Revealing the (111) surface electronic structure of epitaxially grown Na${}_2$KSb photocathode

A recent study has established the Na${}_2$KSb(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 Na${}_2$KSb 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 Na${}_2$KSb(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 Na${}_2$KSb(Cs) photocathodes and for rationally improving their properties.