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.

arXiv commentTo appear in Nature Nanotechnology

References in corpus (19)

• Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
• Electrical Control of 2D Magnetism in Bilayer CrI3
• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Electric-field switching of two-dimensional van der Waals magnets
• Strongly enhanced charge-density-wave order in monolayer NbSe${}_2$
• Giant and nonreciprocal second harmonic generation from layered antiferromagnetism in bilayer CrI3
• Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3
• Direct photoluminescence probing of ferromagnetism in monolayer two-dimensional CrBr3
• Ligand-field helical luminescence in a 2D ferromagnetic insulator
• Giant enhancement of interlayer exchange in an ultrathin 2D magnet
• Antiferromagnetic ordering in van der Waals two-dimensional magnetic material MnPS3 probed by Raman spectroscopy
• Amplitude `Higgs' mode in 2H-NbSe2 Superconductor
• Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
• Gate-controllable magneto-optic Kerr effect in layered collinear antiferromagnets
• Raman fingerprint of two terahertz spin wave branches in a two-dimensional honeycomb Ising ferromagnet
• Distinct spin-lattice and spin-phonon interactions in monolayer magnetic CrI${}_3$
• Physical origin of Davydov splitting and resonant Raman spectroscopy of Davydov components in multilayer MoTe2
• Raman Spectrum of CrI${}_3$: an ab-initio study
• Chiral Spin Mode on the Surface of a Topological Insulator

Cited by in corpus (36)

• Magnetic Order and Symmetry in the 2D Semiconductor CrSBr
• Engineering symmetry breaking in two-dimensional layered materials
• Interlayer Electronic Coupling on Demand in a 2D Magnetic Semiconductor
• Direct observation of 2D magnons in atomically thin CrI${}_3$
• Twist engineering of the two-dimensional magnetism in double bilayer chromium triiodide homostructures
• Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3
• Magnetic field effect on topological spin excitations in CrI${}_3$
• Magnetic field-induced quantum phase transitions in a van der Waals magnet
• Magnetic order induced polarization anomaly of Raman scattering in 2D magnet CrI${}_3$
• Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet $\mathrm{Cr}{\mathrm{I}}_3$
• Giant magneto-birefringence effect and tuneable colouration of 2D crystals' suspensions
• Observation of nonreciprocal magneto-optical scattering in nonencapsulated few-layered CrI3
• Spin Dynamics in van der Waals Magnetic Systems
• Coherent Helicity-Dependent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3
• 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${}_3$
• Spin-Valley Polarized Quantum Anomalous Hall Effect and a Valley-Controlled Half Metal in Bilayer Graphene
• Two-dimensional ferromagnetic semiconductor VBr3 with tunable anisotropy
• Magnon-phonon interactions enhance the gap at the Dirac point in the spin-wave spectra of CrI${}_3$ two-dimensional magnets
• Thickness dependence of antiferromagnetic phase transition in Heisenberg-type MnPS3
• 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${}_3$
• Large cross-polarized Raman signal in CrI${}_3$: A first-principles study
• 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
• Raman spectroscopy of van der Waals topological magnet GdGaI