The morphology of sequentially sputtered metallic precursors and CuIn1−xGaxSe2 thin films prepared using a novel two‐stage selenization process was found to change from initially very smooth layers with a root‐mean‐square (rms) surface roughness of <10 Å to coalescing grains with a fine (∼200 Å) subgrain structure, three‐dimensional ∼9000 Å size islands, and finally to compact, well‐faceted, large ∼1 μm grain‐size CuIn1−xGaxSe2 thin films with a rms roughness of 950–1500 Å. Insitu homogenization of Cu‐rich precursors prior to the first selenization and a maximum selenization temperature of 550–560 °C that provided beneficial fluxing action of copper selenide improved the morphology of completed CuIn1−xGaxSe2 thin films and the photovoltaic conversion efficiency of the solar cells.

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