Electronic structure of rhombohedral CrX3 (X=Br, Cl, I) van der Waals crystals

Abstract

We perform a comprehensive analysis of both the chemical and correlated electronic structure reconstruction of rhombohedral $\mathrm{Cr}{X}_{3}$ $(X=\text{Br}, \mathrm{Cl}, \mathrm{I})$ van der Waals bulk crystals. Using the generalized gradient approximation (GGA) plus dynamical mean-field theory we explicitly demonstrate the importance of local dynamical correlations for a consistent understanding of emergent Kondo quasiparticles and Mott localized electronic states, showing the interplay between material-dependent one-electron GGA line-shape and multiorbital electronic interactions. To probe the correlated paramagnetic electronic state we performed x-ray absorption spectroscopy measurements for ${\mathrm{CrCl}}_{3}$ and ${\mathrm{CrBr}}_{3}$ bulk crystals. Our correlated many-body study is relevant to understanding the electronic structure reconstruction of paramagnetic Cr-trihalide crystals and should be widely applicable to other van der Waals magnetic materials.