Abstract
Ultrafast pump-push-probe/photocurrent experiments have confirmed that free charges can be spontaneously generated in single-component organic solar cells. A deeper understanding of the experimental results is expected to further modulate the charge yield. Herein, the effect of an infrared push pulse on the relaxed exciton in conjugated polymers is theoretically studied. We find that the relaxed exciton can be pushed into different hot excitons depending on the energy of this infrared pulse. In particular, the dynamics of the transition from localized to delocalized excitons is explicitly presented. Moreover, we attempt to demonstrate that the delocalization effect of hot exciton is favorable for charge generation by introducing a driving field. The results suggest that the strength of the driving field and timescale required for the dissociation of hot exciton is significantly reduced compared to this relaxed exciton. Finally, the influence of the photoexcitation conditions on the charge generation is discussed to further elucidate the effect of hot exciton delocalization. Overall, this work has the potential to provide further information for the analysis and control of charge generation by hot exciton dissociation.
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