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Flash Formation of I-Rich Clusters during Multistage Halide Segregation Studied in MAPbI1.5Br1.5

Wide bandgap mixed halide perovskites such as MAPb(I1-xBrx)3 sparked great research interest due to their outstanding optoelectronic properties, ease of fabrication and bandgap tunability. Their application thus far is however limited by light-induced halide segregation in which microscopic clusters with high iodide content are formed and act as recombination centers. The key mechanism(s) underlying this halide segregation process are still debated. Here we present a study on the photoluminescence evolution in MAPb(I1.5Br1.5) perovskites with varying microstructure under constant illumination at room temperature and at elevated temperature. Our findings reveal a more complicated picture of the segregation mechanism occurring in three stages instead of two as commonly reported. The process starts with a flash formation of I-rich nanodomains. Following is a rapid blue shift before the gradual and typically observed red shift occurs. The evolution of the three stages is fully reversible in the dark and is also present at elevated temperatures (50 °C). We explain the existence of multiple stages during light-induced halide segregation by natural compositional fluctuations of the halides and the formation of halide clusters with a dynamically changing distribution in I-Br content. The variation in I-Br ratio depends on the grain size and film heterogeneity. These findings add further details in the quest of