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Suppressing non‐radiative recombination via passivating surface defects of perovskite films has demonstrated an excellent strategy for high‐performance perovskite solar cells (PSCs). However, it is still hard to realize both high open‐circuit voltage (Voc) of >1.2 V and high power conversion efficiency (PCE) of >22%, because the optimized bandgap of perovskite films is less than 1.60 eV for efficient light harvesting and Voc deficit is generally unavoidable due to carriers recombination. Here, the surface of the perovskite film is treated with a series of phenylhydroxylammonium halide salts and it is found that all of them can remarkably prolong the carrier lifetime owing to their excellent capability of surface defects passivation. The best PSC with phenylbutylammonium bromide treatment realizes a PCE of 22.67% with a Voc of 1.216 V, corresponding to a small Voc deficit of ≈344 mV. [ABSTRACT FROM AUTHOR]

Adding a small amount of CsI into mixed cation‐halide perovskite film via a one‐step method has been demonstrated as an excellent strategy for high‐performance perovskite solar cells (PSCs). However, the one‐step method generally relies on an antisolvent washing process, which is hard to control and not suitable for fabricating large‐area devices. Here, CsF is employed and Cs is incorporated into perovskite film via a two‐step method. It is revealed that CsF can effectively diffuse into the PbI2 seed film, and drastically enhances perovskite crystallization, leading to high‐quality Cs‐doped perovskite film with a very long photoluminescence carrier lifetime (1413 ns), remarkable light stability, thermal stability, and humidity stability. The fabricated PSCs show power conversion efficiency (PCE) of over 21%, and they are highly thermally stable: in the aging test at 60 °C for 300 h, 96% of the original PCE remains. The CsF incorporation process provides a new avenue for stable high‐performance PSCs. [ABSTRACT FROM AUTHOR]