Magnetic order induced polarization anomaly of Raman scattering in 2D magnet CrI${}_3$

Abstract

The recent discovery of 2D magnets has revealed various intriguing phenomena due to the coupling between spin and other degree of freedoms (such as helical photoluminescence, nonreciprocal SHG). Previous research on the spin-phonon coupling effect mainly focuses on the renormalization of phonon frequency. Here we demonstrate that the Raman polarization selection rules of optical phonons can be greatly modified by the magnetic ordering in 2D magnet CrI${}_3$. For monolayer samples, the dominant A${}_{1g}$ peak shows abnormally high intensity in the cross polarization channel at low temperature, which is forbidden by the selection rule based on the lattice symmetry. While for bilayer, this peak is absent in the cross polarization channel for the layered antiferromagnetic (AFM) state and reappears when it is tuned to the ferromagnetic (FM) state by an external magnetic field. Our findings shed light on exploring the emergent magneto-optical effects in 2D magnets.

arXiv comment15 pages, 4 figures

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• Magnetic field-induced quantum phase transitions in a van der Waals magnet
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• Progress and Prospects in Two-Dimensional Magnetism of van der Waals Materials
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• Magnetoelectric Response of Antiferromagnetic Van der Waals Bilayers
• Designing magnetic properties in CrSBr through hydrostatic pressure and ligand substitution
• Structural Monoclinicity and Its Coupling to Layered Magnetism in Few-Layer $\mathrm{Cr}{\mathrm{I}}_3$
• On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS${}_3$ and CrI${}_3$
• Uncovering the Hidden Ferroaxial Density Wave as the Origin of the Axial Higgs Mode in RTe${}_3$
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