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Reducing the interfacial defects between the perovskite/electron transport layer (ETL) is the key point to improving the efficient and stable performance of perovskite solar cells (PSCs). In this study, two self-assembled molecules ((aminomethyl)phosphonic acid and glycine) with different functional groups (phosphonic acid (-H2PO3) and carboxylic acid (-COOH)) were mixed to form the buried bottom interface of PSCs. The synergistic effect of -H2PO3 with its higher anchoring ability and -COOH with its fast carrier transport improved the performance of PSCs. Additionally, the SnO2 modified by mixed self-assembly molecules (M-SAM) showed a more appropriate energy level alignment, favoring charge transport and minimizing energy loss. In addition, the amine group (-NH2) on the two small molecules effectively interacted with uncoordinated Pb2+ in perovskite and improved the quality of the perovskite films. Consequently, the (FAPbI3)0.992(MAPbBr3)0.008 PSCs with M-SAM reached a PCE of 24.69% (0.08 cm2) and the perovskite modules achieved a champion efficiency of 18.57% (12.25 cm2 aperture area). Meanwhile, it still maintained more than 91% of its initial PCE after being placed in nitrogen atmosphere at 25 °C for 1500 h, which is better than that of the single-SAM and control devices. Further reference is provided for the future commercialization of perovskite with efficient and stable characteristics. [ABSTRACT FROM AUTHOR]

Ligand‐solvent engineering has been widely applied to improve the quality of perovskite films by forming intermediate films. However, there is an inconsistent understanding in the studies on the composition and mechanism of intermediate films formed by different ligand solvents, and the influence on perovskite film morphology is still elusive. Herein, the pure intermediate films (composed of pure crystal nucleus and amorphous precursor) are fabricated by the addition of ligand solvents with different coordination abilities. Notably, a single heterogeneous nucleation process is induced by the pure intermediate film, resulting in the formation of vertically arranged internal perovskite crystals with few horizontal boundaries, that improve charge transfer and device performance. Furthermore, the small and uniform crystals obtained by adding a ligand solvent with weak coordination ability result in smooth films and a smaller device current (Jsc = 22.74 mA cm−2, PCE = 19.58%). In contrast, the large and uneven crystals obtained by strong coordination ability lead to rough films and a larger device current (Jsc = 23.24 mA cm−2, PCE = 20.72%). This study is devoted to providing a significance reference for the fabrication of perovskite films with vertically arranged internal grains and superior surface textures. [ABSTRACT FROM AUTHOR]