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Generalized master equation with non-markovian multichromophoric Förster resonance energy transfer for modular exciton densities

  • Author(s): Jang, S
  • Hoyer, S
  • Fleming, G
  • Whaley, KB
  • et al.

Published Web Location

https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.113.188102
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Abstract

© 2014 American Physical Society. A generalized master equation (GME) governing quantum evolution of modular exciton density (MED) is derived for large scale light harvesting systems composed of weakly interacting modules of multiple chromophores. The GME-MED offers a practical framework to incorporate real time coherent quantum dynamics calculations of small length scales into dynamics over large length scales, and also provides a non-Markovian generalization and rigorous derivation of the Pauli master equation employing multichromophoric Förster resonance energy transfer rates. A test of the GME-MED for four sites of the Fenna-Matthews-Olson complex demonstrates how coherent dynamics of excitonic populations over coupled chromophores can be accurately described by transitions between subgroups (modules) of delocalized excitons. Application of the GME-MED to the exciton dynamics between a pair of light harvesting complexes in purple bacteria demonstrates its promise as a computationally efficient tool to investigate large scale exciton dynamics in complex environments.

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