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The mechanism of electron-hole separation in organic solar cells is currentlyhotly debated. Recent experimental work suggests that these charges canseparate on extremely short timescales (<100 fs). This can be understood interms of delocalised transport within fullerene aggregates, which is thought toemerge on short timescales before vibronic relaxation induces polaronformation. However, in the optimal heterojunction morphology, electrons andholes will often re-encounter each other before reaching the electrodes. Ifsuch charges trap and cannot separate, then device efficiency will suffer. Herewe extend the theory of ultrafast charge separation to incorporate polaronformation, and find that the same delocalised transport used to explainultrafast charge separation can account for the suppression of nongeminaterecombination in the best devices.

Ultrafast Charge Separation and Nongeminate Electron-Hole Recombination in Organic Photovoltaics