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

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.

journal_name

Nat Commun

journal_title

Nature communications

authors

Jin W,Kim HH,Ye Z,Ye G,Rojas L,Luo X,Yang B,Yin F,Horng JSA,Tian S,Fu Y,Xu G,Deng H,Lei H,Tsen AW,Sun K,He R,Zhao L

doi

10.1038/s41467-020-18627-x

subject

Has Abstract

pub_date

2020-09-22 00:00:00

pages

4780

issue

1

issn

2041-1723

pii

10.1038/s41467-020-18627-x

journal_volume

11

pub_type

杂志文章

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