Switchable Interlayer Magnetic Coupling of Bilayer CrI(3)

Due to the weak van der Waals (vdW) interlayer interaction, interfacial geometry of two-dimensional (2D) magnetic vdW materials can be freely assembled, and the stacking order between layers can be readily controlled, such as laterally shifting or rotating, which may trigger the variation of magnetic order. We investigate the H-type bilayer CrI [Formula: see text] where the two layers are aligned in anti-parallel directions. Based on first-principles calculations, we propose two states with different interlayer magnetic couplings, i.e., ferromagnetic and antiferromagnetic, and analyze the superexchange mechanism inside. It is found that the two magnetic coupling states are stacking-dependent, and could be switched by applying out-of-plane axial strain and electron doping. Our findings show great application potential in the design of heterostructural and spintronic devices based on 2D magnetic vdW materials.