Fused aromatic rings are widely employed in organic solar cell (OSC) materials due to their planarity and rigidity. Here, we designed and synthesized four two-dimensional non-fullerene acceptors, D6-4F, D6-4Cl, DTT-4F, and DTT-4Cl, based on two new fused planar ring structures of f-DTBDT-C6 and f-DTTBDT. Owing to the desirable phase separation formed in the blend films and the higher energy levels induced by the extra alkyl groups, PM6:D6-4F-based devices achieved a high = 0.91 V with PCE = 11.10%, FF = 68.54%, and = 17.75 mA/cm. Because of the longer π-conjugation of the f-DTTBDT core with nine fused rings, DTT-4F and DTT-4Cl showed high molar extinction coefficients and broad absorption bands that enhanced the current density of OSCs. Finally, the PM6:DTT-4F-based devices achieved a = 19.82 mA/cm with PCE = 9.68%, = 0.83 V, and FF = 58.85%.
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