Thermally-Induced Degradation in PM6:Y6-Based Bulk Heterojunction Organic Solar Cells

Thermally induced degradation of organic photovoltaic devices hinders the commercialization of this emerging PV technology. Thus, a precise understanding of the origin of thermal device instability, as well as identifying strategies to circumvent degradation is of utmost importance. Here, it investigates thermally-induced degradation of state-of-the-art PBDB-T-2F (PM6):BTP (Y6) bulk heterojunction solar cells at different temperatures and reveal changes of their optical properties, photophysics, and morphology. The open-circuit voltage and fill factor of thermally degraded devices are limited by dissociation and charge collection efficiency differences, while the short-circuit current density is only slightly affected. Energy-resolved electrochemical impedance spectroscopy measurements reveal that thermally degraded samples exhibit a higher energy barrier for the charge-transfer state to charge-separated state conversion. Furthermore, the field dependence of charge generation, recombination, and extraction are studied by time-delayed collection field and transient photocurrent and photovoltage experiments, indicating significant bimolecular recombination limits device performance. Finally, coupled optical-electrical device simulations are conducted to fit the devices’ current-voltage characteristics, enabling us to find useful correlations between optical and electrical properties of the active layers and device performance parameters.