Effects of Charge Transfer on the Critical Distance of the Interlayer Ferromagnetic Order Transition in SCrSe‐Based van der Waals Bilayers

Recently, the distance‐dependent interlayer magnetism transition from antiferromagnetic (AFM) to ferromagnetic (FM) has been predicted in many 2D FM bilayers. Effectively controlling critical distance is a key point for reversible AFM–FM transitions. Based on first‐principles calculations, it is found that the critical distance can be modulated by the charge transfer induced by elemental substitution of anionic sublayers in SCrSe‐based van der Waals (vdW) bilayer structures. The interlayer AFM–FM transition is dependent on the interlayer p z overlap, which is determined by the bonding strength (ΔE b) of the covalent‐like quasibonding (CLQB) from the coupling of interlayer p z orbitals. Large critical distance is achieved when the ΔE b is significant in the bilayers. The interlayer p z overlap is altered by inducing intralayer or interlayer charge transfer, modulating the critical distance of interlayer AFM–FM transition. This work contributes to the control of magnetic configurations in layered 2D FM materials. Charge transfer induced by the mutual substitution between S and Se in SCrSe‐based van der Waals (vdW) bilayers modulates the interlayer p z overlap and the critical distance of interlayer AFM–FM transition.