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Near-Neighbor Electron Orbital Coupling Effect of Single-Atomic-Layer Au Cluster Intercalated Bilayer 2H-TaS2 for Surface Enhanced Raman Scattering Sensing

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    Physical Insights into Materials and Molecular Properties

    Near-Neighbor Electron Orbital Coupling Effect of Single-Atomic-Layer Au Cluster Intercalated Bilayer 2H-TaS2 for Surface Enhanced Raman Scattering Sensing
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    • Shirui Weng
      Shirui Weng
      Institute of Health and Medical Technology, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China
      More by Shirui Weng
    • Wenjun Chu
      Wenjun Chu
      Key Laboratory of Precision and Intelligent Chemistry, University of Science & Technology of China, Hefei 230026, Anhui, China
      More by Wenjun Chu
      Orcidhttps://orcid.org/0000-0002-2701-3325
    • Huaze Zhu
      Huaze Zhu
      Department of Materials Science and Engineering, Westlake University, Hangzhou 310024, Zhejiang, China
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    • Junxiang Li
      Junxiang Li
      Institute of Health and Medical Technology, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China
      More by Junxiang Li
    • Ronglu Dong
      Ronglu Dong
      Institute of Health and Medical Technology, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China
      More by Ronglu Dong
    • Rui Niu
      Rui Niu
      High Magnetic Field Laboratory of Anhui Province, Chinese Academy of Sciences, Hefei 230031, China
      More by Rui Niu
    • Jun Yang
      Jun Yang
      Department of Materials Science and Engineering, Westlake University, Hangzhou 310024, Zhejiang, China
      More by Jun Yang
    • Changjin Zhang
      Changjin Zhang
      High Magnetic Field Laboratory of Anhui Province, Chinese Academy of Sciences, Hefei 230031, China
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    • Zhenyu Li
      Zhenyu Li
      Key Laboratory of Precision and Intelligent Chemistry, University of Science & Technology of China, Hefei 230026, Anhui, China
      More by Zhenyu Li
      Orcidhttps://orcid.org/0000-0003-2112-9834
    • Liangbao Yang*
      Liangbao Yang
      Institute of Health and Medical Technology, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China
      Department of Pharmacy, Hefei Cancer Hospital, Chinese Academy of Sciences, Hefei 230031, Anhui, China
      *Email: [email protected]
      More by Liangbao Yang
      Orcidhttps://orcid.org/0000-0002-6559-6947
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2023, 14, 38, 8477–8484
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    https://doi.org/10.1021/acs.jpclett.3c02225
    Published September 18, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    It is difficult to perfectly analyze the enhancement mechanism of two-dimensional (2D) materials and their combination with precious metals as surface enhanced Raman scattering (SERS) substrates using chemical enhancement mechanisms. Here, we propose a new mentality based on the coupling effect of neighboring electron orbitals to elucidate the electromagnetic field enhancement mechanism of single-atom-layer Au clusters embedded in double-layer 2H-TaS2 for SRES sensing. The insertion of Au atoms into the 2H-TaS2 interlayer was verified by XRD, AFM, and HRTEM, and a SERS signal enhancement of 2 orders of magnitude was obtained compared to the pure 2H-TaS2. XPS and micro-UV/vis–NIR spectra indicate that the outer electrons of neighboring Au and 2H-TaS2 overlap and migrate from Au to 2H-TaS2. First-principles calculations suggest strong electronic coupling between Au and 2H-TaS2. This study offers insights into SERS enhancement in nonprecious metal compounds and guides the development of new SERS substrates.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.3c02225.

    • Additional experimental details, typical optical image of single crystal 2H-TaS2, specific process of Au intercalation 2H-TaS2, EDS mapping data of the Au-2H-TaS2 on the Si substrate by SEM, corresponding selected area electron diffraction (SAED) pattern and the microlattice diffraction fringes of Au-2H-TaS2, Raman spectra of 2H-TaS2 and Au-2H-TaS2 stored for 1 day and 90 days, SERS mapping at 1617 cm–1 of CV of 10–7 M, XPS survey spectra of 2H-TaS2 and Au-2H-TaS2 nanosheets, UV/vis–NIR diffuse reflectance spectra of the 2H-TaS2 and Au-2H-TaS2 with or without CV, calculated single-atomic-layer (SAL) Au clusters on the TaS2 interlayer with different Au atoms, calculated density of states of different Au atoms, intercalated in the 2H-TaS2 surface (including Figures S1–S10) (PDF)

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    This article is cited by 3 publications.

    1. Junxiang Li, Qiqi Li, Haochuan Feng, Keke Jiao, Changjin Zhang, Shirui Weng, Liangbao Yang. Tuning d-Orbital Electronic Structure via Au-Intercalated Two-Dimensional Fe3GeTe2 to Increase Surface Plasmon Activity. The Journal of Physical Chemistry Letters 2024, 15 (7) , 1818-1827. https://doi.org/10.1021/acs.jpclett.3c02742
    2. Yaning Fu, Nan Wang, Mengyao Huang, Zhongjun Li, Youcai Lu, Qingchao Liu. Precisely Engineering of Ångström‐Scale Dual Single Atom Drive [Co‐O] Spin‐Orbit Coupling to Boost Lithium–Oxygen Batteries Electrocatalysis. Advanced Functional Materials 2024, 134 https://doi.org/10.1002/adfm.202418098
    3. Jiawei Shen, Jiaxin Zhang, Zirui Fu, Yan Pan, Xiaowan Li, Shuyi Wu, Yun Shan, Lizhe Liu. Dynamic repulsive interaction enables an asymmetric electron–phonon coupling for improving Raman scattering. Physical Chemistry Chemical Physics 2024, 26 (9) , 7343-7350. https://doi.org/10.1039/D3CP05835B
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2023, 14, 38, 8477–8484
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.3c02225
    Published September 18, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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