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Generalized Master Equation with Non-Markovian Multichromophoric Förster Resonance Energy Transfer for Modular Exciton Densities

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      The Semiclassical Initial Value Representation:  A Potentially Practical Way for Adding Quantum Effects to Classical Molecular Dynamics Simulations

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        Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature.

        The observation of long-lived electronic coherence in a photosynthetic pigment-protein complex, the Fenna-Matthews-Olson (FMO) complex, is suggestive that quantum coherence might play a significant role in achieving the remarkable efficiency of photosynthetic electronic energy transfer (EET), although the data were acquired at cryogenic temperature [Engel GS, et al. (2007) Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems. Nature 446:782-786]. In this paper, the spatial and temporal dynamics of EET through the FMO complex at physiological temperature are investigated theoretically. The numerical results reveal that quantum wave-like motion persists for several hundred femtoseconds even at physiological temperature, and suggest that the FMO complex may work as a rectifier for unidirectional energy flow from the peripheral light-harvesting antenna to the reaction center complex by taking advantage of quantum coherence and the energy landscape of pigments tuned by the protein scaffold. A potential role of quantum coherence is to overcome local energetic traps and aid efficient trapping of electronic energy by the pigments facing the reaction center complex.
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          Unified treatment of quantum coherent and incoherent hopping dynamics in electronic energy transfer: reduced hierarchy equation approach.

          A new quantum dynamic equation for excitation energy transfer is developed which can describe quantum coherent wavelike motion and incoherent hopping in a unified manner. The developed equation reduces to the conventional Redfield theory and Forster theory in their respective limits of validity. In the regime of coherent wavelike motion, the equation predicts several times longer lifetime of electronic coherence between chromophores than does the conventional Redfield equation. Furthermore, we show quantum coherent motion can be observed even when reorganization energy is large in comparison to intersite electronic coupling (the Forster incoherent regime). In the region of small reorganization energy, slow fluctuation sustains longer-lived coherent oscillation, whereas the Markov approximation in the Redfield framework causes infinitely fast fluctuation and then collapses the quantum coherence. In the region of large reorganization energy, sluggish dissipation of reorganization energy increases the time electronic excitation stays above an energy barrier separating chromophores and thus prolongs delocalization over the chromophores.
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            Author and article information

            Journal
            PRLTAO
            Physical Review Letters
            Phys. Rev. Lett.
            American Physical Society (APS)
            0031-9007
            1079-7114
            October 2014
            October 31 2014
            : 113
            : 18
            10.1103/PhysRevLett.113.188102
            © 2014

            http://link.aps.org/licenses/aps-default-license

            http://link.aps.org/licenses/aps-default-accepted-manuscript-license

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