Large cross-polarized Raman signal in CrI${}_3$: A first-principles study

Abstract

We find unusually large cross-polarized (and anti-symmetric) Raman signature of A${}_{\mathrm{g}}$ phonon mode in CrI${}_3$, in agreement with experiments. The signal is present only when the following three effects are considered in concert: ferromagnetism on Cr atoms, spin-orbit interaction, and resonant effects. Somewhat surprisingly, we find that the relevant spin-orbit interaction potential originates from iodine atoms, despite magnetism being mostly on chromium atoms. We analyze the Raman signature as a function of magnetic order, the direction of the magnetic moment, energy and polarization of light used for Raman scattering, as well as carrier lifetime. In addition to a strong cross-polarized Raman signal, we also find unusually strong phonon modulated magneto-optical Kerr effect (MOKE) in CrI${}_3$.

arXiv comment10 pages, 12 figures

References in corpus (27)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
• Optimized norm-conserving Vanderbilt pseudopotentials
• Electric-field switching of two-dimensional van der Waals magnets
• On the origin of magnetic anisotropy in two dimensional CrI${}_3$
• Very Large Tunneling Magnetoresistance in Layered Magnetic Semiconductor CrI${}_3$
• Pressure-controlled interlayer magnetism in atomically thin CrI3
• Ligand-field helical luminescence in a 2D ferromagnetic insulator
• Giant enhancement of interlayer exchange in an ultrathin 2D magnet
• Raman Spectroscopy, Photocatalytic Degradation and Stabilization of Atomically Thin Chromium Triiodide
• Direct observation of 2D magnons in atomically thin CrI${}_3$
• Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
• Tuning Inelastic Light Scattering via Symmetry Control in 2D Magnet CrI${}_3$
• Three-dimensional magnetic critical behavior in CrI${}_3$
• Distinct spin-lattice and spin-phonon interactions in monolayer magnetic CrI${}_3$
• Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3
• Magnetism and Magneto-optical Effects in Bulk and Few-layer CrI${}_3$: A Theoretical GGA + U Study
• Magnetic field-induced quantum phase transitions in a van der Waals magnet
• Microscopic origin of ferromagnetism in trihalides CrCl${}_3$ and CrI${}_3$
• Magnetic order induced polarization anomaly of Raman scattering in 2D magnet CrI${}_3$
• Magneto-optical response of chromium trihalide monolayers: chemical trends
• Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet $\mathrm{Cr}{\mathrm{I}}_3$
• Lattice dynamics and phase transition in CrI${}_3$ single crystals
• Raman Spectrum of CrI${}_3$: an ab-initio study
• Accessing new magnetic regimes by tuning the ligand spin-orbit coupling in van der Waals magnets
• Layer Dependence of Stacking Order in Nonencapsulated Few-layer CrI3
• Phonon-mediated dimensional crossover in bilayer CrI3

Cited by in corpus (3)

• Coherent Helicity-Dependent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3
• Terahertz Magnetic and Lattice Excitations in van der Waals Ferromagnet VI3
• Superexchange and spin-orbit coupling in monolayer and bilayer chromium trihalides