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Nanoscale investigations by scanning probe microscopy have provided majorcontributions to the rapid development of organic-inorganic halide perovskites(OIHP) as optoelectronic devices. Further improvement of device levelproperties requires a deeper understanding of the performance-limitingmechanisms such as ion migration, phase segregation and their effects on chargeextraction both at the nano- and macroscale. Here, we have studied the dynamicelectrical response of Cs0.05(FA0.83-MA0.17)0.95PbI3-xBrx perovskite structuresby employing conventional and microsecond time-resolved Kelvin probe forcemicroscopy (KPFM). Our results indicate strong negative charge carrier trappingupon illumination and very slow (>1s) relaxation of charges at the grainboundaries. The fast electronic recombination and transport dynamics on themicrosecond scale probed by time-resolved KPFM show diffusion of chargecarriers towards grain boundaries and indicate locally higher recombinationrates due to intrinsic spatial heterogeneity. The nanoscale electrostaticeffects revealed are summarized in a collective model for mixed-halide CsFAMA.Results on multilayer solar cell structures draw direct relations betweennanoscale ionic transport, electron accumulation, recombination properties andthe final device performance. Our findings extend the current understanding ofcomplex charge carrier dynamics in stable multi-cation OIHP structures.

Nanoscale charge accumulation and its effect on carrier dynamics in tri-cation perovskite structures