Freestanding Ferroelectric Bubble Domains

Abstract Bubble‐like domains, typically a precursor to the electrical skyrmions, arise in ultrathin complex oxide ferroelectric–dielectric–ferroelectric heterostructures epitaxially clamped with flat substrates. Here, it is reported that these specially ordered electric dipoles can also be retained in a freestanding state despite the presence of inhomogeneously distributed structural ripples. By probing local piezo and capacitive responses and using atomistic simulations, this study analyzes these ripples, sheds light on how the bubbles are stabilized in the modified electromechanical energy landscape, and discusses the difference in morphology between bubbles in freestanding and as‐grown states. These results are anticipated to be the starting point of a new paradigm for the exploration of electric skyrmions with arbitrary boundaries and physically flexible topological orders in ferroelectric curvilinear space.