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Energy Transfer in Photosystem I of Cyanobacteria Synechococcus elongatus: Model Study with Structure-Based Semi-Empirical Hamiltonian and Experimental Spectral Density

Mino Yang, Ana Damjanovi, Harsha M. Vaswani and Graham R. Fleming

Department of Chemistry, University of California, Berkeley and Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California

Correspondence: Address reprint requests to Graham R. Fleming. E-mail: GRFleming{at}lbl.gov.

We model the energy transfer and trapping kinetics in PSI. Rather than simply applying Förster theory, we develop a new approach to self-consistently describe energy transfer in a complex with heterogeneous couplings. Experimentally determined spectral densities are employed to calculate the energy transfer rates. The absorption spectrum and fluorescence decay time components of the complex at room temperature were reasonably reproduced. The roles of the special chlorophylls (red, linker, and reaction center, respectively) molecules are discussed. A formally exact expression for the trapping time is derived in terms of the intrinsic trapping time, mean first passage time to trap, and detrapping time. The energy transfer mechanism is discussed and the slowest steps of the arrival at the primary electron donor are found to contain two dominant steps: transfer-to-reaction-center, and transfer-to-trap-from-reaction-center. The intrinsic charge transfer time is estimated to be 0.81.7 ps. The optimality with respect to the trapping time of the calculated transition energies and the orientation of Chls is discussed.

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