AbstractOrganic photovoltaics (OPV) now can exceed 20% power conversion efficiency in single junction solar cells. To close the remaining gap to competing technologies, both fill factor and open‐circuit voltage must be optimized. The Langevin reduction factor is a well‐known concept that measures the degree to which charge extraction is favored over charge recombination. It is therefore ideally suited as an optimization target in high‐throughput workflows; however, its evaluation so far requires expert interaction. Here, an integrated high‐throughput workflow is presented, able to obtain the Langevin reduction factor within a few seconds with high accuracy without human intervention and thus suited for autonomous experiments. This is achieved by combining evidence from UV–vis spectra, current–voltage curves, and a novel implementation of microsecond transient absorption kinetics allowing, for the first time, the intrinsic determination of charge absorption cross‐sections, which is crucial to reporting stationary charge densities. The method is demonstrated by varying the donor:acceptor ratio of the high performance OPV blend PM6:Y12. The high reproducibility of the method allows to find a strictly exponential relationship between the PM6 exciton energy and the Langevin reduction factor.
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