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Alkali antimonide semiconductor photocathodes provide a promising platform for the generation of high-brightness electron beams, which are necessary for the development of cutting-edge probes, including x-ray free electron lasers and ultrafast electron diffraction. Nonetheless, to harness the intrinsic brightness limits in these compounds, extrinsic degrading factors, including surface roughness and contamination, must be overcome. By exploring the growth of CsxSb thin films monitored by in situ electron diffraction, the conditions to reproducibly synthesize atomically smooth films of CsSb on 3C–SiC (100) and graphene-coated TiO2 (110) substrates are identified, and detailed structural, morphological, and electronic characterization is presented. These films combine high quantum efficiency in the visible (up to 1.2% at 400 nm), an easily accessible photoemission threshold of 566 nm, low surface roughness (down to 600 pm on a 1 μm scale), and a robustness against oxidation up to 15 times greater than Cs3Sb. These properties lead us to suggest that CsSb has the potential to operate as an alternative to Cs3Sb in electron source applications where the demands of the vacuum environment might otherwise preclude the use of traditional alkali antimonides. [ABSTRACT FROM AUTHOR]