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Conventional methods, such as using nonvolatile small molecular additives to slow the reaction, often result in buried interfacial voids and molecule diffusion, compromising the devices\u2019 operational stability. In this study, we introduced a molecular \u201cthruster\u201d\u2014a hypervalent iodine (III) compound with three carbonyl groups and a C\n                    <jats:sup>\u2212<\/jats:sup>\n                    \u2212I\n                    <jats:sup>+<\/jats:sup>\n                    bond\u2014that possesses coordination and dissociation abilities, enabling programed modulation of perovskite\u2010film growth kinetics. Initially, the three carbonyl groups coordinate with PbI\n                    <jats:sub>2<\/jats:sub>\n                    to slow the reaction between FAI and PbI\n                    <jats:sub>2<\/jats:sub>\n                    , preventing \u03b4\u2010phase formation. As temperature rises, the C\n                    <jats:sup>\u2212<\/jats:sup>\n                    \u2212I\n                    <jats:sup>+<\/jats:sup>\n                    bond dissociates, promoting perovskite growth and the dissociated product iodobenzene will promote solvent volatilization, thus avoiding buried interfacial voids. Another product, a carbene compound with eight lone pair electrons sufficiently passivate the undercoordinated Pb\n                    <jats:sup>2+<\/jats:sup>\n                    defects and anchors at grain boundaries without diffusion. Consequently, the resultant FAPbI\n                    <jats:sub>3<\/jats:sub>\n                    film displays high\u2010quality with enhanced phase purity, compact morphology, and reduced defects. Evidently, 0.062\u2010 and 1.004\u2010cm\n                    <jats:sup>2<\/jats:sup>\n                    pero\u2010SCs achieve power conversion efficiencies (PCEs) of up to 26.06\u2009% (25.79\u2009% certified) and 24.65\u2009%, respectively. This approach also controls perovskite\u2010film growth on plastic substrates, resulting in flexible pero\u2010SCs with an impressive PCE of 25.12\u2009%.\n                  <\/jats:p>","DOI":"10.1002\/anie.202419726","type":"journal-article","created":{"date-parts":[[2024,12,17]],"date-time":"2024-12-17T11:08:47Z","timestamp":1734433727000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Program\u2010Modulated Kinetics of Perovskite\u2010Film Growth by Molecular \u201cThruster\u201d for High\u2010Efficiency and Stable Perovskite Solar Cells"],"prefix":"10.1002","volume":"64","author":[{"given":"Chuanshuai","family":"Han","sequence":"first","affiliation":[{"name":"Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou 215123 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Semiconductor-optoelectronics Materials and Devices, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou 215123 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shihao","family":"Huang","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou 215123 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunxiu","family":"Shen","sequence":"additional","affiliation":[{"name":"Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, College of Chemistry, Chemical Engineering and Materials Science Soochow University  Suzhou 215123 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