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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]

The nucleation and crystallization processes within solution‐processed deposition is key for obtaining perovskite films with high quality. Herein, the synergistic effect of Cs+, ligand solvent (tetramethylene sulfoxide, TMSO), and methylammonium ions (MA+) on nucleation and crystallization procedures of preparing perovskites films is studied. The results reveal that producing α‐phase nuclei in the intermediate‐phase film (a perovskite film formed by removing the solvent before annealing) is the key factor for obtaining α‐phase‐pure perovskites, wherein Cs+ is necessary for reducing the formation energy of the α‐phase. In addition, the nonvolatile ligand (TMSO) is used to inhibit rapid nucleation, because it can form a stable intermediate phase. Furthermore, the introduction of the volatile MA+ cations compound (MACl) combined with Cs+ contributed to the direct formation of α‐phase nuclei in the intermediate‐phase film, and ion exchange (between FA+ and MA+) occurs during the subsequent annealing process, which leads to the formation of large‐grain perovskite film with good crystallinity. Maximum power conversion efficiencies of 22.08% and 16.88% are obtained via this strategy for a perovskite solar cell on a small area (active area: 0.09 cm2) and a perovskite solar module (aperture area: 12.92 cm2), respectively. [ABSTRACT FROM AUTHOR]