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

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).We thank M. Kaltak for sharing his cRPA implementation with us. M.I.K. acknowledges support by European Research Council via Synergy Grant 854843—FASTCORR. D.S. thanks financial support from EU through the MSCA project Nr. 796795 SOT-2DvdW. ANR acknowledges partial support from the Russian Science Foundation, Grant No. 21-72-10136. Part of this work was carried out on the Dutch national e-infrastructure with the support of SURF Cooperative