanisms of the alloying-dealloying process are uncovered, which will facilitate broader explorations of high-index facet nanoparticle synthesis.},

note = {Faceted nanoparticles with high-index planes exposed usually bear promising material functionalities. Here, the authors directly observe the coarsening and facet regulation process of tetrahexahedra Pt nanoparticles by using in-situ gas-phase TEM.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Coherent heteroepitaxial growth of I-III-VI2 Ag(In,Ga)S2 colloidal nanocrystals with near-unity quantum yield for use in luminescent solar concentrators},

author = {Hak June Lee and Seongbin Im and Dongju Jung and Kyuri Kim and Jong Ah Chae and Jaemin Lim and Jeong Woo Park and Doyoon Shin and Kookheon Char and Byeong Guk Jeong and Ji-Sang Park and Euyheon Hwang and Doh C. Lee and Young-Shin Park and Hyung-Jun Song and Jun Hyuk Chang and Wan Ki Bae },

url = {https://www.nature.com/articles/s41467-023-39509-y.pdf},

doi = {10.1038/s41467-023-39509-y},

year  = {2023},

date = {2023-06-23},

urldate = {2023-06-23},

journal = {Nature Communications},

volume = {14},

number = {3779},

abstract = {Colloidal Ag(In,Ga)S2 nanocrystals (AIGS NCs) with the band gap tunability by their size and composition within visible range have garnered surging interest. High absorption cross-section and narrow emission linewidth of AIGS NCs make them ideally suited to address the challenges of Cd-free NCs in wide-ranging photonic applications. However, AIGS NCs have shown relatively underwhelming photoluminescence quantum yield (PL QY) to date, primarily because coherent heteroepitaxy has not been realized. Here, we report the heteroepitaxy for AIGS-AgGaS2 (AIGS-AGS) core-shell NCs bearing near-unity PL QYs in almost full visible range (460 to 620 nm) and enhanced photochemical stability. Key to the successful growth of AIGS-AGS NCs is the use of the Ag-S-Ga(OA)2 complex, which complements the reactivities among cations for both homogeneous AIGS cores in various compositions and uniform AGS shell growth. The heteroepitaxy between AIGS and AGS results in the Type I heterojunction that effectively confines charge carriers within the emissive core without optically active interfacial defects. AIGS-AGS NCs show higher extinction coefficient and narrower spectral linewidth compared to state-of-the-art heavy metal-free NCs, prompting their immediate use in practicable applications including displays and luminescent solar concentrators (LSCs).},

note = {Colloidal semiconductor core-shell nanocrystals are sought after for photonic applications. Here, the authors report coherent heteroepitaxial growth of Ag(In,Ga)S2 core-shell nanocrystals with near-unity photoluminescence quantum yield across almost the full visible range.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Asymmetric transformation of achiral gold nanoclusters with negative nonlinear dependence between chiroptical activity and enantiomeric excess},

author = {Chang Liu and Yan Zhao and Tai-Song Zhang and Cheng-Bo Tao and Wenwen Fei and Sheng Zhang and Man-Bo Li },

url = {https://www.nature.com/articles/s41467-023-39462-w.pdf},

doi = {10.1038/s41467-023-39462-w},

year  = {2023},

date = {2023-06-22},

urldate = {2023-06-22},

journal = {Nature Communications},

volume = {14},

number = {3730},

abstract = {The investigation of chirality at the nanoscale is important to bridge the gap between molecular and macroscopic chirality. Atomically precise metal nanoclusters provide an ideal platform for this research, while their enantiopure preparation poses a challenge. Here, we describe an efficient approach to enantiopure metal nanoclusters via asymmetric transformation, that is, achiral Au23(SC6H11)16 nanoclusters are converted into chiral and enantiopure Au24(L)2(SC6H11)16 nanoclusters by a chiral inducer phosphoramidite (L). Two enantiomers of Au24(L)2(SC6H11)16 are obtained and the crystal structures reveal their hierarchical chirality, which originates from the two introduced chiral L molecules, the transformation-triggered asymmetric rearrangement of the staple motifs on the surface of the gold core, and the helical arrangement of nanocluster molecules. The construction of this type of enantiomerically pure nanoclusters is achieved based on the easy-to-synthesize and modular L. Lastly, the chirality-related chiroptical performance was investigated, revealing a negative nonlinear CD-ee dependence.},

