Revealing the (111) surface electronic structure of epitaxially grown Na2KSb photocathode

A recent study has established the Na2KSb(Cs) photocathode as a highly efficient emitter of spin-polarized electrons. However, the electronic structure of alkali antimonides remains poorly understood. In this work, we report the first crystalline epitaxial growth of Na2KSb films, achieved via chemical vapor deposition (CVD) on a graphene-coated SiC(0001) substrate. The high crystalline quality of these films enabled a direct investigation of the material’s electronic structure using angle-resolved photoemission spectroscopy (ARPES). By comparing the experimental results with density functional theory (DFT) calculations, we have identified dispersive surface states originating from different terminations of the Na2KSb(111) surface. Furthermore, we demonstrate that the crystalline order of the film is preserved following its activation via the deposition of Cs and Sb. This finding opens a pathway for investigating the electronic structure of multialkali Na2KSb(Cs) photocathodes and for rationally improving their properties.