Interlayer magnetic interactions in π / 3 -twisted bilayer CrI₃

The interlayer magnetic interaction in bilayer CrI3 plays a crucial role for its device applications. In this work, we studied the interlayer magnetic interaction in π / 3-twisted bilayer CrI3 using first-principles calculations. Our calculations show that the interlayer coupling can be ferromagnetic or antiferromagnetic depending crucially on lateral shift. The strongest antiferromagnetic interlayer interaction appears in the A ¯ A-stacking. The magnetic force theory calculations demonstrate that such an antiferromagnetic interaction is dominated by the eg-eg channel. Particularly, the interlayer antiferromagnetic interaction is very sensitive to external pressure. This highly tunable interlayer interaction makes π / 3-twisted bilayer CrI3 a potential building block for magnetic field effect transistors and pressure sensors.