Ferroelectrics have become indispensable in the development of energy-efficient oxide electronics.Their domain state is closely linked to the final device functionality,making domain engineering in technology-compatible thin films of paramount importance.Here we demonstrate the local control of domain formation in two-dimensional epitaxial ferroelectric films using structural defect engineering through the substrate topography.Using a combination of first-principles calculations,atom probe tomography,and scanning probe microscopy,we show that out-of-phase boundaries induced at the substrate step edges combined with local off-stoichiometry trigger the formation of ferroelectric domain walls in the layered ferroelectric Bi5FeTi3O_(15)Aurivillius thin films.The substrate treatment and the miscut angle selection allow for precise control of domain size and location in both single layers and multilayer architectures.With this work,we establish a new route for ferroelectric domain engineering and stabilization of functional domain walls in ultrathin ferroelectric layers.
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