List of Edited Articles
Recently published articles handled as primary editor:
Recently published articles handled as primary editor:
Hajir Hilal, Qiang Zhao, Jeongwon Kim, Sungwoo Lee, MohammadNavid Haddadnezhad, Sungjae Yoo, Soohyun Lee, Woongkyu Park, Woocheol Park, Jaewon Lee, Joong Wook Lee, Insub Jung, Sungho Park
Three-dimensional nanoframes with dual rims as nanoprobes for biosensing (Journal Article)
In: Nature Communications, vol. 13, no. 4813, 2022, ( Most SERS-active nanostructures suffer from low robustness against misalignment to field polarization. Here, the authors demonstrate three-dimensional nanoframes of octahedral geometry, with two rims engraved on each facet, as polarization-independent SERS nanoprobes.).
Three-dimensional (3D) nanoframe structures are very appealing because their inner voids and ridges interact efficiently with light and analytes, allowing for effective optical-based sensing. However, the realization of complex nanoframe architecture with high yield is challenging because the systematic design of such a complicated nanostructure lacks an appropriate synthesis protocol. Here, we show the synthesis method for complex 3D nanoframes wherein two-dimensional (2D) dual-rim nanostructures are engraved on each facet of octahedral nanoframes. The synthetic scheme proceeds through multiple executable on-demand steps. With Au octahedral nanoparticles as a sacrificial template, sequential processes of edge-selective Pt deposition and inner Au etching lead to Pt octahedral mono-rim nanoframes. Then, adlayers of Au are grown on Pt skeletons via the Frank-van der Merwe mode, forming sharp and well-developed edges. Next, Pt selective deposition on both the inner and outer boundaries leads to tunable geometric patterning on Au. Finally, after the selective etching of Au, Pt octahedral dual-rim nanoframes with highly homogeneous size and shape are achieved. In order to endow plasmonic features, Au is coated around Pt frames while retaining their geometric shape. The resultant plasmonic dual-rim engraved nanoframes possess strong light entrapping capability verified by single-particle surface-enhanced Raman scattering (SERS) and show the potential of nanoprobes for biosensing through SERS-based immunoassay.
Lei Zhang, Chen Yang, Chenxi Lu, Xingxing Li, Yilin Guo, Jianning Zhang, Jinglong Lin, Zhizhou Li, Chuancheng Jia, Jinlong Yang, K. N. Houk, Fanyang Mo, Xuefeng Guo
Precise electrical gating of the single-molecule Mizoroki-Heck reaction (Journal Article)
In: Nature Communications, vol. 13, no. 4552 , 2022, (Guiding chemical reactions in a predictable and controllable manner is an ultimate goal of chemistry. Here, the authors show tuning of the single-molecule Mizoroki-Heck catalytic cycle through electrical gating and direct in-situ detection.).
Precise tuning of chemical reactions with predictable and controllable manners, an ultimate goal chemists desire to achieve, is valuable in the scientific community. This tunability is necessary to understand and regulate chemical transformations at both macroscopic and single-molecule levels to meet demands in potential application scenarios. Herein, we realise accurate tuning of a single-molecule Mizoroki-Heck reaction via applying gate voltages as well as complete deciphering of its detailed intrinsic mechanism by employing an in-situ electrical single-molecule detection, which possesses the capability of single-event tracking. The Mizoroki-Heck reaction can be regulated in different dimensions with a constant catalyst molecule, including the molecular orbital gating of Pd(0) catalyst, the on/off switching of the Mizoroki-Heck reaction, the promotion of its turnover frequency, and the regulation of each elementary reaction within the Mizoroki-Heck catalytic cycle. These results extend the tuning scope of chemical reactions from the macroscopic view to the single-molecule approach, inspiring new insights into designing different strategies or devices to unveil reaction mechanisms and discover novel phenomena.
Sungjae Yoo, Jaewon Lee, Hajir Hilal, Insub Jung, Woongkyu Park, Joong Wook Lee, Soobong Choi, Sungho Park
Nesting of multiple polyhedral plasmonic nanoframes into a single entity (Journal Article)
In: Nature Communications, vol. 13, no. 4544 , 2022, (The spatial configuration of nanostructure building blocks determines the physical and optical properties of their superstructures. Here, the authors report on complex nanoparticles in which different geometric forms of nanoframes are nested into a single entity by multistep chemical reactions.).
The development of plasmonic nanostructures with intricate nanoframe morphologies has attracted considerable interest for improving catalytic and optical properties. However, arranging multiple nanoframes in one nanostructure especially, in a solution phase remains a great challenge. Herein, we show complex nanoparticles by embedding various shapes of three-dimensional polyhedral nanoframes within a single entity through rationally designed synthetic pathways. This synthetic strategy is based on the selective deposition of platinum atoms on high surface energy facets and subsequent growth into solid platonic nanoparticles, followed by the etching of inner Au domains, leaving complex nanoframes. Our synthetic routes are rationally designed and executable on-demand with a high structural controllability. Diverse Au solid nanostructures (octahedra, truncated octahedra, cuboctahedra, and cubes) evolved into complex multi-layered nanoframes with different numbers/shapes/sizes of internal nanoframes. After coating the surface of the nanoframes with plasmonically active metal (like Ag), the materials exhibited highly enhanced electromagnetic near-field focusing embedded within the internal complicated rim architecture.
