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A key challenge is how to design acceptor materials that attain high PLQY while preserving favorable crystallinity and aggregation behavior, as these properties are often mutually conflicting. Here, we address this challenge by developing a series of dimeric acceptors linked via benzene, naphthalene, and anthracene bridges (named Ph\u2010dimer, Naph\u2010dimer, and Ant\u2010dimer). Although the conjugation length and intrinsic emission of these cores increase from benzene to anthracene, the photovoltaic performance of the resulting dimeric acceptors shows no linear correlation with this trend. Among them, the Naph\u2010dimer optimally balances crystallinity and PLQY, with enhanced molecular packing and reduced disorder, suppressing energy loss (\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>loss<\/jats:sub>\n                    ) and facilitating charge extraction. Consequently, the PM6:Naph\u2010dimer OSC exhibits a power conversion efficiency (PCE) of 18.90%, an open\u2010circuit voltage (\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>oc<\/jats:sub>\n                    ) of 0.974\u00a0V and a low \u0394\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>3<\/jats:sub>\n                    of 0.192\u00a0eV, outperforming PM6:Ph\u2010dimer and PM6:Ant\u2010dimer counterparts. Moreover, incorporating Naph\u2010dimer into a PM6:L8\u2010BO host yields a PCE of 21.02%. These findings indicate that precise bridge modulation is an effective strategy for harmonizing high PLQY with crystalline order in OSCs.\n                  <\/jats:p>","DOI":"10.1002\/anie.4058890","type":"journal-article","created":{"date-parts":[[2026,10,6]],"date-time":"2026-10-06T05:24:22Z","timestamp":1791264262000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Using Aromatic\u2010Bridge\u2010Tuned Dimer Acceptors to Harmonize Photoluminescence Quantum Yield and Crystallinity for Organic Solar Cells Exceeding 21% Efficiency"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-0568-6382","authenticated-orcid":false,"given":"Yue","family":"Chen","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science International Research Center For Carbon Neutralization Hangzhou International Innovation Institute Beihang University Hangzhou P. R. 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