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While photovoltaic blends based on non‐fullerene acceptors are touted for their thermal stability, this type of acceptor tends to crystallize, which can result in a gradual decrease in photovoltaic performance and affects the reproducibility of the devices. Two halogenated indacenodithienothiophene‐based acceptors that readily co‐crystallize upon mixing are studied, which indicates that the use of an acceptor mixture alone does not guarantee the formation of a disordered mixture. The addition of the donor polymer to the acceptor mixture readily suppresses the crystallization, which results in a fine‐grained ternary blend with nanometer‐sized domains that do not coarsen due to a high Tg ≈ 200 °C. As a result, annealing at temperatures of up to 170 °C does not markedly affect the photovoltaic performance of ternary devices, in contrast to binary devices that suffer from acceptor crystallization in the active layer. The results indicate that the ternary approach enables the use of high‐temperature processing protocols, which are needed for upscaling and high‐throughput fabrication of organic solar cells. Further, ternary devices display a stable photovoltaic performance at 130 °C for at least 205 h, which indicates that the use of acceptor mixtures allows to fabricate devices with excellent thermal stability. [ABSTRACT FROM AUTHOR]

Abstract: Nonfullerene acceptors (NFAs) in blends with highly crystalline donor polymers have been shown to yield particularly high device voltage outputs, but typically more modest quantum yields for photocurrent generation as well as often lower fill factors (FF). In this study, we employ transient optical and optoelectronic analysis to elucidate the factors determining device photocurrent and FF in blends of the highly crystalline donor polymer PffBT4T‐2OD with the promising NFA FBR or the more widely studied fullerene acceptor PC71BM. Geminate recombination losses, as measured by ultrafast transient absorption spectroscopy, are observed to be significantly higher for PffBT4T‐2OD:FBR blends. This is assigned to the smaller LUMO‐LUMO offset of the PffBT4T‐2OD:FBR blends relative to PffBT4T‐2OD:PC71BM, resulting in the lower photocurrent generation efficiency obtained with FBR. Employing time delayed charge extraction measurements, these geminate recombination losses are observed to be field dependent, resulting in the lower FF observed with PffBT4T‐2OD:FBR devices. These data therefore provide a detailed understanding of the impact of acceptor design, and particularly acceptor energetics, on organic solar cell performance. Our study concludes with a discussion of the implications of these results for the design of NFAs in organic solar cells. [ABSTRACT FROM AUTHOR]