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The presence of unreacted lead iodide in organic-inorganic lead halideperovskite solar cells is widely correlated with an increase in powerconversion efficiency. We investigate the mechanism for this increase byidentifying the role of surfaces and interfaces present between methylammoniumlead iodide perovskite films and excess lead iodide. We show how type I and IIband alignments arising under different conditions result in either passivationof surface defects or hole injection. Through first-principles simulations ofsolid-solid interfaces, we find that lead iodide captures holes frommethylammonium lead iodide and modulates the formation of defects in theperovskite, affecting recombination. Using surface-sensitive opticalspectroscopy techniques, such as transient reflectance and time-resolvedphotoluminescence, we show how excess lead iodide affects the diffusion andsurface recombination velocity of charge carriers in methylammonium lead iodidefilms. Our coupled experimental and theoretical results elucidate the role ofexcess lead iodide in perovskite solar cells.

Understanding the Effect of Lead Iodide Excess on the Performance of Methylammonium Lead Iodide Perovskite Solar Cells