High‐Efficiency Organic Solar Cells Based on Asymmetric Acceptors Bearing One 3D Shape‐Persistent Terminal Group.

Three asymmetric non‐fullerene acceptors (LL2, LL3, and LL4) are designed and synthesized with one norbornyl‐modified 1,1‐dicyanomethylene‐3‐indanone (CBIC) terminal group and one chlorinated 1,1‐dicyanomethylene‐3‐indanone (IC‐2Cl) terminal group. The three‐dimensional shape‐persistent CBIC terminal group can effectively enhance the solubility and tune the packing mode of acceptors. Compared with their symmetric counterparts (LL2‐2Cl, LL3‐2Cl, and LL4‐2Cl) bearing two IC‐2Cl terminals, the asymmetric acceptors show improved solubilities, giving rise to enhanced crystallinity and favored nanomorphology for charge transport in the blend films with PBDB‐T. Asymmetric acceptors based organic solar cells (OSCs) also show much lower voltage loss due to their higher ECT and EQEEL values. Therefore, they exhibit 17−27% higher power conversion efficiency (PCE) than OSCs based on the corresponding symmetric acceptors. Among these six acceptors, LL3 with a central benzotriazole core shows the best PCE of 16.82% with an outstanding Jsc of 26.97 mA cm−2 and a low nonradiative voltage loss (ΔVnr) of 0.18 V, the best values for PBDB‐T based OSCs. The Jsc and ΔVnr also represent the best reported for asymmetric non‐fullerene acceptors‐based OSCs to date. The results demonstrate that the combination of the unique CBIC terminal group with the asymmetric strategy is a promising way to enhance the performance of OSCs. [ABSTRACT FROM AUTHOR]