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Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet CrI3

Author

Listed:
  • Wencan Jin

    (University of Michigan
    Auburn University)

  • Hyun Ho Kim

    (University of Waterloo, Waterloo, 200 University Ave W
    School of Materials Science and Engineering, Kumoh National Institute of Technology)

  • Zhipeng Ye

    (910 Boston Avenue, Texas Tech University)

  • Gaihua Ye

    (910 Boston Avenue, Texas Tech University)

  • Laura Rojas

    (910 Boston Avenue, Texas Tech University)

  • Xiangpeng Luo

    (University of Michigan)

  • Bowen Yang

    (University of Waterloo, Waterloo, 200 University Ave W)

  • Fangzhou Yin

    (University of Waterloo, Waterloo, 200 University Ave W)

  • Jason Shih An Horng

    (University of Michigan)

  • Shangjie Tian

    (Renmin University of China)

  • Yang Fu

    (Renmin University of China)

  • Gongjun Xu

    (University of Michigan, 1085 South University)

  • Hui Deng

    (University of Michigan)

  • Hechang Lei

    (Renmin University of China)

  • Adam W. Tsen

    (University of Waterloo, Waterloo, 200 University Ave W)

  • Kai Sun

    (University of Michigan)

  • Rui He

    (910 Boston Avenue, Texas Tech University)

  • Liuyan Zhao

    (University of Michigan)

Abstract

Exciton dynamics can be strongly affected by lattice vibrations through electron-phonon coupling. This is rarely explored in two-dimensional magnetic semiconductors. Focusing on bilayer CrI3, we first show the presence of strong electron-phonon coupling through temperature-dependent photoluminescence and absorption spectroscopy. We then report the observation of periodic broad modes up to the 8th order in Raman spectra, attributed to the polaronic character of excitons. We establish that this polaronic character is dominated by the coupling between the charge-transfer exciton at 1.96 eV and a longitudinal optical phonon at 120.6 cm−1. We further show that the emergence of long-range magnetic order enhances the electron-phonon coupling strength by ~50% and that the transition from layered antiferromagnetic to ferromagnetic order tunes the spectral intensity of the periodic broad modes, suggesting a strong coupling among the lattice, charge and spin in two-dimensional CrI3. Our study opens opportunities for tailoring light-matter interactions in two-dimensional magnetic semiconductors.

Suggested Citation

  • Wencan Jin & Hyun Ho Kim & Zhipeng Ye & Gaihua Ye & Laura Rojas & Xiangpeng Luo & Bowen Yang & Fangzhou Yin & Jason Shih An Horng & Shangjie Tian & Yang Fu & Gongjun Xu & Hui Deng & Hechang Lei & Adam, 2020. "Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet CrI3," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18627-x
    DOI: 10.1038/s41467-020-18627-x
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    Cited by:

    1. Emre Ergeçen & Batyr Ilyas & Dan Mao & Hoi Chun Po & Mehmet Burak Yilmaz & Junghyun Kim & Je-Geun Park & T. Senthil & Nuh Gedik, 2022. "Magnetically brightened dark electron-phonon bound states in a van der Waals antiferromagnet," Nature Communications, Nature, vol. 13(1), pages 1-7, December.

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