Tao Lei1, Kyung-Hwan Jin2, Nian Zhang1, Jia-Li Zhao1, Chen Liu1, Wen-Jie Li3, Jia-Ou Wang1, Rui Wu1, Hai-Jie Qian1, Feng Liu2,4,5 and Kurash Ibrahim1,5

The electronic state evolution of single bilayer (1BL) Bi(1 1 1) deposited on three-dimensional (3D) Bi2SexTe3−x topological insulators at x = 0, 1.26, 2, 2.46, 3 is systematically investigated by angle-resolved photoemission spectroscopy (ARPES). Our results indicate that the electronic structures of epitaxial Bi films are strongly influenced by the substrate especially the topmost sublayer near the Bi films, manifesting in two main aspects. First, the Se atoms cause a stronger charge transfer effect, which induces a giant Rashba-spin splitting, while the low electronegativity of Te atoms induces a strong hybridization at the interface. Second, the lattice strain notably modifies the band dispersion of the surface bands. Furthermore, our experimental results are elucidated by first-principles band structure calculations.