Nonlinear Optical Response of Disordered J Aggregates in the Motional Narrowing Limit

Abstract

We discuss the theory of nonlinear optical response of molecular aggregates with frequency disorder. In contrast to the usual modeling, we allow for spatial correlations in the disorder. We show that the joint distribution of all multi-exciton frequencies can be determined analytically to first order in the disorder. It is demonstrated that, unlike linear absorption measurements, two-color pump-probe experiments may be used to observe intermolecular disorder correlations.