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However, the intensity of interaction affects more precise control of crystallization speed. Herein, we introduce two pyridinium cation species to compare the intensity of their interaction with iodide. Our systematic investigation reveals that the more electron deficient 1\u2010methyl\u20104\u2010(trifluoromethyl)pyridinium (CF\n                    <jats:sub>3<\/jats:sub>\n                    Py\n                    <jats:sup>+<\/jats:sup>\n                    )\u2010based hybrid SAM enables a champion power conversion efficiency (PCE) of 27.07% (certified 26.8%) for a 0.06\u2010cm\n                    <jats:sup>2<\/jats:sup>\n                    PSC, surpassing hybrid 1\u2010methylpyridinium (Py\n                    <jats:sup>+<\/jats:sup>\n                    )\u2010based device (26.42%) and pure 4PADCB\u2010based device (25.12%). The impressive PCE stems from fine\u2010tuning of crystallization speed through more intensive interaction between CF\n                    <jats:sub>3<\/jats:sub>\n                    Py\n                    <jats:sup>+<\/jats:sup>\n                    and I\n                    <jats:sup>\u2212<\/jats:sup>\n                    . Moreover, the stronger interaction inhibits iodide migration, which improves the light and thermal stability of the optimized PSCs. Our work demonstrates an effective approach to strengthening the interaction between pyridinium cations and iodide by incorporating an electron\u2010withdrawing group into the aromatic core, providing crucial insights into the manipulation of perovskite film crystallization.\n                  <\/jats:p>","DOI":"10.1002\/anie.1360189","type":"journal-article","created":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T13:13:16Z","timestamp":1788441196000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Crystallization Manipulation Through Buried Pyridinium\u2010Induced Tunable Interactions in Perovskite Solar Cells"],"prefix":"10.1002","volume":"65","author":[{"given":"Xingzheng","family":"Yan","sequence":"first","affiliation":[{"name":"Zhejiang Provincial Engineering Research Center of Energy Optoelectronic Materials and Devices Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences  Ningbo People's Republic of China"},{"name":"Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Songyu","family":"Du","sequence":"additional","affiliation":[{"name":"Zhejiang Provincial Engineering Research Center of Energy Optoelectronic Materials and Devices Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences  Ningbo People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyu","family":"Tong","sequence":"additional","affiliation":[{"name":"Zhejiang Provincial Engineering Research Center of Energy Optoelectronic Materials and Devices Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences  Ningbo People's Republic of 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Chinese Academy of Sciences  Ningbo People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuan","family":"Luan","sequence":"additional","affiliation":[{"name":"Zhejiang Provincial Engineering Research Center of Energy Optoelectronic Materials and Devices Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences  Ningbo People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2019-4298","authenticated-orcid":false,"given":"Mengjin","family":"Yang","sequence":"additional","affiliation":[{"name":"Zhejiang Provincial Engineering Research Center of Energy Optoelectronic Materials and Devices Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences  Ningbo People's Republic of 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