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Nonperturbative theory for the optical response to strong light of the light harvesting complex II of plants: saturation of the fluorescence quantum yield.

Recent progress in resolution of the structure of the light harvesting complex II provides the basis for theoretical predictions on nonlinear optical properties from microscopic calculations. An approach to absorption and fluorescence is presented within the framework of Bloch equations using a correlation expansion of relevant many particle interactions. The equations derived within the framework of this theory are applied to describe fluorescence saturation phenomena. The experimentally observed decrease of the normalized fluorescence quantum yield from 1 to 0.0001 upon increasing the intensity of laser pulse excitation at 645 nm by five orders of magnitude [R Schödel et al., Biophys. J. 71, 3370 (1996)] is explained by Pauli blocking effects of optical excitation and excitation energy transfer.