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However, WBG PSCs often suffer from severe light\u2010induced phase segregation and significant non\u2010radiative recombination losses due to uncontrolled rapid crystallization. Here, polyfluoride molecular additives are designed and incorporated via (diacetoxyiodo)benzene into WBG perovskite, to regulate crystallization process of perovskite films and thereby reduce defects. (Bis(trifluoroacetoxy)iodo)benzene (BTFIB) can passivate uncoordinated lead ions and iodide vacancies, thereby inhibiting phase separation caused by iodide migration and reducing non\u2010radiative recombination loss during charge transport. Moreover, the introduction of BTFIB can effectively moderate the film formation process and confer excellent hydrophobic properties to the films. Consequently, BTFIB\u2010based 1.67 eV\u2010WBG perovskite devices yield a champion efficiency of 23.05% (certified efficiency of 22.21%), enabling a 31.20% efficiency in four\u2010terminal PSTSCs, along with excellent open\u2010circuit voltage of 1.246\u00a0V and fill factor of 85.34%. After 2500\u00a0h of aging in a glovebox, the device retained 80% of its initial efficiency.\n                  <\/jats:p>","DOI":"10.1002\/adma.202503269","type":"journal-article","created":{"date-parts":[[2025,4,8]],"date-time":"2025-04-08T07:11:16Z","timestamp":1744096276000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":51,"title":["Customized Multifunctional Additive Regulates 1.67 eV\u2010Wide\u2010Bandgap Perovskite Crystallization for Four\u2010Terminal Perovskite\/Silicon Tandem Solar Cells"],"prefix":"10.1002","volume":"37","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-2404-2207","authenticated-orcid":false,"given":"Shenghan","family":"Wu","sequence":"first","affiliation":[{"name":"College of Materials Science and Engineering &amp; Institute of New Energy and Low\u2010Carbon Technology &amp; Engineering Research Center of Alternative Energy Materials &amp; Devices Ministry of Education Sichuan University  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