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In ferroelectric heterostructures, the interaction between intrinsic polarization and the electric field generates a rich set of localized electrical properties. The local electric field is determined by several connected factors, including the charge distribution of individual unit cells, the interfacial electromechanical boundary conditions, and chemical composition of the interfaces. However, especially in ferroelectric perovskites, a complete description of the local electric field across micro-, nano-, and atomic-length scales is missing. Here, by applying four-dimensional scanning transmission electron microscopy (4D STEM) with multiple probe sizes matching the size of structural features, we directly image the electric field of polarization vortices in (PbTiO3)16/(SrTiO3)16 superlattices and reveal different electric field configurations corresponding to the atomic scale electronic ordering and the nanoscale boundary conditions. The separability of two different fields probed by 4D STEM offers the possibility to reveal how each contributes to the electronic properties of the film.

The potential for creating hierarchical domain structures, or mixtures of energetically degenerate phases with distinct patterns that can be modified continually, in ferroelectric thin films offers a pathway to control their mesoscale structure beyond lattice‐mismatch strain with a substrate. Here, it is demonstrated that varying the strontium content provides deterministic strain‐driven control of hierarchical domain structures in Pb_1−xSr_xTiO₃ solid‐solution thin films wherein two types,c/aanda₁/a₂, of nanodomains can coexist. Combining phase‐field simulations, epitaxial thin‐film growth, detailed structural, domain, and physical‐property characterization, it is observed that the system undergoes a gradual transformation (with increasing strontium content) from droplet‐likea₁/a₂ domains in ac/adomain matrix, to a connected‐labyrinth geometry ofc/adomains, to a disconnected labyrinth structure of the same, and, finally, to droplet‐likec/adomains in ana₁/a₂ domain matrix. A relationship between the different mixed‐phase modulation patterns and its topological nature is established. Annealing the connected‐labyrinth structure leads to domain coarsening forming distinctive regions of parallelc/aanda₁/a₂ domain stripes, offering additional design flexibility. Finally, it is found that the connected‐labyrinth domain patterns exhibit the highest dielectric permittivity.

Ferroelectric materials owning a polymorphic nanodomain structure usually exhibit colossal susceptibilities to external mechanical, electrical, and thermal stimuli, thus holding huge potential for relevant applications. Despite the success of traditional strategies by means of complex composition design, alternative simple methods such as strain engineering have been intensively sought to achieve a polymorphic nanodomain state in lead‐free, simple‐composition ferroelectric oxides in recent years. Here, a nanodomain configuration with morphed structural phases is realized in an epitaxial BaTiO₃film grown on a (111)‐oriented SrTiO₃substrate. Using a combination of experimental and theoretical approaches, it is revealed that a threefold rotational symmetry element enforced by the epitaxial constraint along the [111] direction of BaTiO₃introduces considerable instability among intrinsic tetragonal, orthorhombic, and rhombohedral phases. Such phase degeneracy induces ultrafine ferroelectric nanodomains (1–10 nm) with low‐angle domain walls, which exhibit significantly enhanced dielectric and piezoelectric responses compared to the (001)‐oriented BaTiO₃film with uniaxial ferroelectricity. Therefore, the finding highlights the important role of epitaxial symmetry in domain engineering of oxide ferroelectrics and facilitates the development of dielectric capacitors and piezoelectric devices.