Evidence for highly p-type doping and type II band alignment in large scale monolayer WSe₂/Se-terminated GaAs...

Two-dimensional materials (2D) arranged in hybrid van der Waals (vdW) heterostructures provide a route toward the assembly of 2D and conventional III-V semiconductors. Here, we report the structural and electronic properties of single layer WSe₂ grown by molecular beam epitaxy on Se-terminated GaAs(111)B. Reflection high-energy electron diffraction images exhibit sharp streaky features indicative of a high-quality WSe₂ layer produced via vdW epitaxy. This is confirmed by in-plane X-ray diffraction. The single layer of WSe₂ and the absence of interdiffusion at the interface are confirmed by high resolution X-ray photoemission spectroscopy and high-resolution transmission microscopy. Angle-resolved photoemission investigation revealed a well-defined WSe₂ band dispersion and a high p-doping coming from the charge transfer between the WSe₂ monolayer and the Se-terminated GaAs substrate. By comparing our results with local and hybrid functionals theoretical calculation, we find that the top of the valence band of the experimental heterostructure is close to the calculations for free standing single layer WSe₂. Our experiments demonstrate that the proximity of the Se-terminated GaAs substrate can significantly tune the electronic properties of WSe₂. The valence band maximum (VBM, located at the K point of the Brillouin zone) presents an upshift of about 0.56 eV toward the Fermi level with respect to the VBM of the WSe₂ on graphene layer, which is indicative of high p-type doping and a key feature for applications in nanoelectronics and optoelectronics.