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In this paper a detailed theoretical analysis is presented of the temperature dependent radiative decay in aggregates of pseudoisocyanine (PIC). Our approach extends the original linear exciton-phonon coupling model used by Spano, Kuklinsky, and Mukamel [Phys. Rev. Lett. 65, 212 (1990)] including static disorder and second order exciton-phonon interactions. It is shown that for a one-dimensional exciton model neither of these additional effects alone or in combination with linear electron–phonon coupling can explain the steep rise in radiative lifetime at 40 K observed in the J-aggregate of PIC. However, when the aggregate assembles into a two-dimensional bricklike structure its radiative dynamics can be simulated, with linear exciton-optical phonon coupling as the only source for exciton scattering. Exciton-phonon scattering transfers oscillator strength from the k=0 state to other band states and also generates a nonequilibrium population among the exciton states, which persists during the superradiant ...

Exciton superradiance in aggregates: The effect of disorder, higher order exciton-phonon coupling and dimensionality