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The relationship of the temperature–light intensity dependence of open‐circuit voltage Voc in nonfullerene‐based organic solar cells with their material characteristics and multimechanism recombination parameters is described. The systematic variation of the effective bandgap Eg,eff and the electrode layers allows the observation of different relative contributions of bimolecular, bulk, and surface trap‐assisted recombination mechanisms. The complementary advantages of the analytical model and the established voltage‐impedance spectroscopy technique provide a useful tool to quantify multimechanism recombination parameters, effective density of states Nc, and energetic disorder σ in organic solar cells under operating conditions. The validity of the proposed model to understand the temperature and light intensity dependent of Voc is shown by applying it to four different donor:nonfullerene acceptor blend systems with conventional or inverted device architectures. [ABSTRACT FROM AUTHOR]

Even though significant breakthroughs with over 18% power conversion efficiencies (PCEs) in polymer:non‐fullerene acceptor (NFA) bulk heterojunction organic solar cells (OSCs) have been achieved, not many studies have focused on acquiring a comprehensive understanding of the underlying mechanisms governing these systems. This is because it can be challenging to delineate device photophysics in polymer:NFA blends comprehensively, and even more complicated to trace the origins of the differences in device photophysics to the subtle differences in energetics and morphology. Here, a systematic study of a series of polymer:NFA blends is conducted to unify and correlate the cumulative effects of i) voltage losses, ii) charge generation efficiencies, iii) non‐geminate recombination and extraction dynamics, and iv) nuanced morphological differences with device performances. Most importantly, a deconvolution of the major loss processes in polymer:NFA blends and their connections to the complex BHJ morphology and energetics are established. An extension to advanced morphological techniques, such as solid‐state NMR (for atomic level insights on the local ordering and donor:acceptor ππ interactions) and resonant soft X‐ray scattering (for donor and acceptor interfacial area and domain spacings), provide detailed insights on how efficient charge generation, transport, and extraction processes can outweigh increased voltage losses to yield high PCEs. [ABSTRACT FROM AUTHOR]