The role of atomic oxygen irradiation in the epitaxial crystallization of yttrium-doped barium zirconate thin films fabricated by pulsed laser deposition (PLD) was investigated. X-ray diffraction and transmission electron microscopy revealed that, for films deposited without irradiation, random nucleation and growth occurred below the onset temperature for continuous crystallization at the film-interlayer interface. In contrast, for films deposited with oxygen irradiation, random nucleation and

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... growth was not detected at the temperature of continuous crystallization, which facilitates epitaxial crystallization in these films. This study suggests the combined low temperature deposition with atomic oxygen irradiation and postannealing could control microstructure of solid-state electrochemical devices such as solid oxide fuel cells and solid-state lithium secondary batteries.