note = {Atomically precise metal nanoclusters provide an ideal platform for studying chirality at the nanoscale. Here, the authors use a phosphoramidite ligand as a chiral inducer to asymmetrically transform achiral into chiral gold nanoclusters with negative nonlinear CD-ee dependence.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Artificial intelligence driven design of catalysts and materials for ring opening polymerization using a domain-specific language},

author = {Nathaniel H. Park and Matteo Manica and Jannis Born and James L. Hedrick and Tim Erdmann and Dmitry Yu. Zubarev and Nil Adell-Mill and Pedro L. Arrechea },

url = {https://www.nature.com/articles/s41467-023-39396-3.pdf},

doi = {10.1038/s41467-023-39396-3},

year  = {2023},

date = {2023-06-21},

urldate = {2023-06-21},

journal = {Nature Communications},

volume = {14},

number = {3686},

abstract = {Advances in machine learning (ML) and automated experimentation are poised to vastly accelerate research in polymer science. Data representation is a critical aspect for enabling ML integration in research workflows, yet many data models impose significant rigidity making it difficult to accommodate a broad array of experiment and data types found in polymer science. This inflexibility presents a significant barrier for researchers to leverage their historical data in ML development. Here we show that a domain specific language, termed Chemical Markdown Language (CMDL), provides flexible, extensible, and consistent representation of disparate experiment types and polymer structures. CMDL enables seamless use of historical experimental data to fine-tune regression transformer (RT) models for generative molecular design tasks. We demonstrate the utility of this approach through the generation and the experimental validation of catalysts and polymers in the context of ring-opening polymerization—although we provide examples of how CMDL can be more broadly applied to other polymer classes. Critically, we show how the CMDL tuned model preserves key functional groups within the polymer structure, allowing for experimental validation. These results reveal the versatility of CMDL and how it facilitates translation of historical data into meaningful predictive and generative models to produce experimentally actionable output.},

note = {Developing accessible polymeric materials is a challenging task for generative AI models. Here, the authors show that a domain-specific language enables the use of historical data to tune generative models to produce experimentally achievable material designs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Voltage-driven control of single-molecule keto-enol equilibrium in a two-terminal junction system},

author = {Chun Tang and Thijs Stuyver and Taige Lu and Junyang Liu and Yiling Ye and Tengyang Gao and Luchun Lin and Jueting Zheng and Wenqing Liu and Jia Shi and Sason Shaik and Haiping Xia and Wenjing Hong },

url = {https://www.nature.com/articles/s41467-023-39198-7.pdf},

doi = {10.1038/s41467-023-39198-7},

year  = {2023},

date = {2023-06-20},

urldate = {2023-06-20},

journal = {Nature Communications},

volume = {14},

number = {3657},

abstract = {Keto-enol tautomerism, describing an equilibrium involving two tautomers with distinctive structures, provides a promising platform for modulating nanoscale charge transport. However, such equilibria are generally dominated by the keto form, while a high isomerization barrier limits the transformation to the enol form, suggesting a considerable challenge to control the tautomerism. Here, we achieve single-molecule control of a keto-enol equilibrium at room temperature by using a strategy that combines redox control and electric field modulation. Based on the control of charge injection in the single-molecule junction, we could access charged potential energy surfaces with opposite thermodynamic driving forces, i.e., exhibiting a preference for the conducting enol form, while the isomerization barrier is also significantly reduced. Thus, we could selectively obtain desired and stable tautomers, which leads to significant modulation of the single-molecule conductance. This work highlights the concept of single-molecule control of chemical reactions on more than one potential energy surface.},

note = {Keto-enol tautomerism offers a promising platform for modulating charge transport at the nanoscale. Here, the authors show that the keto-enol equilibrium can be modulated on the single-molecule scale by controlling charge injection in a two-terminal junction system.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Collective photothermal bending of flexible organic crystals modified with MXene-polymer multilayers as optical waveguide arrays},

author = {Xuesong Yang and Linfeng Lan and Liang Li and Jinyang Yu and Xiaokong Liu and Ying Tao and Quan-Hong Yang and Panče Naumov and Hongyu Zhang },

