The development of simple and water-/alcohol-soluble interfacial materials is crucial for the cost-effective fabrication process of polymer solar cells (PSCs). Herein, highly efficient PSCs are reported employing water-/alcohol-soluble and low-cost rhodamines as cathode interfacial layers (CILs). The results reveal that rhodamine-based CILs can reduce the work function of the Al cathode and simultaneously increase the open-circuit voltage, current density, fill factor, and power conversion efficiency (PCE) of PSCs. The solution-processed rhodamine-based PSCs demonstrated a remarkable PCE of 10.39%, which is one of the best efficiencies reported for thieno[3,4-b]thiophene/benzodithiophene:[6,6]-phenyl C-butyric acid methyl ester-based PSCs so far. The efficiency is also 42.3% higher than that of the vacuum-deposited Ca-based device (PCE of 7.30%) and 21.5% higher than that of the complicated solution-processable polymeric electrolyte poly[(9,9-bis(3-(N,N-dimethylamino)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)]-based device (PCE of 8.55%). Notably, rhodamines are very economical and have been extensively used as dyes in industries. Our work indicates that rhodamines have shown a strong potential as CILs compared to their counterparts in the large-area fabrication process of PSCs.
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