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Layer engineering with different layer numbers inside Aurivillius-type layered structure, similar to interface engineering in heterojunctions or superlattices, can give rise to excellent physical properties due to the correlated layer-stacked interfaces of two different layer phases with different strain states. In this work, using the solid-state reactions from Aurivillius-type Bi3TiNbO9 (2-layer) and Bi4Ti3O12 (3-layer) ferroelectric powder mixtures, single-phase compound of Bi7Ti4NbO21 with an intergrowth structure of 2-layer and 3-layer perovskite slabs sandwiched between the Bi-O layers was synthesized and the effects of this layer-engineered strategy on the structure, Raman-vibration and ferroelectric properties were systematically investigated. The mostly-ordered intergrowth phase was observed clearly by utilizing X-ray diffraction and advanced electron micro-techniques. Uniformly dispersions and collaborative vibrations of Ti and Nb ions in the layer-engineered Bi7Ti4NbO21 were demonstrated. Remarkably, dielectric and ferroelectric properties were also recorded and an enhanced ferroelectric response was found in the layer-engineered mixed-layer sample with high ferroelectric Curie temperature, compared with the homogeneous 2-layer and 3-layer samples. Analyses of the Raman spectra and atomic structures confirmed that the performance improvement of the layer-engineered sample is intrinsic to the correlated layer-stacked interfaces inside the Aurivillius-type layered oxides, arising from strain-induced lattice distortions at the interfaces.

Engineered Layer-Stacked Interfaces Inside Aurivillius-Type Layered Oxides Enables Superior Ferroelectric Property