Molecular-Scale Understanding of Cohesion and Fracture in P3HT:Fullerene Blends

Quantifying cohesion and understanding fracture phenomena in thin-film electronic devices are necessary for improved materials design and processing criteria. For organic photovoltaics (OPVs), the cohesion of the photoactive layer portends its mechanical flexibility, reliability, and lifetime. Here, the molecular mechanism for the initiation of cohesive failure in bulk heterojunction (BHJ) OPV active layers derived from the semiconducting polymer poly(3-hexylthiophene) [P3HT] and two monosubstituted fullerenes is examined experimentally and through molecular-dynamics simulations. The results detail how, under identical conditions, cohesion significantly changes due to minor variations in the fullerene adduct functionality, an important materials consideration that needs to be taken into account across fields where soluble fullerene derivatives are used.