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• A simple solvent engineering strategy was employed to control morphology of PbI 2 films effectively by water processing. • Platelet-like PbI 2 films can successfully control the residual amount of PbI 2 in perovskite film. • Platelet-like PbI 2 films can control the morphology of the perovskite film and improve the device efficiency [Display omitted] The performance of organic-inorganic perovskite solar cells depends largely on the quality of perovskite film. Currently, various methods are applied to prepare the perovskite film. Among them, the two-step method is counted as a promising candidate to obtain high-quality perovskite film. In this study, we attain a special platelet-like PbI 2 films by applying pure water to cover wet PbI 2 film and standing for a period of time. The unique morphology contributes to the entry of organic cations solution into the PbI 2 and promoting its reaction with PbI 2 , which reducing the residual amount of PbI 2 in the perovskite film. Compared to the traditional two-step method, water processing method can obtain a high-quality perovskite film with enlarged grain size, improved crystallization, and prolonged carrier lifetime. As a result, the efficiency of the prepared device based on the film has increased from 17.90% without water processing to 20.14% of water processing. Which demonstrates that this solvent engineering for PbI 2 film opens up a possibility to prepare high-quality perovskite in a two-step method and obtain highly efficient perovskite solar cells. [ABSTRACT FROM AUTHOR]

Gas-quenching fabrication of perovskite films demonstrates promising compatibility for commercialization of perovskite photovoltaics. Seeking suitable ligand for the perovskite precursor inks to improve the crystalline quality of gas-quenched methylammonium free perovskite films is critical for realizing up-scalable fabrication of stable perovskite solar cells. In this work, a series of pyrrolidone-based ligands are employed in gas-quenching fabrication of FA 0.9 Cs 0.1 PbI 3 perovskite films. Optical and morphological characterizations indicate 2-pyrrolidone is the most preferred ligand to deliver a neat buried-interface as well as a light-trapping surface at the rear of the device, which maximized the light-harvesting and the photocurrent of the device. The corresponding device achieved a power conversion efficiency of 21.6% without any interfacial passivation, as well as reduced defect density from their electrical characteristics. Moreover, a more stable performance of the device is obtained with 2-pyrrolidone compared to other pyrrolidone-based ligands, demonstrating 2-pyrrolidone as a promising ligand in designing the perovskite inks for methylammonium-free perovskite solar cells. • Various pyrrolidone-based ligands are studied in gas-quenching of FA 0.9 Cs 0.1 PbI 3 films. • Bifacial optical properties of perovskite films are optimized with NP ligand. • smoother buried interface and a rougher surface contribute to enhanced light harvesting. • NP device achieved 21.6% efficiency without any interfacial passivation [ABSTRACT FROM AUTHOR]

[Display omitted] • A novel heterogeneous lead iodide, exhibiting two (0 0 1) interplanar distances of 6.9 Å and 9.0 Å, was constructed. • The heterogeneous structure can regulate the crystallization process of PbI 2 and perovskite films. • The V OC and PCE were raised to 1.21 V and 24.24%. At present, the highest power conversion efficiency (PCE) of perovskite solar cells (PSCs) has exceeded 25%, which exhibits great potential for commercial applications. Obtaining pinhole-free, superior crystal, and high-quality perovskite films with fewer defects by adjusting the lead iodide (PbI 2) intermediate films in a two-step sequential deposition has become research arousing general interest. Herein, a heterogeneous lead iodide (HLI) structure with two (0 0 1) interplanar distances (9.0 Å and 6.9 Å), can optimize the crystallization process of perovskite to get better surface morphology and is constructed by intercalated choline chloride (a kind of vitamin B4, VB4). HLI simultaneously improves the carrier lifetime of perovskite film from 1.96 µs to 3.28 µs and reduces defect state density. Together with better morphology and lower defect state density, the open circuit voltage (V OC) and PCE based on (FAPbI 3) 0.97 (MAPbBr 3) 0.03 is significantly boosted. In addition, with double-sided modification, HLI produces an excellent PCE of 24.27% with a V OC of 1.21 V. We believe that the novel heterogeneous PbI 2 structure could be a generic method to improve the efficiency of PSCs. [ABSTRACT FROM AUTHOR]