This study successfully designed and synthesized two nonfused ring electron acceptors, 412-6F and 412-6Cl, modified with fluorine and chlorine substituents, respectively. Single-crystal analysis revealed that 412-6F possesses a planar molecular backbone and exhibits pronounced dipole-dipole interactions between the fluorine atoms on the lateral phenyl groups and the carbonyl oxygen atoms on the end groups. This specific interaction promotes dense end-group stacking, leading to a reduced interlayer spacing. Improved crystallinity and coherence length are observed in the D18 : 412-6F blend film. Conversely, 412-6Cl adopts a more distorted configuration and lacks these interactions. As a result, the organic solar cell (OSC) based on D18 : 412-6F achieved a remarkable power conversion efficiency of 18.03 %, surpassing the performance of the D18 : 412-6Cl OSC. This underscores the importance of designing novel acceptors with beneficial intermolecular interactions to enhance OSC efficiency, thus providing a new direction for organic photovoltaic advancement.
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