Mingu Kang, Hyun Woo Kim, Elham Oleiki, Yeonjeong Koo, Hyeongwoo Lee, Huitae Joo, Jinseong Choi, Taeyong Eom, Geunsik Lee, Yung Doug Suh, Kyoung-Duck Park
Conformational heterogeneity of molecules physisorbed on a gold surface at room temperature (Journal Article)
In: Nature Communications, vol. 13, no. 4133, 2022, (Tip-enhanced vibrational spectroscopy at room temperature is complicated by molecular conformational dynamics, photobleaching, contaminations, and chemical reactions in air. This study demonstrates that a sub-nm protective layer of Al2O3 provides robust conditions for probing single-molecule conformations.).
A quantitative single-molecule tip-enhanced Raman spectroscopy (TERS) study at room temperature remained a challenge due to the rapid structural dynamics of molecules exposed to air. Here, we demonstrate the hyperspectral TERS imaging of single or a few brilliant cresyl blue (BCB) molecules at room temperature, along with quantitative spectral analyses. Robust chemical imaging is enabled by the freeze-frame approach using a thin Al2O3 capping layer, which suppresses spectral diffusions and inhibits chemical reactions and contamination in air. For the molecules resolved spatially in the TERS image, a clear Raman peak variation up to 7.5 cm−1 is observed, which cannot be found in molecular ensembles. From density functional theory-based quantitative analyses of the varied TERS peaks, we reveal the conformational heterogeneity at the single-molecule level. This work provides a facile way to investigate the single-molecule properties in interacting media, expanding the scope of single-molecule vibrational spectroscopy studies.
Nam Heon Cho, Young Bi Kim, Yoon Young Lee, Sang Won Im, Ryeong Myeong Kim, Jeong Won Kim, Seok Daniel Namgung, Hye-Eun Lee, Hyeohn Kim, Jeong Hyun Han, Hye Won Chung, Yoon Ho Lee, Jeong Woo Han, Ki Tae Nam
Adenine oligomer directed synthesis of chiral gold nanoparticles (Journal Article)
In: Nature Communications, vol. 13, no. 3831, 2022, (Chiral plasmonic nanoparticles are of great interest in nanotechnology. Here, the authors demonstrate chiral shape guidance by single-stranded oligonucleotides during particle growth based on sequence-specific hydrogen bonding within the strand.).
Precise control of morphology and optical response of 3-dimensional chiral nanoparticles remain as a significant challenge. This work demonstrates chiral gold nanoparticle synthesis using single-stranded oligonucleotide as a chiral shape modifier. The homo-oligonucleotide composed of Adenine nucleobase specifically show a distinct chirality development with a dissymmetric factor up to g ~ 0.04 at visible wavelength, whereas other nucleobases show no development of chirality. The synthesized nanoparticle shows a counter-clockwise rotation of generated chiral arms with approximately 200 nm edge length. The molecular dynamics and density functional theory simulations reveal that Adenine shows the highest enantioselective interaction with Au(321)R/S facet in terms of binding orientation and affinity. This is attributed to the formation of sequence-specific intra-strand hydrogen bonding between nucleobases. We also found that different sequence programming of Adenine-and Cytosine-based oligomers result in chiral gold nanoparticles’ morphological and optical change. These results extend our understanding of the biomolecule-directed synthesis of chiral gold nanoparticles to sequence programmable deoxyribonucleic acid and provides a foundation for programmable synthesis of chiral gold nanoparticles.
Li-Zhe Feng, Jing-Jing Wang, Tao Ma, Yi-Chen Yin, Kuang-Hui Song, Zi-Du Li, Man-Man Zhou, Shan Jin, Taotao Zhuang, Fengjia Fan, Manzhou Zhu, Hong-Bin Yao
Biomimetic non-classical crystallization drives hierarchical structuring of efficient circularly polarized phosphors (Journal Article)
In: Nature Communications, vol. 13, no. 3339, 2022, (Chiral emitters with high photoluminescence quantum yield are desirable for use in circularly polarized LEDs. The authors demonstrate the transfer of chirality from nanoscale copper iodide clusters to microscale chiral luminescent polycrystals by non-classical crystallization.).
Hierarchically structured chiral luminescent materials hold promise for achieving efficient circularly polarized luminescence. However, a feasible chemical route to fabricate hierarchically structured chiral luminescent polycrystals is still elusive because of their complex structures and complicated formation process. We here report a biomimetic non-classical crystallization (BNCC) strategy for preparing efficient hierarchically structured chiral luminescent polycrystals using well-designed highly luminescent homochiral copper(I)-iodide hybrid clusters as basic units for non-classical crystallization. By monitoring the crystallization process, we unravel the BNCC mechanism, which involves crystal nucleation, nanoparticles aggregation, oriented attachment, and mesoscopic transformation processes. We finally obtain the circularly polarized phosphors with both high luminescent efficiency of 32% and high luminescent dissymmetry factor of 1.5 × 10^−2, achieving the demonstration of a circularly polarized phosphor converted light emitting diode with a polarization degree of 1.84% at room temperature. Our designed BNCC strategy provides a simple, reliable, and large-scale synthetic route for preparing bright circularly polarized phosphors.