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Nano Research 2021, 14(1): 239-244 https://doi.org/10.1007/s12274-020-3075-3
Research Article | Issue | Published: 05 January 2021

Breakdown of Raman selection rules by Fröhlich interaction in few-layer WS2

Show Author's Information Qing-Hai Tan1,  Yu-Jia Sun1,  Xue-Lu Liu1,  Kai-Xuan Xu1,  Yuan-Fei Gao1,2,  Shu-Liang Ren1,  Ping-Heng Tan1,2,  Jun Zhang1,2( )
State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Center of Materials Science and Optoelectronics Engineering, CAS Center of Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing 100083, China
Beijing Academy of Quantum Information Science, Beijing 100193, China
Keywords:
WS2, resonant Raman scattering, dark exciton, Raman section rules, Fröhlich interaction
Topics:
Electron energy levels ElectronsRaman scatteringRaman spectroscopyTungsten compounds
Cite this article:
Tan Q-H, Sun Y-J, Liu X-L, et al. Breakdown of Raman selection rules by Fröhlich interaction in few-layer WS2. Nano Research, 2021, 14(1): 239-244. https://doi.org/10.1007/s12274-020-3075-3
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Abstract Full text Electronic supplementary material About this article

The polarization selection rule of Raman scattering is crucial in symmetry analysis of elementary excitations in semiconductors and correlated electron systems. Here we reported the observation of breakdown of Raman selection rules in few-layer WS2 by using resonant Raman spectroscopy. When the excitation energy is close to the dark A exciton state, we observed some infrared active modes and backscattering forbidden modes. Importantly, we found that all observed phonon modes follow the same paralleled-polarization behavior. According to the electron-phonon coupling near the band edge in WS2, we proposed a theoretical model based on the intraband Fröhlich interaction. In this case, the polarization response of the scattering signal is no longer determined by the original Raman tensor of scattered phonons. Instead, it is determined by a new isotropic Raman tensor that generated from this intraband Fröhlich interaction between dark A exciton and phonons. We found that this theoretical model is in excellent agreement with the observed results. The breakdown of Raman selection rules can violate the conventional limitations of the optical response and provide an effective method to control the polarization of Raman scattering signals in two-dimensional materials.


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About this article

Breakdown of Raman selection rules by Fröhlich interaction in few-layer WS2

Show Author's information Qing-Hai Tan1, Yu-Jia Sun1, Xue-Lu Liu1, Kai-Xuan Xu1, Yuan-Fei Gao1,2, Shu-Liang Ren1, Ping-Heng Tan1,2, Jun Zhang1,2( )
State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Center of Materials Science and Optoelectronics Engineering, CAS Center of Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing 100083, China
Beijing Academy of Quantum Information Science, Beijing 100193, China

Abstract

The polarization selection rule of Raman scattering is crucial in symmetry analysis of elementary excitations in semiconductors and correlated electron systems. Here we reported the observation of breakdown of Raman selection rules in few-layer WS2 by using resonant Raman spectroscopy. When the excitation energy is close to the dark A exciton state, we observed some infrared active modes and backscattering forbidden modes. Importantly, we found that all observed phonon modes follow the same paralleled-polarization behavior. According to the electron-phonon coupling near the band edge in WS2, we proposed a theoretical model based on the intraband Fröhlich interaction. In this case, the polarization response of the scattering signal is no longer determined by the original Raman tensor of scattered phonons. Instead, it is determined by a new isotropic Raman tensor that generated from this intraband Fröhlich interaction between dark A exciton and phonons. We found that this theoretical model is in excellent agreement with the observed results. The breakdown of Raman selection rules can violate the conventional limitations of the optical response and provide an effective method to control the polarization of Raman scattering signals in two-dimensional materials.

Keywords: WS2, resonant Raman scattering, dark exciton, Raman section rules, Fröhlich interaction

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Publication history
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Acknowledgements

Publication history

Received: 06 July 2020
Revised: 16 August 2020
Accepted: 20 August 2020
Published: 05 January 2021
Issue date: January 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature

Acknowledgements

J. Z. and P. T. acknowledge support from the National Basic Research Program of China (nos. 2017YFA0303401 and 2016YFA0301200), Beijing Natural Science Foundation (No. JQ18014), and the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB28000000).

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