Two-Dimensional Layered Oxide Structures Tailored by Self-Assembled Layer Stacking via Interfacial Strain.

Study of layered complex oxides emerge as one of leading topics in fundamental materials science because of the strong interplay among intrinsic charge, spin, orbital, and lattice. As a fundamental basis of heteroepitaxial thin film growth, interfacial strain can be used to design materials that exhibit new phenomena beyond their conventional forms. Here, we report a strain-driven self-assembly of bismuth-based supercell (SC) with a two-dimensional (2D) layered structure. With combined experimental analysis and first-principles calculations, we investigated the full SC structure and elucidated the fundamental growth mechanism achieved by the strain-enabled self-assembled atomic layer stacking. The unique SC structure exhibits room-temperature ferroelectricity, enhanced magnetic responses, and a distinct optical bandgap from the conventional double perovskite structure. This study reveals the important role of interfacial strain modulation and atomic rearrangement in self-assembling a layered singe-phase multiferroic thin film, which opens up a promising avenue in the search for and design of novel 2D layered complex oxides with enormous promise.