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Recent advances in non-fullerene acceptors (NFAs) have resulted in significant improvement in the power conversion efficiencies (PCEs) of organic solar cells (OSCs). In our efforts to boost open-circuit voltage ( V  OC ) for OSCs, the molecular design employing thiobarbituric acid (TBTA) end groups and an indacenodithieno[3,2- b ]thiophene (IDTT) core gives rise to NFAs with significantly raised lowest unoccupied molecular orbital (LUMO) energy level, which, when paired with PCE10, can achieve V  OC 's over 1.0 V and decent PCEs that outperform the equivalent devices based on the benchmark ITIC acceptor. While the use of a TBTA end group is effective in tuning energy levels, very little is known about how the alkyl substitution on the TBTA group impacts the solar cell performance. To this end, TBTA end groups are alkylated with linear, branched, and aromatic sidechains to understand the influence on thin-film morphology and related device performances. Our study has confirmed the dependence of solar cell performance on the end-group substituents. More importantly, we reveal the presence of an ideal window of crystallinity associated with the medium-length hydrocarbon chains such as ethyl and benzyl. Deviation to the shorter methyl group makes the acceptor too crystalline to mix with the polymer donor and form proper domains, whereas longer and branched alkyl chains are too sterically bulky and hinder charge transport due to nonideal packing. Such findings underline the comprehensive nature of thin-film morphology and the subtle end-group effects for the design of non-fullerene acceptors.

Substitution Effect on Thiobarbituric Acid End Groups for High Open-Circuit Voltage Non-Fullerene Organic Solar Cells