Tunable layered-magnetism-assisted magneto-Raman effect in a two-dimensional magnet CrI3

Wencan Jin, Zhipeng Ye, Xiangpeng Luo, Bowen Yang, Gaihua Ye, Fangzhou Yin, Hyun Ho Kim, Laura Rojas, Shangjie Tian, Yang Fu, Shaohua Yan, Hechang Lei, Kai Sun, Adam W. Tsen, Rui He, Liuyan Zhao

Research output: Contribution to journalArticlepeer-review

Abstract

We used a combination of polarized Raman spectroscopy experiment and model magnetism-phonon coupling calculations to study the rich magneto-Raman effect in the two-dimensional (2D) magnet CrI3. We reveal a layered-magnetism-assisted phonon scattering mechanism below the magnetic onset temperature, whose Raman excitation breaks time-reversal symmetry, has an antisymmetric Raman tensor, and follows the magnetic phase transitions across critical magnetic fields, on top of the presence of the conventional phonon scattering with symmetric Raman tensors in N-layer CrI3. We resolve in data and by calculations that the first-order Ag phonon of the monolayer splits into an N-fold multiplet in N-layer CrI3 due to the interlayer coupling (N≥2) and that the phonons within the multiplet show distinct magnetic field dependence because of their different layered-magnetism-phonon coupling. We further find that such a layered-magnetism-phonon coupled Raman scattering mechanism extends beyond first-order to higher-order multiphonon scattering processes. Our results on the magneto-Raman effect of the first-order phonons in the multiplet and the higherorder multiphonons in N-layer CrI3 demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underline the unique opportunities of spin-phonon physics in van der Waals layered magnets.

Original languageEnglish
Pages (from-to)24664-24669
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume117
Issue number40
DOIs
StatePublished - Oct 6 2020

Keywords

  • Magneto-Raman effect
  • Raman spectroscopy
  • Two-dimensional layered magnetism

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