LAUSR

Abstract A novel, star‐shaped electron acceptor, DMTPA‐PDI3, derived from a planar dimethylmethylene‐bridged triphenylamine core with three acetylene‐linked perylene diimide (PDI) units is developed as a nonfullerene acceptor for organic solar cells (OSCs). DMTPA‐PDI3 manifests significantly reduced intramolecular twisting, enabling sufficient system‐wide π‐electron delocalization leading to broadened spectral absorption and raised lowest unoccupied molecular orbital level. As a result, higher and more balanced hole and electron transport properties are observed. Active layers for OSCs comprising DMTPA‐PDI3 acceptor and PBT7‐Th donor exhibit suppressed intermolecular aggregation, giving rise to uniform nanophase network formation. These OSC devices have afforded respectably high power‐conversion efficiency of about 5%.