url = {https://www.nature.com/articles/s41467-023-39162-5.pdf},

doi = {10.1038/s41467-023-39162-5},

year  = {2023},

date = {2023-06-19},

urldate = {2023-06-19},

journal = {Nature Communications},

volume = {14},

number = {3627},

abstract = {The performance of any engineering material is naturally limited by its structure, and while each material suffers from one or multiple shortcomings when considered for a particular application, these can be potentially circumvented by hybridization with other materials. By combining organic crystals with MXenes as thermal absorbers and charged polymers as adhesive counter-ionic components, we propose a simple access to flexible hybrid organic crystal materials that have the ability to mechanically respond to infrared light. The ensuing hybrid organic crystals are durable, respond fast, and can be cycled between straight and deformed state repeatedly without fatigue. The point of flexure and the curvature of the crystals can be precisely controlled by modulating the position, duration, and power of thermal excitation, and this control can be extended from individual hybrid crystals to motion of ordered two-dimensional arrays of such crystals. We also demonstrate that excitation can be achieved over very long distances (>3 m). The ability to control the shape with infrared light adds to the versatility in the anticipated applications of organic crystals, most immediately in their application as thermally controllable flexible optical waveguides for signal transmission in flexible organic electronics.},

note = {Organic crystals represent potential alternatives to silicon dioxide due to their high flexibility and controllable properties. Here, the authors prepared a hybrid organic crystal material that responds mechanically to infrared light.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Strain and crystallographic identification of the helically concaved gap surfaces of chiral nanoparticles},

author = {Sungwook Choi and Sang Won Im and Ji-Hyeok Huh and Sungwon Kim and Jaeseung Kim and Yae-Chan Lim and Ryeong Myeong Kim and Jeong Hyun Han and Hyeohn Kim and Michael Sprung and Su Yong Lee and Wonsuk Cha and Ross Harder and Seungwoo Lee and Ki Tae Nam and Hyunjung Kim },

url = {https://www.nature.com/articles/s41467-023-39255-1.pdf},

doi = {10.1038/s41467-023-39255-1},

year  = {2023},

date = {2023-06-17},

urldate = {2023-06-17},

journal = {Nature Communications},

volume = {14},

number = {3615 },

abstract = {Identifying the three-dimensional (3D) crystal plane and strain-field distributions of nanocrystals is essential for optical, catalytic, and electronic applications. However, it remains a challenge to image concave surfaces of nanoparticles. Here, we develop a methodology for visualizing the 3D information of chiral gold nanoparticles ≈ 200 nm in size with concave gap structures by Bragg coherent X-ray diffraction imaging. The distribution of the high-Miller-index planes constituting the concave chiral gap is precisely determined. The highly strained region adjacent to the chiral gaps is resolved, which was correlated to the 432-symmetric morphology of the nanoparticles and its corresponding plasmonic properties are numerically predicted from the atomically defined structures. This approach can serve as a comprehensive characterization platform for visualizing the 3D crystallographic and strain distributions of nanoparticles with a few hundred nanometers, especially for applications where structural complexity and local heterogeneity are major determinants, as exemplified in plasmonics.},

note = {Identifying the 3D crystal plane and strain field distributions of nanocrystals with concave surfaces is challenging. Here, the authors analyze the hidden concave gaps of chiral nanoparticles by using coherent Bragg X-ray diffraction imaging.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Nanowire-based smart windows combining electro- and thermochromics for dynamic regulation of solar radiation},

author = {Si-Zhe Sheng and Jin-Long Wang and Bin Zhao and Zhen He and Xue-Fei Feng and Qi-Guo Shang and Cheng Chen and Gang Pei and Jun Zhou and Jian-Wei Liu and Shu-Hong Yu },

url = {https://www.nature.com/articles/s41467-023-38353-4.pdf},

doi = {10.1038/s41467-023-38353-4},

year  = {2023},

date = {2023-06-03},

urldate = {2023-06-03},

journal = {Nature Communications},

volume = {14},

number = {3231},

abstract = {Smart window is an attractive option for efficient heat management to minimize energy consumption and improve indoor living comfort owing to their optical properties of adjusting sunlight. To effectively improve the sunlight modulation and heat management capability of smart windows, here, we propose a co-assembly strategy to fabricate the electrochromic and thermochromic smart windows with tunable components and ordered structures for the dynamic regulation of solar radiation. Firstly, to enhance both illumination and cooling efficiency in electrochromic windows, the aspect ratio and mixed type of Au nanorods are tuned to selectively absorb the near-infrared wavelength range of 760 to 1360 nm. Furthermore, when assembled with electrochromic W18O49 nanowires in the colored state, the Au nanorods exhibit a synergistic effect, resulting in a 90% reduction of near-infrared light and a corresponding 5 °C cooling effect under 1-sun irradiation. Secondly, to extend the fixed response temperature value to a wider range of 30–50 °C in thermochromic windows, the doping amount and mixed type of W-VO2 nanowires are carefully regulated. Last but not the least, the ordered assembly structure of the nanowires can greatly reduce the level of haze and enhance visibility in the windows.},

