As organic photovoltaic performance approaches 20% efficiencies, causal structure-performance relationships must be established for devices to realize theoretical limits and become commercially competitive. Here, we reveal evidence of a causal relationship between mixed donor-acceptor interfaces and charge generation in polymer-fullerene solar cells. To do this, we combine a holistic loss analysis of device performance with quantitative synchrotron X-ray nanocharacterization to identify a >98% anticorrelation between field-dependent geminate recombination and nanodomain purity.
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