Crossover from Ising- to Rashba-type superconductivity in epitaxial Bi₂Se₃/monolayer NbSe₂ heterostructures

A topological insulator (TI) interfaced with an s-wave superconductor has been predicted to host topological superconductivity. Although the growth of epitaxial TI films on s-wave superconductors has been achieved by molecular-beam epitaxy, it remains an outstanding challenge for synthesizing atomically thin TI/superconductor heterostructures, which are critical for engineering the topological superconducting phase. Here we used molecular-beam epitaxy to grow Bi₂Se₃ films with a controlled thickness on monolayer NbSe₂ and performed in situ angle-resolved photoemission spectroscopy and ex situ magnetotransport measurements on these heterostructures. We found that the emergence of Rashba-type bulk quantum-well bands and spin-non-degenerate surface states coincides with a marked suppression of the in-plane upper critical magnetic field of the superconductivity in Bi₂Se₃/monolayer NbSe₂ heterostructures. This is a signature of a crossover from Ising- to Rashba-type superconducting pairings, induced by altering the Bi₂Se₃ film thickness. Our work opens a route for exploring a robust topological superconducting phase in TI/Ising superconductor heterostructures.