note = {Smart windows offer more efficient sunlight modulation and heat management. Here, the authors propose a co-assembly strategy to produce smart windows that combine electrochromic and thermochromic functions with tunable components and ordered structures for dynamic solar radiation regulation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Critical roles of metal–ligand complexes in the controlled synthesis of various metal nanoclusters},

author = {Ji Soo Kim and Hogeun Chang and Sungsu Kang and Seungwoo Cha and Hanguk Cho and Seung Jae Kwak and Namjun Park and Younhwa Kim and Dohun Kang and Chyan Kyung Song and Jimin Kwag and Ji-Sook Hahn and Won Bo Lee and Taeghwan Hyeon and Jungwon Park },

url = {https://www.nature.com/articles/s41467-023-38955-y.pdf},

doi = {10.1038/s41467-023-38955-y},

year  = {2023},

date = {2023-06-02},

urldate = {2023-06-02},

journal = {Nature Communications},

volume = {14},

number = {3201},

abstract = {Metal nanoclusters (NCs), an important class of nanoparticles (NPs), are extremely small in size and possess quasi-molecular properties. Due to accurate stoichiometry of constituent atoms and ligands, NCs have strong structure-property relationship. The synthesis of NCs is seemingly similar to that of NPs as both are formed by colloidal phase transitions. However, they are considerably different because of metal-ligand complexes in NC synthesis. Reactive ligands can convert metal salts to complexes, actual precursors to metal NCs. During the complex formation, various metal species occur, having different reactivity and fraction depending on synthetic conditions. It can alter their degree of participation in NC synthesis and the homogeneity of final products. Herein, we investigate the effects of complex formation on the entire NC synthesis. By controlling the fraction of various Au species showing different reactivity, we find that the extent of complex formation alters reduction kinetics and the uniformity of Au NCs. We demonstrate that this concept can be universally applied to synthesize Ag, Pt, Pd, and Rh NCs.},

note = {Metal-thiolate complexes are the precursors to atomically precise metal nanoclusters. Here, the authors show that the extent of metal-ligand interaction is key to controlling the size and uniformity in the synthesis of metal nanoclusters.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Probing the atomically diffuse interfaces in Pd@Pt core-shell nanoparticles in three dimensions},

author = {Zezhou Li and Zhiheng Xie and Yao Zhang and Xilong Mu and Jisheng Xie and Hai-Jing Yin and Ya-Wen Zhang and Colin Ophus and Jihan Zhou },

url = {https://www.nature.com/articles/s41467-023-38536-z.pdf},

doi = {10.1038/s41467-023-38536-z},

year  = {2023},

date = {2023-05-22},

urldate = {2023-05-22},

journal = {Nature Communications},

volume = {14},

number = {2934},

abstract = {Deciphering the three-dimensional atomic structure of solid-solid interfaces in core-shell nanomaterials is the key to understand their catalytical, optical and electronic properties. Here, we probe the three-dimensional atomic structures of palladium-platinum core-shell nanoparticles at the single-atom level using atomic resolution electron tomography. We quantify the rich structural variety of core-shell nanoparticles with heteroepitaxy in 3D at atomic resolution. Instead of forming an atomically-sharp boundary, the core-shell interface is found to be atomically diffuse with an average thickness of 4.2 Å, irrespective of the particle’s morphology or crystallographic texture. The high concentration of Pd in the diffusive interface is highly related to the free Pd atoms dissolved from the Pd seeds, which is confirmed by atomic images of Pd and Pt single atoms and sub-nanometer clusters using cryogenic electron microscopy. These results advance our understanding of core-shell structures at the fundamental level, providing potential strategies into precise nanomaterial manipulation and chemical property regulation.},

note = {Deciphering the structure and composition of bimetallic nanomaterial interfaces is key to understanding their properties. Here, the authors investigate the diffuse interfaces in Pd@Pt core-shell nanoparticles in 3D using electron tomography with atomic resolution.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Flattened 1D fragments of fullerene C60 that exhibit robustness toward multi-electron reduction},

