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Given the distinct features of donor and acceptor materials, designing solid additives to selectively control the aggregation behaviors of them represents a key strategy for further development of OSCs. Herein, a series of bithiophene isomers solid additives (2,2\u2010TT, 2,3\u2010TT, and 3,3\u2010TT) are designed for film morphology regulation. Systematic analysis reveals that the addition of 2,2\u2010TT significantly enhances the \u03c0\u2013\u03c0 stacking of L8\u2010BO, yet exerts a relatively limited effect on PM6 aggregation. Conversely, the incorporation of 3,3\u2010TT not only facilitates the formation of compact and highly ordered molecular packing of L8\u2010BO but also substantially promote the denser \u03c0\u2013\u03c0 stacking of PM6. Consequently, the PM6:L8\u2010BO\u2010based OSCs with 3,3\u2010TT treatment achieve a higher efficiency of 19.34%, benefitting from the balanced charge mobility and longer carrier lifetime. More impressively, the D18:L8\u2010BO\u2010based devices treated with 3,3\u2010TT deliver a remarkable efficiency of 20.32%, with an excellent fill factor of 82.47%, which ranks among the best values reported so far. This work highlights the critical role of the solid additive isomerization strategy in selectively regulating the aggregation characteristics of donor and acceptor materials, thereby facilitating the further advancement of OSCs field.<\/jats:p>","DOI":"10.1002\/anie.202514004","type":"journal-article","created":{"date-parts":[[2025,9,1]],"date-time":"2025-09-01T12:44:21Z","timestamp":1756730661000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":24,"title":["Selectively Modulating the Donor and Acceptor Aggregation Behaviors Through Solid Additive Isomerization Engineering for Organic Solar Cells Exceeding 20% Efficiency"],"prefix":"10.1002","volume":"64","author":[{"given":"Keli","family":"Shi","sequence":"first","affiliation":[{"name":"Key Laboratory of Solid State Optoelectronic Devices of Zhejiang Province College of Physics and Electronic Information Engineering Zhejiang Normal University  Jinhua Zhejiang 321004 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