We report the two-dimensional (2D) H-Tl₂O/CrI₃ van der Waals (vdW) heterostructure as a promising valleytronics materials, and investigate the manipulation of valley polarization and valley spin splitting of it by using the first principle calculations. The H-Tl2O/CrI₃ heterostructure displays the valley polarization in both the conduction and valence band at two valleys. Especially, the valley polarization can be reached to 14.95 meV at the conduction band. Also, a large valley spin splitting of 0.57 (0.58) eV at the K (K') points are shown in the conduction band. With the manipulation of the interlayer spacing and the in-plane biaxial strain, both the valley polarization and the valley spin splitting for the H-Tl₂O/CrI₃ heterostructure follow the short-range effects of interfacial orbital hybridization, thus a nearly linear relationship is shown. Our work not only provides the application prospects of the H-Tl₂O/CrI₃ heterostructure nanodevices, but also gives theoretical effective support for further development of valleytronics.

我们报告二维（2D）H-Tl ₂ O / CrI ₃范德华（vdW）异质结构作为一种有前途的山谷电子材料，并利用第一原理计算研究了山谷极化和山谷自旋分裂的操纵。H-Tl2O / CrI ₃异质结构在两个波谷的导带和价带中均显示波谷极化。特别是，在导带处，谷底极化可以达到14.95meV。另外，在导带中显示了在K（K'）点处的0.57（0.58）eV的大谷自旋分裂。通过控制层间间距和面内双轴应变，H-Tl ₂ O / CrI的波谷极化和波谷自旋分裂₃异质结构遵循界面轨道杂交的短程效应，因此显示出近乎线性的关系。我们的工作不仅为H-Tl ₂ O / CrI ₃异质结构纳米器件提供了应用前景，而且为Valleytronics的进一步发展提供了理论上的有效支持。