Proximity exchange effects in MoSe2 and WSe2 heterostructures with CrI3 : Twist angle, layer, and gate dependence

Proximity effects in two-dimensional (2D) van der Waals heterostructures offer controllable ways to tailor the electronic band structure of adjacent materials. Exchange proximity in particular is important for making materials magnetic without hosting magnetic ions. Such synthetic magnets could be used for studying magnetotransport in high-mobility 2D materials, or magneto-optics in highly absorptive nominally nonmagnetic semiconductors. Using first-principles calculations, we show that the proximity exchange in monolayer MoSe$_2$ and WSe$_2$ due to ferromagnetic monolayer CrI$_3$ can be tuned (even qualitatively) by twisting and gating. Remarkably, the proximity exchange remains the same when using antiferromagnetic CrI$_3$ bilayer, paving the way for optical and electrical detection of layered antiferromagnets. Interestingly, the proximity exchange is opposite to the exchange of the adjacent antiferromagnetic layer. Finally, we show that the exchange proximity is confined to the layer adjacent to CrI$_3$, and that adding a separating hBN barrier drastically reduces the proximity effect. We complement our it ab initio results with tight-binding modeling and solve the Bethe-Salpeter equation to provide experimentally verifiable optical signatures (in the exciton spectra) of the proximity exchange effects.