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

S Jang, S Hoyer, G Fleming, KB Whaley - Physical Review Letters, 2014 - APS
Physical Review Letters, 2014APS
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 …
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.
American Physical Society
以上显示的是最相近的搜索结果。 查看全部搜索结果