Atomic ironing for conformal interfaces in freestanding oxide nanomembranes

Atomically well-defined interfaces are essential for realizing functional interlayer coupling in stacked and twisted oxide heterostructures, yet transferred freestanding oxides can develop structural inhomogeneities, including local curvatures, interfacial voids, and incomplete contacts with substrates. Here, we demonstrate that these transfer-induced structural disorders and imperfections evolve substantially and can be suppressed by post-transfer thermal treatments, yielding bulk-like crystalline freestanding oxide nanomembranes. Using freestanding SrTiO3 membranes as a model system, we report a systematic understanding of the role of "atomic ironing" and the associated evolution of lattice mosaicity, interfacial roughness, and optical bandgap. We further demonstrate atomically bonded conformal interfaces in twisted SrTiO3 heterostructures, highlighting the importance of post-transfer thermal processes. These results establish a synthetic strategy to restore the structural integrity and intrinsic bulk-like functionality of freestanding oxide nanomembranes, enabling stacked, twisted, and heterogeneously integrated oxide architectures with atomically well-defined interfaces for emerging quantum functionalities.