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

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 W. Tsen, Kai Sun, Rui He () and Liuyan Zhao ()
Additional contact information
Wencan Jin: University of Michigan
Hyun Ho Kim: University of Waterloo, Waterloo, 200 University Ave W
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

Nature Communications, 2020, vol. 11, issue 1, 1-7

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-18627-x

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