Electronic correlation, magnetic structure and magnetotransport in few-layer CrI3

Abstract: Using density functional theory combined with a Hubbard model (DFT+U ), the electronic band structure of CrI3 multilayers, both free-standing and enclosed between graphene contacts, is calculated. We show that the DFT+U approach, together with the 'around mean field' correction scheme, is able to describe the vertical magnetotransport in line with the experimental measurements of magnetoresistance in multi-layered CrI3 enclosed between graphene contacts. Moreover, by interpolating between different double-counting correction schemes, namely the 'around mean field' correction and the fully localized limit, we show their importance for describing both the band structure and the ground-state total energy consistently. Our description of the magnetic exchange interaction is compatible with the experimentally observed antiferromagnetic ground state in the bilayer CrI3 and the transition to a ferromagnetic arrangement in a small external magnetic field. Thus, using spin-polarized DFT+U with an 'around mean field' correction, a consistent overall picture is achieved.