Distinct spin-lattice and spin-phonon interactions in monolayer magnetic CrI${}_3$

Abstract

We apply the density-functional theory to study various phases (including non-magnetic (NM), anti-ferromagnetic (AFM), and ferromagnetic (FM)) in monolayer magnetic chromium triiodide (CrI${}_3$), a recently fabricated 2D magnetic material. It is found that: (1) the introduction of magnetism in monolayer CrI${}_3$ gives rise to metal-to-semiconductor transition; (2) the electronic band topologies as well as the nature of direct and indirect band gaps in either AFM or FM phases exhibit delicate dependence on the magnetic ordering and spin-orbit coupling; and (3)the phonon modes involving Cr atoms are particularly sensitive to the magnetic ordering, highlighting distinct spin-lattice and spin-phonon coupling in this magnet. First-principles simulations of the Raman spectra demonstrate that both frequencies and intensities of the Raman peaks strongly depend on the magnetic ordering. The polarization dependent $A_{1g}$ modes at 77 cm${}^{-1}$ and 130 cm${}^{-1}$ along with the $E_g$ mode at about 50 cm${}^{-1}$ in the FM phase may offer a useful fingerprint to characterize this material. Our results not only provide a detailed guiding map for experimental characterization of CrI${}_3$, but also reveal how the evolution of magnetism can be tracked by its lattice dynamics and Raman response.

arXiv comment17 pages, 8 figures

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Cited by in corpus (30)

• Strain-tunable magnetic anisotropy in monolayer CrCl${}_3$, CrBr${}_3$, and CrI${}_3$
• Switching 2D Magnetic States via Pressure Tuning of Layer Stacking
• Proximity exchange effects in MoSe${}_2$ and WSe${}_2$ heterostructures with CrI${}_3$: twist angle, layer, and gate dependence
• Microscopic understanding of magnetic interactions in bilayer CrI${}_3$
• Strain-tunable orbital, spin-orbit, and optical properties of monolayer transition-metal dichalcogenides
• Tuning Inelastic Light Scattering via Symmetry Control in 2D Magnet CrI${}_3$
• Relativistic exchange interactions in CrX${}_3$ (X=Cl, Br, I) monolayers
• 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 $\mathrm{Cr}{\mathrm{I}}_3$
• Observation of nonreciprocal magneto-optical scattering in nonencapsulated few-layered CrI3
• Strength of effective Coulomb interaction in two-dimensional transition-metal Halides MX${}_2$ and MX${}_3$ (M=Ti, V, Cr, Mn, Fe, Co, Ni; X=Cl, Br, I)
• First-principles studies of spin-phonon coupling in Cr2Ge2Te6 monolayer
• Electronic structure and magnetic properties of few-layer Cr${}_2$Ge${}_2$Te${}_6$: the key role of nonlocal electron-electron interaction effects
• Strain and electric-field control of spin-spin interactions in monolayer CrI${}_3$
• Coherent Helicity-Dependent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3
• A Combined First Principles Study of the Structural, Magnetic, and Phonon Properties of Monolayer CrI${}_3$
• Spin-lattice couplings in two-dimensional CrI${}_3$ from first-principles study
• Tunable layered-magnetism-assisted magneto-Raman effect in a two-dimensional magnet $\mathrm{Cr}{\mathrm{I}}_3$
• Orbital and magnetic ordering in single-layer FePS3: A DFT+U study
• Layer Dependence of Stacking Order in Nonencapsulated Few-layer CrI3
• Magnon-phonon interactions enhance the gap at the Dirac point in the spin-wave spectra of CrI${}_3$ two-dimensional magnets
• Valence band electronic structure of the van der Waals ferromagnetic insulators: VI${}_3$ and CrI${}_3$
• 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 study of the gap in the spin excitation spectrum of the CrI${}_3$ honeycomb ferromagnet
• Toward improved property prediction of 2D materials using many-body quantum Monte Carlo methods
• Large cross-polarized Raman signal in CrI${}_3$: A first-principles study
• Partitioning interatomic force constants for first-principles phonon calculations: Applications to NaCl, PbTiO${}_3$, monolayer CrI${}_3$, and twisted bilayer graphene
• Group Theory Analysis of Phonons in Monolayer Chromium Trihalides and Their Janus Structures