Interplay between interlayer exchange and stacking in CrI$_3$ bilayers

Abstract: We address the interplay between stacking and interlayer exchange for ferromagnetically ordered CrI$_3$, both for bilayers and bulk. Whereas bulk CrI$_3$ is ferromagnetic, both magneto-optical and transport experiments show that interlayer exchange for CrI$_3$ bilayers is antiferromagnetic. Bulk CrI$_3$ is known to assume two crystal structures, rhombohedral and monoclinic, that differ mostly in the stacking between monolayers. Below 210-220 Kelvin, bulk CrI$_3$ orders in a rhombohedral phase. Our density functional theory calculations show a very strong dependence of interlayer exchange and stacking. Specifically, the ground states of both bulk and free-standing CrI$_3$ bilayers are ferromagnetic for the rhombohedral phase. In contrast, the energy difference between both configurations is more than one order of magnitude smaller for the monoclinic phase, and eventually becomes antiferromagnetic when either positive strain or on-site Hubbard interactions ($U \geq 3$) are considered. We also explore the interplay between interlayer hybrydization and stacking, using a Wannier basis, and between interlayer hybrydization and relative magnetic alignment for CrI$_3$ bilayers, that helps to account for the very large tunnel magnetoresistance obvserved in recent experiments.