Orbitally-resolved ferromagnetism of monolayer CrI${}_3$

Abstract

Few-layer CrI${}_3$ is the most known example among two-dimensional (2D) ferromagnets, which have attracted growing interest in recent years. Despite considerable efforts and progress in understanding the properties of 2D magnets both from theory and experiment, the mechanism behind the formation of in-plane magnetic ordering in chromium halides is still under debate. Here, we propose a microscopic orbitally-resolved description of ferromagnetism in monolayer CrI${}_3$. Starting from first-principles calculations, we construct a low-energy model for the isotropic Heisenberg exchange interactions. We find that there are two competing contributions to the long-range magnetic ordering in CrI${}_3$: (i) Antiferromagnetic Anderson's superexchange between half-filled $t_{2g}$ orbitals of Cr atoms; and (ii) Ferromagnetic exchange governed by the Kugel-Khomskii mechanism, involving the transitions between half-filled $t_{2g}$ and empty $e_g$ orbitals. Using numerical calculations, we estimate the exchange interactions in momentum-space, which allows us to restore the spin-wave spectrum, as well as estimate the Curie temperature. Contrary to the nearest-neighbor effective models, our calculations suggest the presence of sharp resonances in the spin-wave spectrum at 5--7 meV, depending on the vertical bias voltage. Our estimation of the Curie temperature in monolayer CrI${}_3$ yields 55--65 K, which is in good agreement with experimental data.

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• Relativistic exchange interactions in CrX${}_3$ (X=Cl, Br, I) monolayers
• Curved Magnetism in CrI${}_3$
• Magnetic Anisotropy in Spin-3/2 with Heavy Ligand in Honeycomb Mott Insulators: Application to CrI${}_3$
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• Electron correlation effects on exchange interactions and spin excitations in 2D van der Waals materials
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• Magnon valley Hall effect in CrI3-based vdW heterostructures
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• Monolayer CrCl${}_3$ as an ideal Test Bed for the Universality Classes of 2D Magnetism
• Electronic Structure of Chromium Trihalides beyond Density Functional Theory
• Unified Treatment of Magnons and Excitons in Monolayer CrI${}_3$ from Many-Body Perturbation Theory
• Theory of magnetism in the van der Waals magnet CrI3
• Two-dimensional chromium bismuthate: A room-temperature Ising ferromagnet with tunable magneto-optical response
• Plane wave implementation of the magnetic force theorem for magnetic exchange constants: Application to bulk Fe, Co and Ni
• Dynamical correlations in single-layer CrI${}_3$
• Uniaxial pressure effects in the two-dimensional van-der-Waals ferromagnet CrI${}_3$
• On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS${}_3$ and CrI${}_3$
• Computational methods for 2D materials modelling
• Interlayer magnetic interactions in $\pi /3$-twisted bilayer CrI${}_3$
• All optical resonant magnetization switching in ${\text{CrI}}_3$ monolayers
• Electron transport and scattering mechanisms in ferromagnetic monolayer Fe${}_3$GeTe${}_2$
• Giant gate-tunable renormalization of spin-correlated flat-band states and bandgap in a 2D magnetic insulator
• Superexchange and spin-orbit coupling in monolayer and bilayer chromium trihalides
• Reciprocal space study of Heisenberg exchange interactions in ferromagnetic metals
• Electronic correlation, magnetic structure and magnetotransport in few-layer CrI3
• Dispersive dark excitons in van der Waals ferromagnet CrI3
• Delving into the anisotropic interlayer exchange in bilayer CrI${}_3$
• Robust polaritons in magnetic monolayers of CrI3
• Optimizing Hubbard U parameters for Enhanced Description of Electronic and Magnetic Properties in CrI${}_3$ Monolayers and Bilayers
• Orbital correlations in ultrathin films of late transition metals
• Magnetic domain wall dynamics under external electric field in bilayer CrI${}_3$
• Interlayer superexchange in bilayer chromium trihalides
• Discovery of an ultrastable antiferromagnetic two-dimensional CrF3 phase with anisotropic quasi-one-dimensional mechanical, electronic, and thermal properties
• Environmental Screening and Ligand-Field Effects to Magnetism in CrI${}_3$ Monolayer