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We present an exciton/lattice model of the electronic dynamics of primary photoexcitations in a polymeric semiconductor heterojunction which includes both polymer pi-stacking, energetic disorder, and phonon relaxation. Results from our model are consistent with a wide range of recent experimental evidence that excitons decay directly to well-defined polarons on a sub-100 fs timescale, which is substantially faster than exciton relaxation processes. Averaging over multiple samples, we find that as the interfacial offset is increased, a substantial fraction of the density of electronic states in the energy region about the initial exciton carries significant charge-transfer character with two charges separated in the outer regions of the model lattice. The results indicate a slight increase in the density of such current-producing states if the region close to the interface is more disordered. However, since their density of states overlaps the excitation line-shape of the primary exciton, we show that it is possible that the exciton can decay directly into current-producing states via tunneling on an ultrafast time-scale. We find this process to be independent of the location of ene

Author

Bittner, Eric R.; Silva, Carlos

Published

2013

Language

EN