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In this work, a \u201cpolycrystal\u2010induced aggregation\u201d strategy orders the polymer donor (PM6) and non\u2010fullerene acceptor (L8\u2010BO) molecules during solution casting with the assistance of PM6 polycrystals that are incubated through a vapor diffusion method, toward improved solar cell efficiency with either thin or thick photoactive layers. These PM6 polycrystals are redissolved in chloroform to prepare PM6 pre\u2010aggregates (PM6\u2010PA), and further incorporated into the conventional PM6:L8\u2010BO blend solutions, which is found to prolong the molecular organization process and enhance the aggregation of both the PM6 and the L8\u2010BO components. As the results, with the assistance of 10% PM6\u2010PA, PM6:L8\u2010BO solar cell devices obtain power conversion efficiencies (PCEs) from 18.0% and 16.2% to 19.3% and 17.2% with a 100 nm\u2010thick and 300\u00a0nm\u2010thick photoactive layer, respectively.<\/jats:p>","DOI":"10.1002\/adma.202304921","type":"journal-article","created":{"date-parts":[[2023,7,19]],"date-time":"2023-07-19T20:44:15Z","timestamp":1689799455000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":84,"title":["A Polycrystalline Polymer Donor as Pre\u2010Aggregate toward Ordered Molecular Aggregation for 19.3% Efficiency Binary Organic Solar Cells"],"prefix":"10.1002","volume":"35","author":[{"given":"Chuanhang","family":"Guo","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yiwei","family":"Fu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Donghui","family":"Li","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liang","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bojun","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chen","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuandong","family":"Sun","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zirui","family":"Gan","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dan","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Li","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5887-534X","authenticated-orcid":false,"given":"Tao","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Wuhan University of Technology  Wuhan 430070 China"},{"name":"School of Materials and Microelectronics Wuhan University of Technology  Wuhan 430070 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,8,31]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202102694"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.matre.2021.100062"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/S1369-7021(12)70019-6"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/b823001c"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/nn200933r"},{"key":"e_1_2_7_6_1","first-page":"437","volume":"50","author":"Yi C.","year":"2020","journal-title":"Sci. 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