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

The 5 d rare Earth iridate is an intriguing material with exhibiting exotic electronic and magnetic phases due to spin‐orbit coupled states. Ternary iridium oxides Ln 3 IrO 7 contain an unusual Ir 5+ (5 d 4 ) system, which remain a subject of active research. Fabricating epitaxial Ln 3 IrO 7 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 Ir 5+ (5 d 4 ). In this regard, this demonstrates that Pr 3 IrO 7 with its highly anisotropic orthorhombic structure can be epitaxially grown on a cubic (111)‐oriented yttrium‐stabilized ZrO 2 (YSZ) substrate. Pr 3 IrO 7 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 Pr 3 IrO 7 film leads to unique magnetic properties, exhibiting spin‐glass‐like behavior. Pr 3 IrO 7 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.