author = {Masahiro Hayakawa and Naoyuki Sunayama and Shu I. Takagi and Yu Matsuo and Asuka Tamaki and Shigehiro Yamaguchi and Shu Seki and Aiko Fukazawa },

url = {https://www.nature.com/articles/s41467-023-38300-3.pdf},

doi = {10.1038/s41467-023-38300-3},

year  = {2023},

date = {2023-05-15},

urldate = {2023-05-15},

journal = {Nature Communications},

volume = {14},

number = {2741},

abstract = {Fullerenes are compelling molecular materials owing to their exceptional robustness toward multi-electron reduction. Although scientists have attempted to address this feature by synthesizing various fragment molecules, the origin of this electron affinity remains unclear. Several structural factors have been suggested, including high symmetry, pyramidalized carbon atoms, and five-membered ring substructures. To elucidate the role of the five-membered ring substructures without the influence of high symmetry and pyramidalized carbon atoms, we herein report the synthesis and electron-accepting properties of oligo(biindenylidene)s, a flattened one-dimensional fragment of fullerene C60. Electrochemical studies corroborated that oligo(biindenylidene)s can accept electrons up to equal to the number of five-membered rings in their main chains. Moreover, ultraviolet/visible/near-infrared absorption spectroscopy revealed that oligo(biindenylidene)s exhibit enhanced absorption covering the entire visible region relative to C60. These results highlight the significance of the pentagonal substructure for attaining stability toward multi-electron reduction and provide a strategy for the molecular design of electron-accepting π-conjugated hydrocarbons even without electron-withdrawing groups.},

note = {Fullerenes are compelling molecular materials, but the reason for their high robustness to multi-electron reduction is still debated.  Here, the authors synthesize flattened 1D fragments of fullerene C₆₀ with high robustness against multi-electron reduction.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {High-resolution discrimination of homologous and isomeric proteinogenic amino acids in nanopore sensors with ultrashort single-walled carbon nanotubes},

author = {Weichao Peng and Shuaihu Yan and Ke Zhou and Hai-Chen Wu and Lei Liu and Yuliang Zhao },

url = {https://www.nature.com/articles/s41467-023-38399-4.pdf},

doi = {10.1038/s41467-023-38399-4},

year  = {2023},

date = {2023-05-09},

urldate = {2023-05-09},

journal = {Nature Communications},

volume = {14},

number = {2662},

abstract = {The hollow and tubular structure of single-walled carbon nanotubes (SWCNTs) makes them ideal candidates for making nanopores. However, the heterogeneity of SWCNTs hinders the fabrication of robust and reproducible carbon-based nanopore sensors. Here we develop a modified density gradient ultracentrifugation approach to separate ultrashort (≈5-10 nm) SWCNTs with a narrow conductance range and construct high-resolution nanopore sensors with those tubes inserted in lipid bilayers. By conducting ionic current recordings and fluorescent imaging of Ca2+ flux through different nanopores, we prove that the ion mobilities in SWCNT nanopores are 3-5 times higher than the bulk mobility. Furthermore, we employ SWCNT nanopores to discriminate homologue or isomeric proteinogenic amino acids, which are challenging tasks for other nanopore sensors. These successes, coupled with the building of SWCNT nanopore arrays, may constitute a crucial part of the recently burgeoning protein sequencing technologies.},

note = {Ultrashort single-walled carbon nanotubes inserted in lipid bilayers can be used as nanopore sensors. Here, the authors demonstrate the high-resolution discrimination of homologous and isomeric proteinogenic amino acids with such carbon-based nanopores.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Epitaxial growth of highly symmetrical branched noble metal-semiconductor heterostructures with efficient plasmon-induced hot-electron transfer},

author = {Li Zhai and Sara T. Gebre and Bo Chen and Dan Xu and Junze Chen and Zijian Li and Yawei Liu and Hua Yang and Chongyi Ling and Yiyao Ge and Wei Zhai and Changsheng Chen and Lu Ma and Qinghua Zhang and Xuefei Li and Yujie Yan and Xinyu Huang and Lujiang Li and Zhiqiang Guan and Chen-Lei Tao and Zhiqi Huang and Hongyi Wang and Jinze Liang and Ye Zhu and Chun-Sing Lee and Peng Wang and Chunfeng Zhang and Lin Gu and Yonghua Du and Tianquan Lian and Hua Zhang and Xue-Jun Wu },

