Data for: "Electronic structure of the interface between Au and WSe2"

Studying the intricate interactions at the interface requires model systems that enable control of the roughness, purity, and crystallinity of the metal surface. Here, we use angle-resolved photoemission spectroscopy to investigate the layer-dependent electronic structure of WSe2 on template-stripped gold substrates fabricated using both silicon and mica templates, giving crystallographically disordered and Au(111) ordered surfaces, respectively, and contrast these findings with ab initio predictions.

We observe strong hybridization around the Brillouin zone centre at $\overline{\Gamma}$, indicating a covalent admixture in the gold-\WSe~interaction, and band shifts that suggest charge rearrangement at the Au(111) / WSe2 interface. Core-level spectroscopy shows a single chemical environment for the interfacial \WSe~layer on the template-stripped gold, distinct from the subsequent layers. These results reveal a mixture of van der Waals and covalent interactions, best described as a covalent-like quasi-bonding with intermediate interaction strength.