Abstract
Two-pulse four-wave mixing (FWM) and excitation-wavelength-dependent transient absorption experiments are reported for pseudoisocyanine (PIC) J aggregates to investigate the relaxation mechanism of Frenkel excitons. The relaxation time of the coherent polarization is 400 fs and a time-resolved FWM experiment shows no photon-echo signals. Excitation-wavelength-dependent transient absorption changes show strong coupling between excitons and phonons in the aggregates. The results support the model where strong correlations between disorder in the molecular transition energy are effective in the delocalization of excitons.
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