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The fabrication of high‐quality perovskite film highly relies on chemical composition and the synthesis method of perovskite. So far, sequentially deposited MA0.03FA0.97Pb(I0.97Br0.03)3 polycrystalline film is adopted to produce high‐performance perovskite solar cells with record power conversion efficiency (PCE). Fewer grain boundaries and incorporation of inorganic cation (e.g., cesium) would further increase device performance via sequential deposition. Here, cesium chloride (CsCl) is introduced into lead iodide (PbI2) precursor solution that beneficially modulates the property of PbI2 film, leading to larger grains with cesium incorporation in the resulting perovskite film. The enlarged crystal grains originate from a slower nucleation process for CsCl‐containing PbI2 film when reacting with formamidine iodide, confirmed by in situ confocal photoluminescence imaging. Photovoltaic devices based on CsCl‐containing PbI2 film demonstrate a higher averaging efficiency of 21.3% than 20.3% of the devices without CsCl additives for reverse scan. More importantly, the device stability is improved by CsCl additives that retain over 90% of their initial PCE value after 4000 min tracking at maximum power point under 1‐sun illumination. This work paves a way to further improve the photovoltaic performance of mixed‐cation‐halide perovskite solar cells via a sequential deposition method.
Highly efficient mixed‐cation perovskite solar cells are achieved by a cesium chloride (CsCl)‐enhanced PbI2 precursor sequential deposition method. Cs is effectively incorporated into the perovskite film. The Cs‐incorporated film has larger grains and the resulting champion device shows a power conversion efficiency of 22.1% from reverse scan. Device stability is significantly improved by introducing Cs, demonstrating a 4000 min stability.