van der Waals heterostructures made from graphene and three-dimensional topological insulators promise very high electron mobilities, a nontrivial spin texture, and a gate-tunability of electronic properties. Such a combination of advantageous electronic characteristics can only be achieved through proximity effects in heterostructures, as graphene lacks a large enough spin-orbit interaction. In turn, the heterostructures are promising candidates for all-electrical control of proximity-induced spin phenomena. Here, we explore epitaxially grown interfaces between graphene and the lattice-matched topological insulator Bi2Te2Se. For this heterostructure, spin-orbit coupling proximity has been predicted to impart an anisotropic and electronically tunable spin texture. Polarization-resolved second-harmonic generation, Raman spectroscopy, and time-resolved magneto-optic Kerr microscopy are combined to demonstrate that the atomic interfaces align in a commensurate symmetry with characteristic interlayer vibrations. By polarization-resolved photocurrent measurements, we find a circular photogalvanic effect which is drastically enhanced at the Dirac point of the proximitized graphene. We attribute the peculiar gate-tunability to the proximity-induced interfacial spin structure, which could be exploited for, e.g., spin filters.
Keywords: Raman spectroscopy; graphene; heterostructure; photocurrent; second-harmonic generation; topological insulator; van der Waals epitaxy.