Electronic correlation and Mott localization of paramagnetic CrSBr crystal

Abstract

We perform a comprehensive analysis of the correlated electronic structure reconstruction within the paramagnetic phase of CrSBr van der Waals (vdW) crystal. Using generalized gradient approximation plus dynamical mean-field theory calculations, we explicitly demonstrate the importance of local dynamical correlations for a consistent understanding of the emergent Mott localized electronic state, showing the interplay between one-electron lineshape and multi-orbital \(t_{2g}\) electronic interactions. Our strongly correlated many-body scenario is relevant to understanding the electronic structure reconstruction of the \(\hbox {Cr}^{3+}\) oxidation state with nearly half-filled \(t_{2g}\) orbitals and should be applicable to other vdW materials from bulk down to the low-dimensional limit. This work is a step forward in understanding the manifestation of orbital-selective Mott localization and its link to angle-resolved photoemission spectroscopy, electrical resistivity, and the current–voltage characteristic. The presented theoretical results indicate how orbital reconstruction leads to volatile memristive functionality of CrSBr for future neuromorphic computing.