Quantitative relations between interaction parameter, miscibility and function in organic solar cells

TL;DR: This work establishes a quantitative ‘constant-kink-saturation’ relation between χaa and the fill factor in organic solar cells that is verified in detail in a model system and delineated across numerous high- and low-performing materials systems, including fullerene and non-fullerene acceptors.

Abstract: Although it is known that molecular interactions govern morphology formation and purity of mixed domains of conjugated polymer donors and small-molecule acceptors, and thus largely control the achievable performance of organic solar cells, quantifying interaction–function relations has remained elusive. Here, we first determine the temperature-dependent effective amorphous–amorphous interaction parameter, χaa(T), by mapping out the phase diagram of a model amorphous polymer:fullerene material system. We then establish a quantitative ‘constant-kink-saturation’ relation between χaa and the fill factor in organic solar cells that is verified in detail in a model system and delineated across numerous high- and low-performing materials systems, including fullerene and non-fullerene acceptors. Our experimental and computational data reveal that a high fill factor is obtained only when χaa is large enough to lead to strong phase separation. Our work outlines a basis for using various miscibility tests and future simulation methods that will significantly reduce or eliminate trial-and-error approaches to material synthesis and device fabrication of functional semiconducting blends and organic blends in general. This work reports a quantitative investigation of the interaction parameter and miscibility of donor and acceptor organic molecules and their relationship with the fill factor and photovoltaic performance of bulk-heterojunction organic solar cells.