url = {https://www.nature.com/articles/s41467-023-38237-7.pdf},

doi = {10.1038/s41467-023-38237-7},

year  = {2023},

date = {2023-05-03},

urldate = {2023-05-03},

journal = {Nature Communications},

volume = {14},

number = {2538},

abstract = {Epitaxial growth is one of the most commonly used strategies to precisely tailor heterostructures with well-defined compositions, morphologies, crystal phases, and interfaces for various applications. However, as epitaxial growth requires a small interfacial lattice mismatch between the components, it remains a challenge for the epitaxial synthesis of heterostructures constructed by materials with large lattice mismatch and/or different chemical bonding, especially the noble metal-semiconductor heterostructures. Here, we develop a noble metal-seeded epitaxial growth strategy to prepare highly symmetrical noble metal-semiconductor branched heterostructures with desired spatial configurations, i.e., twenty CdS (or CdSe) nanorods epitaxially grown on twenty exposed (111) facets of Ag icosahedral nanocrystal, albeit a large lattice mismatch (more than 40%). Importantly, a high quantum yield (QY) of plasmon-induced hot-electron transferred from Ag to CdS was observed in epitaxial Ag-CdS icosapods (18.1%). This work demonstrates that epitaxial growth can be achieved in heterostructures composed of materials with large lattice mismatches. The constructed epitaxial noble metal-semiconductor interfaces could be an ideal platform for investigating the role of interfaces in various physicochemical processes.},

note = {Epitaxial growth of heterostructures composed of materials with large lattice mismatch is challenging. Here, the authors reported the epitaxy of II-VI semiconductor nanorods on plasmonic noble metal, despite a lattice mismatch of more than 40%.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Atomically precise gold nanoclusters at the molecular-to-metallic transition with intrinsic chirality from surface layers},

author = {Li-Juan Liu and Fahri Alkan and Shengli Zhuang and Dongyi Liu and Tehseen Nawaz and Jun Guo and Xiaozhou Luo and Jian He},

url = {https://www.nature.com/articles/s41467-023-38179-0.pdf},

doi = {10.1038/s41467-023-38179-0},

year  = {2023},

date = {2023-04-26},

urldate = {2023-04-26},

journal = {Nature Communications},

volume = {14},

number = {2397},

abstract = {The advances in determining the total structure of atomically precise metal nanoclusters have prompted extensive exploration into the origins of chirality in nanoscale systems. While chirality is generally transferrable from the surface layer to the metal–ligand interface and kernel, we present here an alternative type of gold nanoclusters (138 gold core atoms with 48 2,4-dimethylbenzenethiolate surface ligands) whose inner structures are not asymmetrically induced by chiral patterns of the outermost aromatic substituents. This phenomenon can be explained by the highly dynamic behaviors of aromatic rings in the thiolates assembled via π − π stacking and C − H···π interactions. In addition to being a thiolate-protected nanocluster with uncoordinated surface gold atoms, the reported Au138 motif expands the size range of gold nanoclusters having both molecular and metallic properties. Our current work introduces an important class of nanoclusters with intrinsic chirality from surface layers rather than inner structures and will aid in elucidating the transition of gold nanoclusters from their molecular to metallic states.},

note = {Chiral metal nanoclusters prepared from achiral ligands generally contain chiral kernel structures. Here, the authors report an alternative type of gold nanoclusters whose intrinsic chirality arises solely from the arrangement of the organic components on their surface.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Condensation and asymmetric amplification of chirality in achiral molecules adsorbed on an achiral surface},

author = {Huiru Liu and Heping Li and Yu He and Peng Cheng and Yi-Qi Zhang and Baojie Feng and Hui Li and Kehui Wu and Lan Chen },

