Controllable and enormous spin splitting in antiferromagnetic MnPSe3 through interfacial coupling with Janus MoSSe

Abstract

Abstract The manipulation of spin and valley degree of freedom in two-dimensional materials is desirable for emerging applications in next-generation electronics. Here, we report a regulation of the spin splitting in monolayer antiferromagnetic MnPSe3 through stacking van der Waals (vdW) heterostructures with transition-metal dichalcogenides (TMDs). Different TMDs including Janus MoSSe, MoSe2, and MoS2 are engaged and the spin and valley dependences on stacking configurations, interfacial atoms, and interlayer spacings are comprehensively investigated based on first-principles calculations. The results show that spin degeneracy of MnPSe3 can be lifted through the interfacial interaction in the vdW heterostructures. Compared with the MnPSe3 interfacing with traditional TMDs (MoSe2 and MoS2), those with Janus TMDs (MoSSe or MoSeS) have larger spin splitting. A maximal spin splitting of 50.8 meV at valence band maximum is achieved in MoSSe/MnPSe3 heterostructure, and such splitting is further enhanced to 243.0 meV when the interlayer spacing is reduced to 2.9 Å. It is found that the different hybridizations between the d-orbitals of the two inequivalent Mn atoms in MnPSe3 and the above TMDs lead to the occurrence of net magnetic moments, and thus induce spin splitting. This work paves a novel way to modify the spin-valley properties of two-dimensional semiconductors.