Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV16)
Publication date: 28th March 2016
Although organic heterojunctions can separate charges with near-unity efficiency and on a sub-picosecond timescale, the full details of the charge-separation process remain unclear. In typical models, the Coulomb binding between the electron and the hole can exceed the thermal energy kBT by an order of magnitude, making it impossible for the charges to separate before recombining. Here, we consider the entropic contribution to charge separation in the presence of disorder and find that even modest amounts of disorder have a decisive effect, reducing the charge-separation barrier to about kBT or eliminating it altogether. Therefore, the charges are usually not thermodynamically bound at all and could separate spontaneously if the kinetics otherwise allowed it, i.e., if the hopping frequency is high compared to the recombination rate. Our conclusion holds despite the worst-case assumption of localised, thermalised carriers, and is only strengthened if mechanisms like delocalisation or 'hot' states are also present and drive the barrier down even further.
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