Interfacial Oxygen Octahedral Coupling-Driven Robust Ferroelectricity in Epitaxial Na_0.5Bi_0.5TiO₃ Thin Films

The oxygen octahedral rotation (OOR) forms fundamental atomic distortions and symmetries in perovskite oxides and definitely determines their properties and functionalities. Therefore, epitaxial strain and interfacial structural coupling engineering have been developed to modulate the OOR patterns and explore novel properties, but it is difficult to distinguish the 2 mechanisms. Here, different symmetries are induced in Na_0.5Bi_0.5TiO₃ (NBT) epitaxial films by interfacial oxygen octahedral coupling rather than epitaxial strain. The NBT film grown on the Nb:SrTiO₃ substrate exhibits a paraelectric tetragonal phase, while with La_0.5Sr_0.5MnO₃ as a buffer layer, a monoclinic phase and robust ferroelectricity are obtained, with a remanent polarization of 42 μC cm^-2 and a breakdown strength of 7.89 MV cm^-1, which are the highest record among NBT-based films. Moreover, the interfacial oxygen octahedral coupling effect is demonstrated to propagate to the entire thickness of the film, suggesting an intriguing long-range effect. This work provides a deep insight into understanding the structure modulation in perovskite heterostructures and an important avenue for achieving unique functionalities.