How charges separate: correlating disorder, free energy, and open-circuit voltage in organic photovoltaics

Abstract

In order for a photovoltaic cell to function, charge carriers produced by photoexcitation must fully dissociate and overcome their mutual Coulomb attraction to form free polarons. This becomes problematic in organic systems in which the low dielectric constant of the material portends a long separation distance between independent polaron pairs. In this paper, we discuss our recent efforts to correlate the role of density of states, entropy, and configurational and energetic disorder to the open-circuit voltage, V_OC, of model type-II organic polymer photovoltaics. By comparing the results of a fully interacting lattice model to those predicted by a Wigner–Weisskopf type model we find that energetic disorder does play a significant role in determining the V_OC; however, mobility perpendicular to the interface plays the deciding role in the eventual fate of a charge-separated pair.