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Perovskite oxynitrides have been studied with regard to their visible light-driven photocatalytic activity and novel electronic functionalities. The assessment of the intrinsic physical and/or electrochemical properties of oxynitrides requires the epitaxial growth of single-crystalline films. However, the heteroepitaxy of perovskite oxynitrides has not yet matured compared to the progress realized in work with perovskite oxides. Herein, we report the heteroepitaxial growth of CaTaO 2 N thin films with (100) pc , (110) pc , and (111) pc crystallographic surface orientations (where the subscript pc denotes a pseudocubic cell) on SrTiO 3 substrates using reactive radio frequency magnetron sputtering, along with investigations of crystallinity and surface morphology. Irrespective of surface orientation, stoichiometric CaTaO 2 N epitaxial thin films were grown coherently on SrTiO 3 substrates and showed clear step and terrace surfaces in the case of low values of film thickness of approximately 20 nm. A (110) pc -oriented film was also more highly crystalline than (100) pc - and (111) pc -oriented specimens. This relationship between crystallinity and surface orientation is ascribed to the number of inequivalent in-plane rotational domains, which stems from the symmetry mismatch between the orthorhombic CaTaO 2 N and cubic SrTiO 3 . A CaTaO 2 N thin film grown on a lattice- and symmetry-matched orthorhombic DyScO 3 substrate exhibited a significant crystallinity and a clear step and terrace surface even though the film was thick (∼190 nm). These results are expected to assist in developing the heteroepitaxial growth of high-quality perovskite oxynitride thin films.

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High-Quality Heteroepitaxial Growth of Thin Films of the Perovskite Oxynitride CaTaO<sub>2</sub>N: Importance of Interfacial Symmetry Matching between Films and Substrates

High-Quality Heteroepitaxial Growth of Thin Films of the Perovskite Oxynitride CaTaO2N: Importance of Interfacial Symmetry Matching between Films and Substrates

High-Quality Heteroepitaxial Growth of Thin Films of the Perovskite Oxynitride CaTaO₂N: Importance of Interfacial Symmetry Matching between Films and Substrates