The Importance of Entanglements in Optimizing the Mechanical and Electrical Performance of All-Polymer Solar Cells

Organic solar cells that have all-polymer active layers may have several advantages compared with polymer–small molecule systems including improved mechanical and thermodynamic stability; however, an all-polymer active layer does not guarantee robust mechanical behavior. Here, we consider key parameters that may influence the mechanical behavior and power conversion efficiency of all-polymer solar cells (all-PSCs). Considerations include the thermal transition temperature of the polymers, the molecular weight (MW) of the polymers, and film morphology. The impact these features have on mechanical behavior is probed by measuring the cohesive fracture energy (G c), crack onset strain, and elastic modulus. We find that the selection of ductile polymers with high MW enhances interchain interactions that improve the mechanical resilience of the films. High-MW polymers are also found to maximize the power conversion efficiency (PCE). Using this strategy, BHJ films with the best reported combination of G c (7.96 J m–2) and PCE (6.94%) are demonstrated. Finally, it is found that increasing the film thickness increases the fracture energy of the films but at the cost of PCE. These findings provide a fundamental perspective on the design strategy to achieve high performance and mechanically robust organic solar cells.