A chlorinated nonacyclic carbazole-based acceptor affords over 15% efficiency in organic solar cells

In this contribution, a dithienocyclopentacarbazole (DTC)-based and two dithieno[3,2- b ]thiophenecyclopentacarbazole (DTTC)-based non-fullerene acceptors (NFAs) named DTC-4F, DTTC-4F and DTTC-4Cl were exploited to elucidate the effects of conjugation extension and end group chlorination. DTTC-4F was designed through conjugation extension on the basis of DTC-4F by fusing one additional thiophene on both flanks of the heptacyclic DTC core, generating the nonacyclic DTTC core. Compared with DTC-4F, DTTC-4F features up-shifted energy levels, red-shifted absorption and enhanced π-π interaction. PM6:DTTC-4F exhibits a decent PCE of 13.89% with a V OC of 0.95 V, a J SC of 21.66 mA cm −2 and a FF of 67.60% . Although DTTC-4F affords a reduced FF compared to DTC-4F, a DTTC-4F-based device delivers a higher PCE than DTC-4F-based devices due to the extended absorption range of DTCC-4F in comparison with DTC-4F. Since chlorinated NFAs are known to possess stronger π-π interaction than fluorinated NFAs, DTTC-4Cl was therefore synthesized by end-capping DTTC core with 2Cl-IC groups instead of 2F-IC groups. Moreover, DTTC-4Cl demonstrates a red-shifted absorption in comparison with DTTC-4F, which is beneficial for light-harvesting. Overall, PM6:DTTC-4Cl affords an outstanding PCE of 15.42% with a V OC of 0.92 V, a J SC of 22.64 mA cm −2 and a FF of 74.04%, which is the record PCE observed in carbazole-based NFAs. A systematic approach involving conjugation extension and end group chlorination is capable of enhancing both J SC and PCE. Overall, the PM6:DTTC-4Cl-based device delivers a remarkable PCE of 15.42% with a V OC of 0.92 V, a J SC of 22.64 mA cm −2 and an FF of 74.04%.