Deterministic Synthesis of a Two-Dimensional MAPbI3 Nanosheet and Twisted Structure with Moiré Superlattice

The synthesis of extremely thin 2D halide perovskites and the exploration of their interlayer interactions have garnered significant attention in current research. A recent advancement we have made involves the development of a successful technique for generating ultrathin MAPbI 3 nanosheets with controlled thickness and an exposed intrinsic surface. This innovative method relies on utilizing the Ruddlesden–Popper (RP) phase perovskite (BA 2 MA n –1 Pb n I 3 n +1 ) as a template. However, the precise reaction mechanism remains incompletely understood. In this work, we systematically examined the dynamic evolution of the phase conversion process, with a specific focus on the influence of inorganic slab (composed of [PbI 6 ] 4– octahedrons) numbers on regulating the thickness and quality of the resulting MAPbI 3 nanosheets. Additionally, the atomic structure is directly visualized using the transmission electron microscopy (TEM) method, confirming its exceptional quality. To illustrate interfacial interactions in ultrathin structures, artificial moiré superlattices are constructed through a physical transfer approach, revealing multiple localized high-symmetry stacks within a distinctive square moiré pattern. These findings establish a novel framework for investigating the physics of interfacial interactions in ionic semiconducting crystals.