The hole transporting layers (HTLs) between the electrode and light absorber play a vital role in charge extraction and transport processes in organic solar cells (OSCs). Herein, a bilayer structure HTL of CuSCN/TFB is formed by soluble copper(I) thiocyanate (CuSCN) and poly[(9,9-dioctylfluorenyl-2,7-diyl)--(4,4'-(-(4-butylphenyl)))] (TFB). The excellent charge extraction capability is proved in nonfullerene PM6:Y6 and fullerene PTB7-Th:PCBM blend system-based cells. The introduction of TFB tunes the work function and polishes the interfacial contact between the HTL and light absorber, which favors the hole extraction process in cells. Meanwhile, lower recombination loss, higher exciton dissociation probability, and larger domain size are observed in CuSCN/TFB HTL-based cells compared to those of the reference cell with the pristine CuSCN HTL, which significantly improve the photovoltaic performance. As a result, a champion efficiency of 15.10% is obtained, which is >14% higher than the efficiency of 13.15% obtained in the reference cell. This study suggests that CuSCN/TFB is a promising HTL to achieve high efficiency for OSCs.
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