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However, the underlying principles governing the rational design of volatile solid additives remain elusive. Herein, a series of efficient volatile solid additives are successfully developed by the crossbreeding effect of chalcogenation and iodination for optimizing the morphology and improving the photovoltaic performances of OSCs. Five benzene derivatives of 1,4\u2010dimethoxybenzene (DOB), 1\u2010iodo\u20104\u2010methoxybenzene (OIB), 1\u2010iodo\u20104\u2010methylthiobenzene (SIB), 1,4\u2010dimethylthiobenzene (DSB) and 1,4\u2010diiodobenzene (DIB) are systematically studied, where the widely used DIB is used as the reference. The effect of chalcogenation and iodination on the overall property is comprehensively investigated, which indicates that the versatile functional groups provided various types of noncovalent interactions with the host materials for modulating the morphology. Among them, SIB with the combination of sulphuration and iodination enabled more appropriate interactions with the host blend, giving rise to a highly ordered molecular packing and more favorable morphology. As a result, the binary OSCs based on PM6:L8\u2010BO and PBTz\u2010F:L8\u2010BO as well as the ternary OSCs based on PBTz\u2010F:PM6:L8\u2010BO achieved impressive high PCEs of 18.87%, 18.81% and 19.68%, respectively, which are among the highest values for OSCs.<\/jats:p>","DOI":"10.1002\/advs.202401405","type":"journal-article","created":{"date-parts":[[2024,3,26]],"date-time":"2024-03-26T01:19:36Z","timestamp":1711415976000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Crossbreeding Effect of Chalcogenation and Iodination on Benzene Additives Enables Optimized Morphology and 19.68% Efficiency of Organic Solar Cells"],"prefix":"10.1002","volume":"11","author":[{"given":"Tao","family":"Zhou","sequence":"first","affiliation":[{"name":"School of Chemical Engineering and State Key Laboratory of Polymer Materials Engineering Sichuan University  Chengdu 610065 P. R. 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