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| - On the Mechanism of Light Harvesting in Photosynthetic Purple Bacteria: B800 to B850Energy Transfer
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| - The rate of energy transfer from B800 to B850 in the peripheral light harvesting complex LH2 is modeledin detail. A method for determining ensemble average energy transfer rates in complex, coupledmultichromophoric systems is reported and is employed to investigate the interplay of electron−phononcoupling (fast fluctuations of the protein) and site energy disorder (slow fluctuations) on the spectral overlapbetween donor and acceptor, and therefore the energy transfer rate. A series of model calculations for Rb.sphaeroides is reported. The disorder is found to have a marked influence on the calculated rate of energytransfer and is responsible for a faster energy transfer time than would occur in its absence and furthermoreaccounts for the weak temperature dependence observed in experiment. The excitonic nature of the acceptor(albeit dynamically localized) also has impact in terms of how B850 functions as an energy acceptor. Theseconclusions are further elucidated by calculations of Rps. acidophila B800−B850 and a series of reconstitutedcomplexes containing a systematically blue-shifted B800 absorption band. The role of dielectric effects isconsidered. It is reported that interaction of the B800 and B850 transition densities with the carotenoids hasan effect on the B800−B850 electronic couplings.
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