Achieving a High Fill Factor and Stability in Perylene Diimide–Based Polymer Solar Cells Using the Molecular Lock Effect between 4,4′‐Bipyridine and a Tri(8‐hydroxyquinoline)aluminum(III) Core

Abstract

AbstractTwo novel perylene diimide (PDI)–based derivatives, Alq3‐PDI and Alq3‐PDI2, are synthesized by flanking a 3D tri(8‐hydroxyquinoline)aluminum(III) (Alq3) core with PDI and a helical PDI dimer (PDI2) to construct high‐performance small molecular nonfullerene acceptors (SMAs). The 3D Alq3 core significantly suppresses the molecular aggregation of the resulting SMAs, leading to a well‐mixed blend with a PTTEA donor polymer and weak phase separation. Compared with Alq3‐PDI, the extended π‐conjugation of Alq3‐PDI2 results in higher‐order molecular packing, which improves the absorption and phase separation behavior. Thus, the Alq3‐PDI2 devices have higher Jsc and FF values and better device performance, which are further enhanced by a small amount of 4,4′‐bipyridine (Bipy) as an additive. The coordination between Bipy and the Alq3 core promotes molecular packing and phase separation, which lower charge recombination and enhanced charge collection in the resulting devices. Therefore, a largely improved Jsc of 15.74 mA cm−2 and very high FF of 71.27% are obtained in the Alq3‐PDI2 devices, resulting in a power conversion efficiency of 9.54%, which is the best value reported for PDI‐based polymer solar cells. The coordination can also serve as a “molecular lock,” which prevents molecular motion and thus improves device stability.