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Colossal structural distortion and interlayer-coupling suppression in a van der Waals crystal induced by atomic vacancies

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Abstract

The interlayer coupling in van der Waals (vdW) crystals has substantial effects on the performance of materials. However, an in-depth understanding of the microscopic mechanism on the defect-modulated interlayer coupling is often elusive, owing partly to the challenge of atomic-scale characterization. Here we report the native Se-vacancies in a charge-density-wave metal 2H-NbSe2, as well as their influence on the local atomic configurations and interlayer coupling. Our low-temperature scanning tunneling microscopy (STM) measurements, complemented by density functional theory calculations, indicate that the Se-vacancies in few-layer NbSe2 can generate obvious atomic distortions due to the Jahn-Teller effect, thus breaking the rotational symmetry on the nanoscale. Moreover, these vacancies can locally generate an in-gap state in single-layer NbSe2, and more importantly, lead to a colossal suppression of interlayer coupling in the bilayer system. Our results provide clear structural and electronic fingerprints around the vacancies in vdW crystals, paving the way for developing functional vdW devices.

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Acknowledgements

This work is financial supported by National Natural Science Foundation of China (Nos. 92163206, 61725107, 12274026, 61971035, 62271048, 11934003, 21961132023, and U1930402), National Key Research and Development Program Program of China (Nos. 2020YFA0308800, 2021YFA1400100, 2022YFA1402502, and 2022YFA1402602), Beijing Natural Science Foundation (No. Z190006), China Postdoctoral Science Foundation (No. 2021M700407), Villum Fonden (No. 00013340), and the Danish Research Foundation (No. DNRF103) for the Center for Nanostructured Graphene (CNG). Computer infrastructure resources are provided by the Niflheim supercomputer.

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Author notes

  1. Liangguang Jia, Fei Gao, and Yu Zhang contributed equally to this work.

Authors and Affiliations

  1. School of Integrated Circuits and Electronics, MIIT Key Laboratory for Low-Dimensional Quantum Structure and Devices, Beijing Institute of Technology, Beijing, 100081, China

    Liangguang Jia, Yu Zhang, Yaoyao Chen, Baofei Hou, Zeping Huang, Quanzhen Zhang, Xu Wu, Liwei Liu & Yeliang Wang

  2. Center for Nanostructured Graphene, Department of Physics, Technical University of Denmark, Kongens Lyngby, DK-2800, Denmark

    Fei Gao & Mads Brandbyge

  3. Advanced Research Institute of Multidisciplinary Sciences, Beijing Institute of Technology, Beijing, 100081, China

    Yu Zhang

  4. Beijing Computational Science Research Center, Beijing, 100193, China

    Shiwu Gao

  5. Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China

    Hong-Jun Gao

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  1. Liangguang Jia
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Correspondence to Yu Zhang or Yeliang Wang.

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12274_2022_5203_MOESM1_ESM.pdf

Colossal structural distortion and interlayer-coupling suppression in a van der Waals crystal induced by atomic vacancies

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Jia, L., Gao, F., Zhang, Y. et al. Colossal structural distortion and interlayer-coupling suppression in a van der Waals crystal induced by atomic vacancies. Nano Res. 16, 5715–5720 (2023). https://doi.org/10.1007/s12274-022-5203-8

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  • DOI: https://doi.org/10.1007/s12274-022-5203-8

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