Tuning Inelastic Light Scattering via Symmetry Control in 2D Magnet CrI${}_3$

Abstract

The coupling between spin and charge degrees of freedom in a crystal imparts strong optical signatures on scattered electromagnetic waves. This has led to magneto-optical effects with a host of applications, from the sensitive detection of local magnetic order to optical modulation and data storage technologies. Here, we demonstrate a new magneto-optical effect, namely, the tuning of inelastically scattered light through symmetry control in atomically thin chromium triiodide (CrI${}_3$). In monolayers, we found an extraordinarily large magneto-optical Raman effect from an A${}_{1g}$ phonon mode due to the emergence of ferromagnetic order. The linearly polarized, inelastically scattered light rotates by ~40${}^o$, more than two orders of magnitude larger than the rotation from MOKE under the same experimental conditions. In CrI${}_3$ bilayers, we show that the same A${}_{1g}$ phonon mode becomes Davydov-split into two modes of opposite parity, exhibiting divergent selection rules that depend on inversion symmetry and the underlying magnetic order. By switching between the antiferromagnetic states and the fully spin-polarized states with applied magnetic and electric fields, we demonstrate the magnetoelectrical control over their selection rules. Our work underscores the unique opportunities provided by 2D magnets for controlling the combined time-reversal and inversion symmetries to manipulate Raman optical selection rules and for exploring emergent magneto-optical effects and spin-phonon coupled physics.

To appear in Nature Nanotechnology

References in corpus (7)

• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3
• Direct photoluminescence probing of ferromagnetism in monolayer two-dimensional CrBr3
• Antiferromagnetic ordering in van der Waals two-dimensional magnetic material MnPS3 probed by Raman spectroscopy
• Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
• Gate-controllable magneto-optic Kerr effect in layered collinear antiferromagnets
• Chiral Spin Mode on the Surface of a Topological Insulator

Cited by in corpus (25)

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• Magnetic order induced polarization anomaly of Raman scattering in 2D magnet CrI${}_3$
• Giant magneto-birefringence effect and tuneable colouration of 2D crystals' suspensions
• Spin Dynamics in van der Waals Magnetic Systems
• Progress and Prospects in Two-Dimensional Magnetism of van der Waals Materials
• Tunable layered-magnetism-assisted magneto-Raman effect in a two-dimensional magnet $\mathrm{Cr}{\mathrm{I}}_3$
• Unified Treatment of Magnons and Excitons in Monolayer CrI${}_3$ from Many-Body Perturbation Theory
• Anisotropic magnetocaloric effect and critical behavior in CrCl${}_3$
• Magnon-phonon interactions enhance the gap at the Dirac point in the spin-wave spectra of CrI${}_3$ two-dimensional magnets
• 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${}_3$
• First-principles calculations of double resonance Raman spectra for monolayer MoTe${}_2$
• Growth of high-quality CrI3 single crystals and engineering of its magnetic properties via V and Mn doping
• Uncovering the Hidden Ferroaxial Density Wave as the Origin of the Axial Higgs Mode in RTe${}_3$
• Rashba-induced spin texture and spin-layer-locking effects in the antiferromagnetic CrI3 bilayer
• Dynamical mean-field theory study of a ferromagnetic CrI3 monolayer
• Van der Waals CrSBr alloys with tunable magnetic and optical properties
• Group Theory Analysis of Phonons in Monolayer Chromium Trihalides and Their Janus Structures
• Symmetry analysis of cross-circular and parallel-circular Raman optical activity
• Resistive anisotropy in the charge density wave phase of Kagome superconductor CsV3Sb5 thin films
• Voltage-controlled topological spin textures in the monolayer limit
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