Dynamical correlations and Mott localization in a paramagnetic VI 3 bulk crystal

We perform a comprehensive study on the correlated electronic structure reconstruction of paramagnetic VI 3 crystal in its rhombohedral and monoclinic structural phases. Using density-functional plus dynamical mean-field theory ( DFT + DMFT ) calculations, we explicitly demonstrate the importance of local dynamical correlations for a consistent understanding of the emergent Mott state, showing the interplay between orbital-dependent one-electron line shape and multiorbital electronic interactions. Our results for the Mott gap are shown to be consistent with extant theory and experimental studies on nonmagnetic VI 3 bulk crystal. We also explore the changes in the strongly correlated electronic state upon increasing the total V band filling of monoclinic VI 3 , showing the robustness of Mott localization against electron doping. Our correlated many-body study is relevant to understanding the electronic structure reconstruction of paramagnetic vanadium-contained trihalide crystals and should be widely applicable to other van der Waals magnetic materials.