Strain Tuning in Complex Oxide Epitaxial Films Using an Ultrathin Strontium Aluminate Buffer Layer

A reliable method to apply biaxial strain over a wide range of values with minimal dislocation generation is critical for the study of strain dependent physical properties in oxide thin films and heterostructures. In this work, we systematically controlled the strain state in a perovskite manganite thin film by as much as 1% using a new ultrathin strain‐releasing buffer layer Sr₃Al₂O₆, and observed signatures of accompanying magnetic and metal–insulator transitions. The near‐zero strain state is achieved within five nanometers of buffer layer thickness, substantially thinner than any oxide epitaxial buffer layers that can continuously tune the film strain states. Furthermore, the majority of misfit dislocations were confined to the Sr₃Al₂O₆ layer, structurally decoupling defects in the film from the substrate.