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Herein, based on two high\u2010boiling solvents, halogenated solvent chlorobenzene (CB) and non\u2010halogenated green solvent ortho\u2010xylene (OX), preparing active layers with the hot solution is put forward to enhance the performance of the OSCs. In situ test and morphological characterization clarify that the hot\u2010casting strategy assists in the fast and synchronous molecular assembly of both donor and acceptor in the active layer, contributing to preferable donor\/acceptor ratio, vertical phase separation, and molecular stacking, which is beneficial to charge generation and extraction. Based on the PM6:BO\u20104Cl, the hot\u2010casting OSCs with a wide processing window achieve efficiencies of 18.03% in CB and 18.12% in OX, which are much higher than the devices processed with room temperature solution. Moreover, the hot\u2010casting devices with PM6:BTP\u2010eC9 deliver a remarkable fill factor\u00a0of 80.31% and efficiency\u00a0of 18.52% in OX, representing the record value among binary devices with green solvent. This work demonstrates a facile strategy to manipulate the molecular distribution and arrangement for boosting the efficiency of OSCs with high\u2010boiling solvents.<\/jats:p>","DOI":"10.1002\/adma.202305356","type":"journal-article","created":{"date-parts":[[2023,8,9]],"date-time":"2023-08-09T07:09:16Z","timestamp":1691564956000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":95,"title":["Hot\u2010Casting Strategy Empowers High\u2010Boiling Solvent\u2010Processed Organic Solar Cells with Over 18.5% Efficiency"],"prefix":"10.1002","volume":"36","author":[{"given":"Chucheng","family":"Yang","sequence":"first","affiliation":[{"name":"Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectric\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengyun","family":"Jiang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectric\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shanshan","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectric\/Electrophotonic Conversion Materials School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing 100081 China"},{"name":"Analysis &amp; 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