Dynamical correlations in single-layer CrI${}_3$

Abstract

Chromium triiodide is an intrinsically magnetic van der Waals material down to the single-layer limit. Here, we provide a first-principles description of finite-temperature magnetic and spectral properties of monolayer (ML) CrI${}_3$ based on fully charge self-consistent density functional theory (DFT) combined with dynamical mean-field theory, revealing a formation of local moments on Cr from strong local Coulomb interactions. We show that the presence of local dynamical correlations leads to a modification of the electronic structure of ferromagnetically ordered CrI${}_3$. In contrast to conventional DFT+$U$ calculations, we find that the top of the valence band in ML CrI${}_3$ demonstrates essentially different orbital character for minority and majority spin states, which is closer to the standard DFT results. This leads to a strong spin polarization of the optical conductivity upon hole doping, which could be verified experimentally.

arXiv commentFinal version; 9 pages, 4 figures

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• Delving into the anisotropic interlayer exchange in bilayer CrI${}_3$
• Robust polaritons in magnetic monolayers of CrI3
• Hole doping as an efficient route to increase the Curie temperature in monolayer CrI${}_3$
• Manifestation of incoherent-coherent crossover and non-Stoner magnetism in the electronic structure of Fe${}_3$GeTe${}_2$
• Linear Response Based Theories for Dzyaloshinskii-Moriya Interactions