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 CaTaO2N thin films with (100)pc, (110)pc,
and (111)pc crystallographic surface orientations (where
the subscript pc denotes a pseudocubic cell) on SrTiO3 substrates
using reactive radio frequency magnetron sputtering, along with investigations
of crystallinity and surface morphology. Irrespective of surface orientation,
stoichiometric CaTaO2N epitaxial thin films were grown
coherently on SrTiO3 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 CaTaO2N and cubic SrTiO3. A CaTaO2N thin film
grown on a lattice- and symmetry-matched orthorhombic DyScO3 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.