LAUSR

Fine-tuning the crystallinity and self-aggregation features of donors/acceptor materials toward high-efficiency organic solar cells (OSCs) is of crucial importance. Here, a convenient yet effective way to simultaneously control the crystallinity and self-aggregation of the fused ring electron acceptor (FREA) is demonstrated by altering the length of the first-position branched alkyl chain on the cyclic unit. Specifically, three carbazole-based FREAs, 4TC-4F-C6C6, 4TC-4F-C8C8, and 4TC-4F-C10C10, are synthesized by changing the length of the first-position branched alkyl chain on the carbazole unit. The crystallinity of the studied acceptors decreases as the branched alkyl chain is lengthened. The ability of the acceptors to undergo self-aggregation decreases in the order 4TC-4F-C10C10, 4TC-4F-C6C6, and 4TC-4F-C8C8. The medium crystallinity and lower self-aggregation properties of 4TC-4F-C8C8 result in favorable phase separation when blended with poly-[(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione))] (PM6), which is conducive to effective exciton dissociation and charge transport. Consequently, the OSC device based on PM6:4TC-4F-C8C8 delivers the best power conversion efficiency of 14.85%.