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Ultrafast Exciton-Exciton Coherent Transfer in Molecular Aggregates

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Abstract Book of the XXIII IUPAP International Conference on Statistical Physics, Genova, Italy, (9-13 July 2007)

Abstract

We have developed the non-Markovian time evolution equation which can describe the exciton-exciton coherent transfer(EECT) in strongly coupled molecular aggregates. Its solutions make it possible to derive explicit contributions from EECT to the nonlinear response function for four-wave-mixing experiments including photon echo. We take into account double-exciton states, static disorder and heat bath coupling represented by arbitrary spectral densities. Our derivation is based on the doorway-window representation and the projection operator method which are now developed for exciton-exciton coherent states. Applications of our analytical expression to strongly coupled B850 monomers in the Light harvest II(LH2) antenna system are discussed. We have found that EECT is indispensable in ultrafast phenomena of strongly coupled molecular aggregates like LH2, and that EECT generates the significant contribution to the nonlinear spectral signals.

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