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Direct characterization of shear phonons in layered materials by mechano-Raman spectroscopy

Nature Photonics volume 17, pages 531–537 (2023)Cite this article

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Abstract

Shear phonons are collective atomic-layer motions in layered materials that carry critical information about mechanical, thermal and optoelectronic properties. Phonon branches with co-directional atomic-layer motions carry unique information about the global structure and hidden interfaces in layered crystals and heterostructures, but they are not detectable due to the very limited electron–phonon coupling. Here we utilize the propagating feature and mechanical coupling between shear phonons and localized plasmonic cavities to successfully realize direct characterization of ground-state shear phonons down to 4 cm−1 in energy by introducing mechano-Raman spectroscopy (MRS). MRS has the ability to characterize the global crystal structure with more than 108-fold enhancement and to accurately measure subpicometre displacements under ambient conditions with a thermal-noise-free feature. The propagating behaviour and the capacity of MRS to detect optically hidden interfaces are demonstrated. The broad tunability of plasmons makes the MRS technique a robust tool for extensive applications, including global crystal flaw detection, mechanical sensing and the mechanical modulation of light.

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Fig. 1: MRS for direct frequency-domain detection of mechanical vibrations.
Fig. 2: MRS for dark phonon observation and quantitative mechanical investigations.
Fig. 3: Thermal-noise-free feature of MRS.
Fig. 4: Propagating behaviour in multi-component vibrators and the capacity for hidden-interface detection.

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Data availability

The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request. Source data are provided with this paper.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (22173044, 21873048 and 22073017), the Natural Science Foundation of Jiangsu Province (BK20220121), the National Key R&D Program of China (2020YFA0406104), the Fundamental Research Funds for the Central Universities in China (021014380177), the Frontiers Science Center for Critical Earth Material Cycling of Nanjing University (DLTD2110), ‘Innovation & Entrepreneurship Talents Plan’ of Jiangsu Province and the Innovation Program for Quantum Science and Technology (2021ZD0303301, 2021ZD0303303 and 2021ZD0303305). Z.J. acknowledges funding support from the CAS Interdisciplinary Innovation Team and the National Natural Science Foundation of China (12074371).

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Author notes

  1. These authors contributed equally: Susu Fang, Sai Duan.

Authors and Affiliations

  1. Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China

    Susu Fang, Li Li, Hua Li, Baichuan Jiang, Chuanhui Liu, Lei Zhang, Daiqian Xie & Weigao Xu

  2. Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, MOE Key Laboratory of Computational Physical Sciences, Department of Chemistry, Fudan University, Shanghai, China

    Sai Duan

  3. Department of Physics, Xiamen University, Xiamen, China

    Xingzhi Wang

  4. School of Optical and Electronic Information, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, China

    Sijie Chen & Xinglin Wen

  5. National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, China

    Nanyang Wang & Yagang Yao

  6. State Key Laboratory for Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing, China

    Jun Zhang

  7. Hefei National Laboratory, Hefei, China

    Daiqian Xie & Yi Luo

  8. Hefei National Research Center for Physical Science at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, China

    Yi Luo

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Contributions

W.X. and S.F. conceived the initial idea. W.X., Y.L., S.D. and S.F. designed the experiments. S.F. fabricated the samples and performed the spectroscopy measurement experiments with help from L.L., H.L., B.J., C.L., N.W. and L.Z., and Y.Y., S.C. and X. Wen performed finite-difference time-domain simulations. S.D., J.Z., X. Wang, D.X., Y.L. and W.X. contributed to theoretical analyses. S.F. collected and organized all experimental data. S.F., S.D., X. Wang, H.L., Y.L. and W.X. co-wrote the manuscript, with input from all authors.

Corresponding authors

Correspondence to Daiqian Xie, Yi Luo or Weigao Xu.

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Supplementary information

Supplementary Information

Supplementary text, Figs. 1–12, Tables 1 and 2, references and caption for Video 1.

Supplementary Video 1

Schematic view of a 1,000,000,000,000 times slow motion of MRS processes driven by ν1 and ν12 shear phonon vibrators in 13LG.

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Fang, S., Duan, S., Wang, X. et al. Direct characterization of shear phonons in layered materials by mechano-Raman spectroscopy. Nat. Photon. 17, 531–537 (2023). https://doi.org/10.1038/s41566-023-01181-5

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