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We present the temperature- and thickness-dependent structural andmorphological evolution of strain induced transformations in highly-strainedepitaxial BiFeO3 films deposited on LaAlO3 (001) substrates. Usinghigh-resolution X-ray diffraction and temperature-dependentscanning-probe-based studies we observe a complex temperature- andthickness-dependent evolution of phases in this system. A thickness-dependenttransformation from a single monoclinically distorted tetragonal-like phase toa complex mixed-phase structure in films with thicknesses up to ~200 nm is theconsequence of a strain-induced spinodal instability in the BiFeO3/LaAlO3system. Additionally, a breakdown of this strain-stabilized metastablemixed-phase structure to non-epitaxial microcrystals of the parent rhombohedralstructure of BiFeO3 is observed to occur at a critical thickness of ~300 nm. Wefurther propose a mechanism for this abrupt breakdown that provides insightinto the competing nature of the phases in this system.

Temperature and thickness evolution and epitaxial breakdown in highly-strained BiFeO3 thin films