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Phase segregation is a critical phenomenon that influences the stability andperformance of mixed halide perovskite based opto-electronic devices. Inaddition to the underlying physical mechanisms, the spatial pattern andrandomness associated with the nanoscale morphology of phase segregationsignificantly influence performance degradation a topic which, along with themultitude of parameter combinations, has remained too complex to address sofar. Given this, with MAPbI1.5Br1.5 as a model system, here we address theinfluence of critical factors like the spatial randomness of phase segregation,influence of ion migration, and the effect of increased non radiativerecombination at material interfaces. Interestingly, our analytical model anddetailed statistical simulations indicate a unique trend morphology evolutionwith increased phase segregation results, surprisingly, in a recovery inefficiency while non-radiative recombination at grain/domain boundaries resultsin efficiency degradation. Further, our quantitative and predictive estimatesidentify critical parameters for interface states beyond which devicevariability could be an important system level bottleneck. Indeed, theseestimates are broadly applicable to systems which undergo phase segregation andhave interesting implications to perovskite based optoelectronic devices fromstability concerns to engineering approaches that attempt to arrest phasesegregation.

Is more Phase Segregation better for mixed halide perovskite devices: Spatial randomness, Ion migration, and Non-radiative recombination