Gate modulation of the long-range magnetic order in a vanadium-doped WSe2 semiconductor

Generation of spin-charge coupling by doping semiconductors with magnetic dopants is a promising approach for gate-tunable spintronic devices without applying an external magnetic field. Here, we demonstrate that the magnetic orders in V-doped WSe2 can be modulated by tuning carrier densities using ab initio calculations. We found that at a low V-doping concentration limit, the long-range ferromagnetic order is enhanced by increasing the hole density. In contrast, this long-range ferromagnetic order is suppressed at high electron density by compensating the p-type V dopant, originating from the strong localized antiferromagnetic coupling between V and W atoms and between V and Se atoms. The hole-mediated long-range magnetic exchange is ∼70 meV, thus strongly suggesting the ferromagnetism in V-doped WSe2 at room temperature. Our findings on strong coupling between charge and spin order in V-doped WSe2 provide plenty of room for multifunctional gate-tunable spintronics.