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Heterostructures of topological insulator Bi$_2$Se$_3$ on transition metaldichalcogenides (TMDCs) offer a new materials platform for studying novelquantum states by exploiting the interplay among topological orders, chargeorders and magnetic orders. The diverse interface attributes, such as materialcombination, charge re-arrangement, defect and strain, can be utilized tomanipulate the quantum properties of this class of materials. Recentexperiments of Bi$_2$Se$_3$/NbSe$_2$ heterostructures show signatures of strongRashba band splitting due to the presence of a BiSe buffer layer, but theatomic level mechanism is not fully understood. We conduct first-principlesstudies of the Bi$_2$Se$_3$/BiSe/TMDC heterostructures with five different TMDCsubstrates (1T phase VSe$_2$, MoSe$_2$, TiSe$_2$, and 2H phase NbSe$_2$,MoSe$_2$). We find significant charge transfer at both BiSe/TMDC andBi$_2$Se$_3$/BiSe interfaces driven by the work function difference, whichstabilizes the BiSe layer as an electron donor and creates interface dipole.The electric field of the interface dipole breaks the inversion symmetry in theBi$_2$Se$_3$ layer, leading to the giant Rashba band splitting in two quintuplelayers and the recovery of the Dirac point in three quintuple layers, with thelatter otherwise only occurring in thicker samples with at least sixBi$_2$Se$_3$ quintuple layers. Besides, we find that strain can significantlyaffect the charge transfer at the interfaces. Our study presents a promisingavenue for tuning topological properties in heterostructures of two-dimensionalmaterials, with potential applications in quantum devices.

Manipulating Topological Properties in Bi$_2$Se$_3$/BiSe/TMDC Heterostructures with Interface Charge Transfer