Tunable layered-magnetism-assisted magneto-Raman effect in a two-dimensional magnet $\mathrm{Cr}{\mathrm{I}}_3$

Abstract

We use 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 $\mathrm{Cr}{\mathrm{I}}_3$. We reveal a novel 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 $\mathrm{Cr}{\mathrm{I}}_3$. We resolve in data and by calculations that the 1st-order $A_g$ phonon of monolayer splits into a $N$-fold multiplet in $N$-layer $\mathrm{Cr}{\mathrm{I}}_3$ due to the interlayer coupling ($N$>=2) and that the phonons with the multiple 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 1st-order to higher-order multi-phonon scattering processes. Our results on magneto-Raman effect of the 1st-order phonons in the multiplet and the higher-order multi-phonons in $N$-layer $\mathrm{Cr}{\mathrm{I}}_3$ demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underlines the unique opportunities of new spin-phonon physics in van der Waals layered magnets.

arXiv comment16 pages, 4 figures + supplementary material

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Cited by in corpus (13)

• Twist engineering of the two-dimensional magnetism in double bilayer chromium triiodide homostructures
• Evidence of Noncollinear Spin Texture in Magnetic Moiré Superlattices
• Roadmap for Photonics with 2D Materials
• Coherent Helicity-Dependent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3
• Spin dynamics slowdown near the antiferromagnetic critical point in atomically thin FePS3
• Progress and Prospects in Two-Dimensional Magnetism of van der Waals Materials
• Structural Monoclinicity and Its Coupling to Layered Magnetism in Few-Layer $\mathrm{Cr}{\mathrm{I}}_3$
• Exotic Magnetic and Electronic Properties of Layered CrI3 Single Crystals Under High Pressure
• Direct optical probe of magnon topology in two-dimensional quantum magnets
• Uncovering the Hidden Ferroaxial Density Wave as the Origin of the Axial Higgs Mode in RTe${}_3$
• Symmetry analysis of cross-circular and parallel-circular Raman optical activity
• Band Splitting and Long-lived Carrier Recombination in Ferromagnetic CrSiTe3 Nanosheets
• Raman spectroscopy of van der Waals topological magnet GdGaI