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The observation of low energy edge photoluminescence and its beneficialeffect on the solar cell efficiency of Ruddlesden-Popper perovskites hasunleashed an intensive research effort to reveal its origin. This effort,however, has been met with more challenges as the underlying material structurehas still not been identified; new modellings and observations also do not seemto converge. Using 2D (BA)2(MA)2Pb3Br10 as an example, we show that 3D MAPbBr3is formed due to the loss of BA on the edge. This self-formed MAPbBr3 canexplain the reported edge emission under various conditions, while the reportedintriguing optoelectronic properties such as fast exciton trapping from theinterior 2D perovskite, rapid exciton dissociation and long carrier lifetimecan be understood via the self-formed 2D/3D lateral perovskite heterostructure.The 3D perovskite is identified by submicron infrared spectroscopy, theemergence of XRD signature from freezer-milled nanometer-sized 2D perovskiteand its photoluminescence response to external hydrostatic pressure. Therevelation of this edge emission mystery and the identification of aself-formed 2D/3D heterostructure provide a new approach to engineering 2Dperovskites for high-performance optoelectronic devices.

chemistry of materials

Self-formed 2D/3D Heterostructure on the Edge of 2D Ruddlesden-Popper  Hybrid Perovskites Responsible for Intriguing Optoelectronic Properties and  Higher Cell Efficiency