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The substitution of hydride anions (H) into transition metal oxides has recently become possible through topotactic reactions or high-pressure synthesis methods. However, the fabrication of oxyhydrides is still difficult because of their inherently less-stable frameworks. In this study, we successfully fabricated perovskite SrCoOH thin films via the topotactic hydride doping of brownmillerite SrCoO epitaxial thin films with CaH. The perovskite-type cation framework was maintained during the topotactic treatment owing to epitaxial stabilization. Structural and chemical analyses accompanied by X-ray absorption spectroscopy measurements revealed that the doped hydride ions form a two-dimensional network of Co-H-Co bonds, in contrast to other reported perovskite oxyhydrides, SrOH ( = Cr, Ti, V). The SrCoOH thin film exhibited insulating behavior and had a direct band gap of 2.1 eV. Thus, topotactic hydride doping of transition-metal-oxide thin films on suitable substrates is a promising method for the synthesis of new transition metal oxyhydrides.


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