Multiple Exciton Effects in Molecular Aggregates: Application to a Photosynthetic Antenna Complex

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Abstract
The creation of multiple exciton states in chromophore complexes achieved by high laser field excitations and followed by ultrafast dissipative exciton-vibrational dynamics is studied theoretically. Concentrating on a molecular heterodimer a unified microscopic description is offered for coherent vibrational dynamics, excited state absorption, and exciton-exciton annihilation processes. The theory explains the intensity dependence of pump-probe signals recently measured at the light harvesting complex of the photosystem II of higher plants [Bittner et al., J. Phys. Chem. 98, 11 821 (1994)]. Signatures of non-Markovian effects in the dissipative dynamics are found.