Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.382
Publication date: 16th December 2024
Lead-based mixed-halide perovskites have a number of uses in solar and in light emitting applications. Unfortuantely, they exhibit ionic instabilities under illumination. Chief among them is photosegregation, a phenomenon first reported by McGehee in 2015. Since then, photosegregation has beceome well established as the light-driven segregation of iodine and bromine anions in mixed-halide lattices into iodine-rich and bromine-rich inclusions of the alloy. The phenomenon is reversible under darkness and segregated anions can remix.
Multiple models have been developed to explain photosegregation. Among them are thermodynamic, polaron, chemical, and trap-related models. While models explain photosegregation to varying extents only a band gap thermodynamic model has explained in a quantitative manner, observations of excitation intensity (Iexc)-dependent terminal halide stoichiometries and photoegregation Iexc thresholds.
One observation that has not been explained by any model though is the recent observation by Bach and co-workers of light-driven anion remixing in methylammonium lead iodide/bromide microcrystals. Hindering a deeper understanding of this photoresponse has been the fact that the Bach report is the only report of persistent photoremixing in a mixed-halide perovskite.
We have recently found that pulsed laser irradiation of photosegregated mixed-halide perovskite films can induce robust and reproducible, persistent photoremixing. This opens the door to furthering our understanding of mixed-halide photoinstabilities since it allows for the first time, concerted studies of photosegregation and photoremixing on the same system. More importantly, it provides an important test for any model seeking to self-consistently rationalize mixed-halide perovskite photoinstabilities.
M.K. thanks the Division of Materials Sciences and Engineering, Office of Basic Energy Sciences, U.S. Department of Energy (DOE) under Award DE-SC0014334 for financial support of this work.
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