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The formation of bound electron-hole pairs, also called charge-transfer (CT)states, in organic-based photovoltaic devices is one of the dominant lossmechanisms hindering performance. While CT state dynamics following electrontransfer from donor to acceptor have been widely studied, there is not muchknown about the dynamics of bound CT states produced by hole transfer from theacceptor to the donor. In this letter, we compare the dynamics of CT statesformed in the different charge-transfer pathways in a range of model systems.We show that the nature and dynamics of the generated CT states are similar inthe case of electron and hole transfer. However the yield of bound and freecharges is observed to be strongly dependent on the HOMOD-HOMOA and LUMOD-LUMOAenergy differences of the material system. We propose a qualitative model inwhich the effects of static disorder and sampling of states during therelaxation determine the probability of accessing CT states favourable forcharge separation.

Charge-Transfer State Dynamics Following Hole and Electron Transfer in Organic Photovoltaic Devices