Emergent Epitaxial Configuration of Pr₃IrO₇ Domains via YSZ (111) Substrate

The 5d rare Earth iridate is an intriguing material with exhibiting exotic electronic and magnetic phases due to spin‐orbit coupled states. Ternary iridium oxides Ln₃IrO₇ contain an unusual Ir⁵⁺ (5d⁴) system, which remain a subject of active research. Fabricating epitaxial Ln₃IrO₇ films is challenging due to substrate compatibility, but it offers a valuable platform to explore electronic and magnetic behaviors under reduced dimensionality and substrate interactions, revealing novel phenomena based on Ir⁵⁺ (5d⁴). In this regard, this demonstrates that Pr₃IrO₇ with its highly anisotropic orthorhombic structure can be epitaxially grown on a cubic (111)‐oriented yttrium‐stabilized ZrO₂ (YSZ) substrate. Pr₃IrO₇ film exhibits six epitaxial domains, where the (220) and (202) planes aligning epitaxially to YSZ (111) with the threefold symmetry. This diverse domain configuration in Pr₃IrO₇ film leads to unique magnetic properties, exhibiting spin‐glass‐like behavior. Pr₃IrO₇ thin film offers a platform for exploring unconventional magnetic states, and their successful heteroepitaxy on YSZ substrates opens new avenues for discovering novel physical phenomena.