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. 2025 Jul 16:e2506241.
doi: 10.1002/adma.202506241. Online ahead of print.

Quantitatively Predicting Angle-Resolved Polarized Raman Intensity of Anisotropic Layered Materials

Jia-Liang Xie  1   2 , Tao Liu  1   2 , Yu-Chen Leng  1 , Rui Mei  1   2 , Heng Wu  1   2 , Chen-Kai Liu  1   2 , Jia-Hong Wang  2   3 , Yang Li  3 , Xue-Feng Yu  2   3 , Miao-Ling Lin  1   2 , Ping-Heng Tan  1   2
Affiliations

Quantitatively Predicting Angle-Resolved Polarized Raman Intensity of Anisotropic Layered Materials

Jia-Liang Xie et al. Adv Mater. .

Abstract

Angle-resolved polarized Raman (ARPR) spectroscopy provides insights into optical anisotropy and symmetry-related electron-photon/electron-phonon couplings of anisotropic layered materials (ALMs). However, since their discovery over ten years ago, ARPR responses in ALM flakes has exhibited a puzzling dependence on flake thickness, excitation wavelength, and dielectric environment, complicating their understanding and prediction. By taking black phosphorus (BP) (⩾20 nm) flakes and four-layer Td-WTe2 as examples, this study introduces intrinsic Raman tensors (Rint) and proposes strategies to predict the ARPR intensity profiles of thick and atomically-thin ALM flakes by considering birefringence, linear dichroism and multilayer interference inside multilayered structures with experimentally determined complex refractive indexes along in-plane axes and complex tensor elements of Rint for the corresponding phonon modes. The tensor elements of effective Raman tensors (Reff), which are directly linked to the polarization vectors of incident and scattered light outside the ALM surface, are derived to quantitatively predict ARPR intensity for these ALM flakes, showing intricate dependence on ALM thickness, dielectric substrates, and excitation wavelengths. This framework can be extended to other ALM flakes from atomically-thin layers to bulk limit, facilitating comprehensive prediction of their ARPR intensity regardless of layer-dependent electronic properties.

Keywords: angle‐resolved polarized Raman intensity; anisotropic layered material; complex Raman tensor; complex refractive index; optical anisotropy.

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References

    1. W. Ma, P. Alonso‐Gonzalez, S. Li, A. Y. Nikitin, J. Yuan, J. Martin‐Sanchez, J. Taboada‐Gutierrez, I. Amenabar, P. Li, S. Velez, C. Tollan, Z. Dai, Y. Zhang, S. Sriram, K. Kalantar‐Zadeh, S.‐T. Lee, R. Hillenbrand, Q. Bao, Nature 2018, 562, 557.
    1. S. Biswas, M. Y. Grajower, K. Watanabe, T. Taniguchi, H. A. Atwater, Science 2021, 374, 448.
    1. S. E. Kim, F. Mujid, A. Rai, F. Eriksson, J. Suh, P. Poddar, A. Ray, C. Park, E. Fransson, Y. Zhong, D. A. Muller, P. Erhart, D. G. Cahill, J. Park, Nautre 2021, 597, 660.
    1. Z. Li, M. Tang, J. Huang, F. Qin, L. Ao, Z. Shen, C. Zhang, P. Chen, X. Bi, C. Qiu, Z. Yu, K. Zhai, T. Ideue, L. Wang, Z. Liu, Y. Tian, Y. Iwasa, H. Yuan, Adv. Mater. 2022, 34, 2201209.
    1. Y. Luo, N. Mao, D. Ding, M.‐H. Chiu, X. Ji, K. Watanabe, T. Taniguchi, V. Tung, H. Park, P. Kim, J. Kong, W. L. Wilson, Nat. Nanotechnol. 2023, 18, 350.