Mapping cation diffusion through lattice defects in epitaxial oxide thin films on the water-soluble buffer layer Sr3Al2O6 using atomic resolution electron microscopy

Recent advances in the synthesis of oxide thin films have led to the discovery of novel functionalities that are not accessible in bulk structures. However, their physical properties are vulnerable to the presence of crystal defects, which can give rise to structural, chemical, and electronic modifications. These issues are central to optimizing the opportunities to create freestanding oxide films using the recently developed buffer layer Sr3Al2O6, which is soluble in room temperature water. To evaluate the general possibility to create atomic scale freestanding oxide heterostructures, it is critical to understand the formation, structure, and role of defects as this buffer layer is employed. Here, using aberration-corrected scanning transmission electron microscopy in combination with electron energy loss spectroscopy, we reveal cation segregation and diffusion along crystal defects that form during growth of an oxide multilayer structure on the Sr3Al2O6 buffer layer. We demonstrate that mass transport of film material can occur either through open dislocation core channels or site-specifically in the crystal lattice, causing local variations in stoichiometry. However, by reducing the thermal driving force for diffusion during growth, we suppress the role of extended defects as cation segregation sites, thereby retaining the inherent properties of the overlaying film.