Environmental Screening and Ligand-Field Effects to Magnetism in CrI3 Monolayer

Abstract

We study the microscopic origin of magnetism in suspended and dielectrically embedded CrI3 monolayer by down-folding minimal generalized Hubbard models from ab initio calculations using the constrained random phase approximation. These models are capable of describing the formation of localized magnetic moments in CrI3 and of reproducing electronic properties of direct ab initio calculations. Utilizing the magnet force theorem, we find a multi-orbital super-exchange mechanism as the origin of magnetism in CrI3 resulting from an interplay between ferro- and anti-ferromagnetic Cr-Cr d coupling channels, which is decisively affected by the ligand p orbitals. We show how environmental screening, such as resulting from encapsulation with hexagonal boron nitride, affects the Coulomb interaction in the film and how this controls its magnetic properties. Driven by a non-monotonic interplay between nearest and next-nearest neighbor exchange interactions we find the magnon dispersion and the Curie temperature to be non-trivially affected by the environmental screening. © 2021, The Author(s).