Epitaxial Oxide Thin Films with High Entropy and Anomalous Crystallinity

Abstract

Pulsed laser deposition (PLD) expands the compositional and structural possibilities of high-entropy oxide (HEO) thin films through far-from-equilibrium growth and kinetic arrest of metastable configurations. This review connects growth kinetics and epitaxial constraints to the roles of individual cations in shaping the resulting films. We focus primarily on rock salt MgCoNiCuZnO and its derivatives, with selected fluorite, spinel, and perovskite examples illustrating broader applicability. In MgCoNiCuZnO, Co valence and Cu coordination illustrate how chemistry and growth conditions jointly enable lattice tuning and coherent nanostructure formation, while aliovalent and size-misfit additions expand the accessible defect and compositional landscapes. These coupled degrees of freedom underpin anomalous crystallinity, the coexistence of extensive chemical disorder with exceptional crystalline quality and epitaxial order, including full coherence in selected systems, particularly rock salts grown on MgO. This combination opens opportunities to discover and engineer functional configurations in high-quality single-layer films and heterostructures.