Manipulation of valley-pseudospin in 2D WTe2/CrI3 van der Waals heterostructure by magnetic proximity effect

Lifting the valley degeneracy is an essential condition for exploiting the valley degrees of freedom to process and store information in valleytronics. The magnetic proximity effect (MPE) has been proven to be an effective method for introducing a magnetic field via interlayer exchange interaction, which can be conveniently achieved by two-dimensional (2D) van der Waals (vdW) heterostructure engineering. We have investigated the electronic properties and valley physics of 2D WTe2/CrI3 heterostructure using first-principles calculations. The results show that a significant valley splitting of 34.01 meV can be obtained in the WTe2/CrI3 heterostructure due to the simultaneous breaking of inversion and time-reversal symmetry, which sensitively depends on the atomic overlap of the projected position in the specific stacking model. In addition, we also show that the valley splitting can be enhanced by applying a vertical external electric field (E-field) or reducing the interlayer distance. More than that, it can be boosted by an order of magnitude (∼115.25 meV) through Cr ion intercalation. This is attributed to that the self-intercalated Cr ion has ferromagnetic (FM) ordering and perpendicular magnetic anisotropy due to the exchange coupling of the CrI3 layer. This result provides fundamental insights and valuable guidance for the application of 2D WTe2/CrI3 heterostructure in novel spintronic and valleytronic devices.