Homogenized halides and alkali cation segregation in alloyed organic-inorganic perovskites
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Science 363 (6427): 627--631 (2019)

For organic-inorganic hybrid solar cells, addition of cesium or rubidium cations can improve power conversion efficiency. Correa-Baena et al. used nanoscale x-ray fluorescence imaging to show that the addition of metal cations at low concentrations homogenized the distribution of bromide and iodide anions and also increased charge-carrier lifetimes. However, at high concentrations, aggregation and cluster formation led to increased charge recombination.Science, this issue p. 627The role of the alkali metal cations in halide perovskite solar cells is not well understood. Using synchrotron-based nano–x-ray fluorescence and complementary measurements, we found that the halide distribution becomes homogenized upon addition of cesium~iodide, either alone or with rubidium~iodide, for substoichiometric, stoichiometric, and overstoichiometric preparations, where the lead halide is varied with respect to organic halide precursors. Halide homogenization coincides with long-lived charge carrier decays, spatially homogeneous carrier dynamics (as visualized by ultrafast microscopy), and improved photovoltaic device performance. We found that rubidium and potassium phase-segregate in highly concentrated clusters. Alkali metals are beneficial at low concentrations, where they homogenize the halide distribution, but at higher concentrations, they form recombination-active second-phase clusters.
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