The correlation between molecular structure and photovoltaic performance is lagging for constructing high-performance indoor organic photovoltaic (OPV) cells. Herein, this relationship is investigated in depth by employing two medium-bandgap nonfullerene acceptors (NFAs). The newly synthesized NFA of FTCCBr exhibits a similar bandgap and molecular energy level, but a much stronger dipole moment and larger average electrostatic potential (ESP) compared with ITCC. After blending with the polymer donor PB2, the PB2:ITCC and PB2:FTCCBr blends exhibit favorable bulk-heterojunction morphologies and the same driving force, but the PB2:FTCCBr blend exhibits a large ESP difference. In OPV cells, the PB2:ITCC-based device produces a power conversion efficiency (PCE) of 11.0%, whereas the PB2:FTCCBr-based device gives an excellent PCE of 14.8% with an open-circuit voltage (V ) of 1.05 V, which is the highest value among OPV cells with V values above 1.0 V. When both acceptor-based devices work under a 1000 lux of 3000 K light-emitting diode, the PB2:ITCC-based 1 cm device yields a good PCE of 25.4%; in contrast, the PB2:FTCCBr-based 1 cm device outputs a record PCE of 30.2%. These results suggest that a large ESP offset in photovoltaic materials is important for achieving high-performance OPV cells.
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