Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement

From spanning bulks to nanoclusters, surface-enhanced Raman scattering (SERS) substrates of noble metals have frequently been explored for a long time. However, further downsizing nanoclusters to the atomic level, the surface plasmon resonance effect disappears, making the research on the SERS effec...

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Main Authors: Yu, Jian, Chen, Chao, Zhang, Qinghua, Lin, Jie, Yang, Xiuyi, Gu, Lin, Zhang, Hui, Liu, Zhi, Wang, Yu, Zhang, Shuo, Wang, Xiaotian, Guo, Lin
Other Authors: School of Materials Science and Engineering
Format: Article
Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/164486
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1644862023-01-30T02:11:12Z Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement Yu, Jian Chen, Chao Zhang, Qinghua Lin, Jie Yang, Xiuyi Gu, Lin Zhang, Hui Liu, Zhi Wang, Yu Zhang, Shuo Wang, Xiaotian Guo, Lin School of Materials Science and Engineering Engineering::Materials Spectroscopy Charge-Transfer From spanning bulks to nanoclusters, surface-enhanced Raman scattering (SERS) substrates of noble metals have frequently been explored for a long time. However, further downsizing nanoclusters to the atomic level, the surface plasmon resonance effect disappears, making the research on the SERS effect of atom-scale noble metal still lacking. Here, we discover a single-atom enhanced Raman scattering (SAERS) effect based on Au single atoms anchored on amorphous C3N4 nanosheets (Au1/ACNs). The Au1/ACN exhibits an excellent spectral stability and reproducibility, as the uniform dispersed Au single atoms avoid the agglomeration of Au atoms to generate nonuniformly dispersed "hotspots" that suffer from poor SERS stability and reproducibility. Even only ∼2.5% Au-coated area in the laser illuminated area can yield an enhancement factor of 2.5 × 104. The SAERS effect is attributed to the synergistic effect of Au single atoms anchored on amorphous C3N4, which increases the dipole moment and polarizability of molecules, enhancing the Raman signal of probe molecules. Furthermore, we propose a novel single-atom charge transfer mechanism that single-atom Au dominates higher electron delocalizability and higher electronic density of states near the HOMO level than the Au cluster. Our results will erect a new milepost for the application of single-atom materials in the field of enhanced Raman spectroscopy. This work was financially supported by the National Natural Science Foundation of China (52022006, 12274018, 21875008, 52002380, and 51532001), China Postdoctoral Science Foundation (2022M710300), and Ningbo 3315 Innovative Teams Program (Grant No. 2019A-14-C). 2023-01-30T02:11:12Z 2023-01-30T02:11:12Z 2022 Journal Article Yu, J., Chen, C., Zhang, Q., Lin, J., Yang, X., Gu, L., Zhang, H., Liu, Z., Wang, Y., Zhang, S., Wang, X. & Guo, L. (2022). Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement. Journal of the American Chemical Society, 144(48), 21908-21915. https://dx.doi.org/10.1021/jacs.2c07413 0002-7863 https://hdl.handle.net/10356/164486 10.1021/jacs.2c07413 36419236 2-s2.0-85143050890 48 144 21908 21915 en Journal of the American Chemical Society © 2022 American Chemical Society. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Materials
Spectroscopy
Charge-Transfer
spellingShingle Engineering::Materials
Spectroscopy
Charge-Transfer
Yu, Jian
Chen, Chao
Zhang, Qinghua
Lin, Jie
Yang, Xiuyi
Gu, Lin
Zhang, Hui
Liu, Zhi
Wang, Yu
Zhang, Shuo
Wang, Xiaotian
Guo, Lin
Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement
description From spanning bulks to nanoclusters, surface-enhanced Raman scattering (SERS) substrates of noble metals have frequently been explored for a long time. However, further downsizing nanoclusters to the atomic level, the surface plasmon resonance effect disappears, making the research on the SERS effect of atom-scale noble metal still lacking. Here, we discover a single-atom enhanced Raman scattering (SAERS) effect based on Au single atoms anchored on amorphous C3N4 nanosheets (Au1/ACNs). The Au1/ACN exhibits an excellent spectral stability and reproducibility, as the uniform dispersed Au single atoms avoid the agglomeration of Au atoms to generate nonuniformly dispersed "hotspots" that suffer from poor SERS stability and reproducibility. Even only ∼2.5% Au-coated area in the laser illuminated area can yield an enhancement factor of 2.5 × 104. The SAERS effect is attributed to the synergistic effect of Au single atoms anchored on amorphous C3N4, which increases the dipole moment and polarizability of molecules, enhancing the Raman signal of probe molecules. Furthermore, we propose a novel single-atom charge transfer mechanism that single-atom Au dominates higher electron delocalizability and higher electronic density of states near the HOMO level than the Au cluster. Our results will erect a new milepost for the application of single-atom materials in the field of enhanced Raman spectroscopy.
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Yu, Jian
Chen, Chao
Zhang, Qinghua
Lin, Jie
Yang, Xiuyi
Gu, Lin
Zhang, Hui
Liu, Zhi
Wang, Yu
Zhang, Shuo
Wang, Xiaotian
Guo, Lin
format Article
author Yu, Jian
Chen, Chao
Zhang, Qinghua
Lin, Jie
Yang, Xiuyi
Gu, Lin
Zhang, Hui
Liu, Zhi
Wang, Yu
Zhang, Shuo
Wang, Xiaotian
Guo, Lin
author_sort Yu, Jian
title Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement
title_short Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement
title_full Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement
title_fullStr Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement
title_full_unstemmed Au atoms anchored on amorphous C₃N₄ for single-site Raman enhancement
title_sort au atoms anchored on amorphous c₃n₄ for single-site raman enhancement
publishDate 2023
url https://hdl.handle.net/10356/164486
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