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Herein, an unconjugated side\u2010chain strategy to design fused\u2010benzodithiophene\u2010based non\u2010fullerene small molecule acceptors (SMAs) via vertical aromatic side\u2010chain engineering on the ladder\u2010type core is employed. Three SMAs named BTTIC\u2010Th, BTTIC\u2010TT, and BTTIC\u2010Ph with thiophene, thieno[3,2\u2010<jats:italic>b<\/jats:italic>]thiophene, and benzene, respectively, as side chains, are designed and synthesized. Three SMAs exhibit similar absorption ranges but different lowest unoccupied molecular orbital (LUMO) energy levels due to the different strength of the \u03b4\u2010inductive effect between vertical aromatic side chains and their electron\u2010rich core. Organic solar cells based on PBDB\u2010T:BTTIC\u2010TT achieve a power conversion efficiency (PCE) of 13.44%, which is higher than the PCE of devices based on PBDB\u2010T:BTTIC\u2010Th (12.91%) and PBDB\u2010T:BTTIC\u2010Ph (9.14%). The difference in device performance is investigated by electrical and morphological characterizations. A large domain size and different types of \u03c0\u2013\u03c0 stacking are found in the bulk heterojunction layer of PBDB\u2010T:BTTIC\u2010Ph blend film, which are detrimental to exciton dissociation and charge transport. Overall, it is demonstrated that when designing unconjugated side chains, thieno[3,2\u2010<jats:italic>b<\/jats:italic>]thiophene is superior to thiophene and benzene through its dual roles of promoting the LUMO energy level and optimizing the morphology. These results shed light on the side\u2010chain engineering of high\u2010performance non\u2010fullerene SMAs.<\/jats:p>","DOI":"10.1002\/adfm.201902155","type":"journal-article","created":{"date-parts":[[2019,5,6]],"date-time":"2019-05-06T16:03:37Z","timestamp":1557158617000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":112,"title":["Unconjugated Side\u2010Chain Engineering Enables Small Molecular Acceptors for Highly Efficient Non\u2010Fullerene Organic Solar Cells: Insights into the Fine\u2010Tuning of Acceptor Properties and Micromorphology"],"prefix":"10.1002","volume":"29","author":[{"given":"Tao","family":"Liu","sequence":"first","affiliation":[{"name":"College of Materials Science and Engineering Shenzhen University  Shenzhen 518060 China"},{"name":"Department of Chemistry and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction Hong Kong University of Science and Technology  Clear Water Bay Kowloon 999077 Hong Kong"}]},{"given":"Wei","family":"Gao","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering Shenzhen University  Shenzhen 518060 China"},{"name":"Department of Chemistry and Hubei Key Lab on Organic and Polymeric Optoelectronic Materials Wuhan University  Wuhan 430072 P. 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