Ruddlesden–Popper Phase in Two-Dimensional Inorganic Halide Perovskites: A Plausible Model and the Supporting Observations

A Ruddlesden–Popper (RP) type structure is well-known in oxide perovskites and is related to many interesting properties such as superconductivity and ferroelectricity. However, the RP phase has not yet been discovered in inorganic halide perovskites. Here, we report the direct observation of unusual structure in two-dimensional CsPbBr3 nanosheets which could be interpreted as the RP phase based on model simulations. Structural details of the plausible RP domains and domain boundaries between the RP and conventional perovskite phases have been revealed on the atomic level using aberration-corrected scanning transmission electron microscopy. The finding marks a major advance toward future inorganic halide RP phase synthesis and theoretical modeling, as well as unraveling their structure–property relationship.