url = {https://www.nature.com/articles/s41467-023-37904-z.pdf},

doi = {10.1038/s41467-023-37904-z},

year  = {2023},

date = {2023-04-13},

urldate = {2023-04-13},

journal = {Nature Communications},

volume = {14},

number = {2100},

abstract = {The origin of homochirality in nature is an important but open question. Here, we demonstrate a simple organizational chiral system constructed by achiral carbon monoxide (CO) molecules adsorbed on an achiral Au(111) substrate. Combining scanning tunneling microscope (STM) measurements with density-functional-theory (DFT) calculations, two dissymmetric cluster phases consisting of chiral CO heptamers are revealed. By applied high bias voltage, the stable racemic cluster phase can be transformed into a metastable uniform phase consisting of CO monomers. Further, during the recondensation of a cluster phase after lowering down bias voltage, an enantiomeric excess and its chiral amplification occur, resulting in a homochirality. Such asymmetry amplification is found to be both kinetically feasible and thermodynamically favorable. Our observations provide insight into the physicochemical origin of homochirality through surface adsorption and suggest a general phenomenon that can influence enantioselective chemical processes such as chiral separations and heterogeneous asymmetric catalysis.},

note = {The origin of homochirality in nature is an important but open question. Here, the authors provide insight into the physicochemical origin of homochirality through surface adsorption on the model of adlayers of achiral carbon monoxide molecules on an achiral Au(111) surface.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Nanoscale thermodynamics needs the concept of a disjoining chemical potential},

author = {Wei Dong},

url = {https://www.nature.com/articles/s41467-023-36970-7.pdf},

doi = {10.1038/s41467-023-36970-7},

year  = {2023},

date = {2023-04-01},

urldate = {2023-04-01},

journal = {Nature Communications},

volume = {14},

number = {1824},

abstract = {Disjoining pressure was discovered by Derjaguin in 1930’s, which describes the difference between the pressure of a strongly confined fluid and the corresponding one in a bulk phase. It has been revealed recently that the disjoining pressure is at the origin of distinct differential and integral surface tensions for strongly confined fluids. Here we show how the twin concept, disjoining chemical potential, arises in a reminiscent way although it comes out eighty years later. This twin concept advances our understanding of nanoscale thermodynamics. Ensemble-dependence (or environment-dependence) is one hallmark of thermodynamics of small systems. We show that integral surface tension is ensemble-dependent while differential surface tension is not. Moreover, two generalized Gibbs-Duhem equations involving integral surface tensions are derived, as well as two additional adsorption equations relating surface tensions to adsorption-induced strains. All the results obtained in this work further evidence that an approach alternative of Hill’s nanothermodynamics is possible, by extending Gibbs surface thermodynamics instead of resorting to Hill’s replica trick. Moreover, we find a compression-expansion hysteresis without any underlying phase transition.},

note = {Matter behaves differently at the nanoscale. Here, the author introduces the concept of a disjoining chemical potential for nanoscale thermodynamics, showing that thermodynamic functions depend on the environment, and suggests possible experimental verifications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Real-time insight into the multistage mechanism of nanoparticle exsolution from a perovskite host surface},

author = {Eleonora Calì and Melonie P. Thomas and Rama Vasudevan and Ji Wu and Oriol Gavalda-Diaz and Katharina Marquardt and Eduardo Saiz and Dragos Neagu and Raymond R. Unocic and Stephen C. Parker and Beth S. Guiton and David J. Payne },

url = {https://www.nature.com/articles/s41467-023-37212-6.pdf},

doi = {10.1038/s41467-023-37212-6},

year  = {2023},

date = {2023-03-29},

urldate = {2023-03-29},

journal = {Nature Communications},

volume = {14},

number = {1754},

abstract = {In exsolution, nanoparticles form by emerging from oxide hosts by application of redox driving forces, leading to transformative advances in stability, activity, and efficiency over deposition techniques, and resulting in a wide range of new opportunities for catalytic, energy and net-zero-related technologies. However, the mechanism of exsolved nanoparticle nucleation and perovskite structural evolution, has, to date, remained unclear. Herein, we shed light on this elusive process by following in real time Ir nanoparticle emergence from a SrTiO3 host oxide lattice, using in situ high-resolution electron microscopy in combination with computational simulations and machine learning analytics. We show that nucleation occurs via atom clustering, in tandem with host evolution, revealing the participation of surface defects and host lattice restructuring in trapping Ir atoms to initiate nanoparticle formation and growth. These insights provide a theoretical platform and practical recommendations to further the development of highly functional and broadly applicable exsolvable materials.},

note = {The separation of nanoparticles from oxide hosts by exsolution forms the basis for catalytic and energy-related applications. Here, the authors elucidate the multistep mechanism of exsolution at perovskite surfaces by combining real-time electron microscopy and computational methods.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}