Ferroelectric oxides are used in many modern technologies including sensors, actuators, thin-film memories and energy harvesting. Ferroelectrics of similar composition often show wide variations in their characteristic properties. Such variations in properties can be largely attributed to differences in the structural arrangements of domains and distributions of defects within a multidomain/polycrystalline material. Recent developments in characterization techniques and first-principle calculations have significantly advanced our understanding of how ferroelectric domains interact with material defects, and thereby influence the properties of a material. This review provides a broad outlook of the contributions from different experimental and computational studies that have clarified the structure of domains, domain walls and defects in perovskite ferroelectric oxides, and the evolution of these structures under the application of electric fields. It is intended that an integrated viewpoint of these issues, as provided here, will further motivate synergistic activities between the various research groups and industries towards the development and characterization of ferroelectric oxides.

This paper establishes the nanoscale poling mechanism operating in A-site disordered lead-free piezoelectric ceramics. Nanoscale domain maps and quantitative structural changes were obtained by deploying high-resolution transmission electron microscopy, dielectric spectroscopy, Raman spectroscopy and neutron scattering. Based on these results a microscopic model is proposed that provides insight into the E-field induced structural transformation. The stripe-like nanodomains in the unpoled system transformed into lamellar tetragonal domains with a reduced degree of displacement disorder during poling. It is proposed that the synergic effect of change in octahedral tilt disorder and cation displacement disorder leads to this transformation under an E-field. The criterion for achieving superior functional response includes stabilization of the long range order and reduction in the tilt disorder through compositional adjustments. Understanding of the poling mechanism in lead-free piezoelectric materials has been mostly limited to the behavior of domains under an applied field. However, this work provides an in-depth understanding of the changes in the local structure along with domain morphology under an applied field.

Perovskite piezoelectric compositions near the morphotropic phase boundary (MPB) are known to exhibit high piezoelectric response. In lead-based ABO₃ compound with B-site disorder, the origin of this enhancement has been associated with the presence of an intermediate monoclinic/orthorhombic state that bridges the adjacent ferroelectric rhombohedral and tetragonal phases. However, the origin of high piezoelectric response in lead-free ABO₃ compounds with A-site disorder has not been conclusively established. We describe a microscopic model derived from comparative analyses of high resolution transmission electron microscopy and neutron diffraction that explains the origin of high piezoelectric response in lead-free MPB compositions of 0.93(Na_0.5Bi_0.5)TiO₃–0.07BaTiO₃. Direct observation of nanotwins with monoclinic symmetry confirmed the presence of an intermediate bridging phase that facilitates a pathway for polarization reorientation. Monoclinic distortions of an average rhombohedral phase are attributed to localized displacements of atoms along the non-polar directions.

This letter provides a comparative description of the properties of textured and randomly oriented poly-crystalline lead-free piezoelectric 0.93(Na0.5Bi0.5TiO3)-0.07BaTiO3 (NBT-BT) ceramics. A high longitudinal piezoelectric constant of (d33) ∼ 322 pC/N was obtained in (001)PC textured NBT-7BT ceramics, which is almost ∼2× times the d33 coefficient reported for randomly oriented ceramics of the same composition. In situ neutron diffraction experiments revealed that characteristically different structural responses are induced in textured and randomly oriented NBT-BT ceramics upon application of electric fields (E), which are likely related to the varying coherence lengths of polar nanoregions and internal stresses induced by domain switching.

Electroluminescent (EL) devices have been extensively integrated into multi-functionalized electronic systems in the role of the vitally constituent light-emitting part. However, the lifetime and reliability of EL devices are often severely restricted by concomitant damage, especially when the strain exceeds the mechanical withstanding limit. We report a self-healable EL device by adopting a modified self-healable polyacrylic acid hydrogel as the electrode and a self-healable polyurethane as a phosphor host to realize the first omni-layer-healable light-emitting device. The physicochemical properties of each functionalized layer can be efficiently restored after experiencing substantial catastrophic damage. As a result, the luminescent performance of the self-healable EL devices is well recovered with a high healing efficiency (83.2% for 10 healing cycles at unfixed spots, and 57.7% for 20 healing cycles at a fixed spot). In addition, inter-device healing has also been developed to realize a conceptual “LEGO”-like assembly process at the device level for light-emitting devices. The design and realization of the self-healable EL devices may revive their performance and expand their lifetime even after undergoing a deadly cut. Our self-healable EL devices may serve as model systems for electroluminescent applications of the recently developed ionically conductive healable hydrogels and dielectric polymers.