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| - Heterogeneous Exciton Dynamics Revealed by Two-Dimensional Optical Spectroscopy
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| - We show that optical two-dimensional (2D) spectroscopy can recover ultrafast heterogeneous dynamics ofclosely spaced delocalized exciton states from a molecular exciton manifold characterized by a single absorptionband. The complete experimental third-order nonlinear optical response from room-temperature J-aggregatesin liquid phase is reproduced for the first time with self-consistent Frenkel exciton theory combined withmodified Redfield theory. We show that exciton relaxation between the exciton states and nuclear-motion-induced exchange-narrowed energy fluctuations of individual delocalized exciton states can be distinguishedbecause these two processes lead to a distinctively different evolution of the absolute 2D spectrum. Ourtechnique also allows recovery of the variation of the exciton relaxation rates as well as the degree of excitondelocalization across the absorption band.
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