Observation and manipulation of valley polarization in two-dimensional H-Tl2O/CrI3 heterostructure

[Display omitted] •The valley polarization (VP) of the H-Tl2O/CrI3 heterostructure is observed in both the conduction and the valence band.•A large valley spin splitting (VSS) of 0.57 (0.58) eV at the K (K') points are shown in the conduction band.•The VP and the VSS can be manipulated by adjusting the interlayer spacing and the in-plane biaxial strains. We report the two-dimensional H-Tl2O/CrI3 van der Waals (vdW) heterostructure as a promising valleytronic material and investigate its valley polarization and valley spin splitting manipulation using first-principles calculations. The H-Tl2O/CrI3 heterostructure displays valley polarization both in the conduction and valence band at two valleys. Particularly, valley polarization can attain 14.95 meV at the conduction band. In addition, a large valley spin splitting of 0.57 (0.58) eV at the K (K') point is shown in the conduction band. With the manipulation of the interlayer spacing and in-plane biaxial strain, the valley polarization and valley spin splitting of the H-Tl2O/CrI3 heterostructure follow the short-range effects of interfacial orbital hybridization, thus a nearly linear relationship is shown. Our work provides not only application prospects of the H-Tl2O/CrI3 heterostructure nanodevices but also theoretical effective support for research and development of valleytronics.