Generalized master equation with non-Markovian multichromophoric Förster resonance energy transfer for modular exciton densities.
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.
Department of Chemistry and Biochemistry, Queens College and the Graduate Center, City University of New York, 65-30 Kissena Boulevard, Flushing, New York 11367, USA.
Seogjoo
S
Jang
Department of Physics, University of California, Berkeley, California 94720, USA.
Stephan
S
Hoyer
Department of Chemistry, University of California, Berkeley, California 94720, USA and Physical Biosciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
Graham
G
Fleming
Department of Chemistry, University of California, Berkeley, California 94720, USA.
K Birgitta
KB
Whaley
D031541:Fluorescence Resonance Energy Transfer / Q000379:methods*; D045342:Light-Harvesting Protein Complexes / Q000737:chemistry*; D020560:Proteobacteria / Q000737:chemistry*; D011789:Quantum Theory
D045342:Light-Harvesting Protein Complexes