Combination of Charge Delocalization and Disorder Enables Efficient Charge Separation at Photoexcited Organic Bilayers

Abstract

We study incoherent charge separation in a lattice model of an all-organic bilayer. Charge delocalization is taken into account by working in the basis of electron–hole pair eigenstates, and the separation is described as a series of incoherent hops between these states. We find that relatively weak energetic disorder, in combination with good charge delocalization, can account for efficient and weakly field- and temperature-dependent separation of the strongly bound charge transfer (CT) state. The separation efficiency is determined by the competition between the recombination from the initial CT state and the escape toward intermediate CT states, from which free-charge states can be reached with certainty. The separation of donor excitons also exhibits quite high yields, less bound excitons separating more efficiently. Overall, our results support the notion that efficient charge separation can be achieved even out of strongly bound pair states without invoking coherent effects.