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State of the art organic solar cells exhibit power conversion efficiencies of 18 % and above. These devices benefit from a significant suppression of free charge recombination with regard to the Langevin-limit of charge encounter in a homogeneous medium. It has been recognized that the main cause of suppressed free charge recombination is the reformation and resplitting of charge transfer states at the interface between donor and acceptor domains. Here, we use kinetic Monte Carlo simulations to understand the interplay between free charge motion and recombination in an energetically-disordered phase-separated donor-acceptor blend. We identify conditions under which recombination is encounter-dominated and resplitting-dominated. In the latter regime, the non-geminate recombination coefficient becomes independent of the attempt-to-hop frequency, and for a given disorder, independent of charge carrier mobility. Our simulations show that free charge encounter in the phase-separated disordered blend is determined by the average mobility of all carriers, while CT reformation and resplitting involves mostly states near the transport energy. As a consequence, charge encounter is more affected by increased disorder than the resplitting of the CT state. As a consequence, the larger is the energetic disorder, the stronger will CT-resplitting suppress non-geminate recombination versus the Langevin-limit. These findings have important implications for the understanding of suppressed recombination in solar cells with non-fullerene acceptors which are known to exhibit lower energetic disorder than fullerenes.
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The power conversion efficiencies (PCEs) of organic solar cells (OSCs) using non-fullerene acceptors (NFAs) have now reached 18%. However, this is still lower than inorganic solar cells, for which PCEs >20% are commonplace. A key reason is that OSCs
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