Tunable Electronic Properties and Large Rashba Splittings Found in Few-Layer Bi2Se3/PtSe2 Van der Waals Heterostructures

Abstract We use first-principles calculations to show that van der Waals (vdW) heterostructures consisting of few-layer Bi2Se3 and PtSe2 exhibit electronic and spintronics properties that can be tuned by varying the constituent layers. Type-II band alignment with layer-tunable band gaps and type-III band alignment with spin-splittings have been found. Most notably, we reveal the coexistence of Rashba-type spin-splittings (with large αR parameters) in both the conduction and valence band stemming from few-layer Bi2Se3 and PtSe2, respectively, which has been confirmed by spin-texture plots. We discuss the role of inversion symmetry breaking, changes in orbital hybridization, and spin–orbit coupling in altering electronic dispersion near the Fermi level. Since low-temperature growth mechanisms are available for both materials, we believe that few-layer Bi2Se3/PtSe2 vdW heterostructures are feasible to realize experimentally, offering great potential for electronic and spintronics applications.