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Cited by 135Spectroscopy and Quantum Chemical StudiesPhotochemistry and Electron Transfer StudiesStrong Light-Matter Interactions

Iterative linearized density matrix propagation for modeling coherent excitation energy transfer in photosynthetic light harvesting

Huo, P., Coker, D. F.·2010·The Journal of Chemical Physics
DOI 10.1063/1.3498901
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Abstract

Rather than incoherent hopping between chromophores, experimental evidence suggests that the excitation energy transfer in some biological light harvesting systems initially occurs coherently, and involves coherent superposition states in which excitation spreads over multiple chromophores separated by several nanometers. Treating such delocalized coherent superposition states in the presence of decoherence and dissipation arising from coupling to an environment is a significant challenge for conventional theoretical tools that either use a perturbative approach or make the Markovian approximation. In this paper, we extend the recently developed iterative linearized density matrix (ILDM) propagation scheme [E. R. Dunkel et al., J. Chem. Phys. 129, 114106 (2008)] to study coherent excitation energy transfer in a model of the Fenna–Matthews–Olsen light harvesting complex from green sulfur bacteria. This approach is nonperturbative and uses a discrete path integral description employing a short time approximation to the density matrix propagator that accounts for interference between forward and backward paths of the quantum excitonic system while linearizing the phase in the difference between the forward and backward paths of the environmental degrees of freedom resulting in a classical-like treatment of these variables. The approach avoids making the Markovian approximation and we demonstrate that it successfully describes the coherent beating of the site populations on different chromophores and gives good agreement with other methods that have been developed recently for going beyond the usual approximations, thus providing a new reliable theoretical tool to study coherent exciton transfer in light harvesting systems. We conclude with a discussion of decoherence in independent bilinearly coupled harmonic chromophore baths. The ILDM propagation approach in principle can be applied to more general descriptions of the environment.

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Crossref · 10.1063/1.3498901

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  • Non-equilibrium exchanges between system and environment can have considerable influence on the system dynamics.

    “This and other non-equilibrium exchanges between system and environment can have considerable influence on the system dynamics [28-35], influence the direction of energy transfer [28] and may even lead to the generation of long-lived quantum coherence in the system [28, 36-38].”

    From Vibrations, quanta and biology (2013) · cites this paper as [32]

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Authors
Huo, P., & Coker, D. F.
Affiliations
  • Boston University (US)
  • University College Dublin (IE)
ORCID
Venue
The Journal of Chemical Physics
Publisher
AIP Publishing
Published
2010-11-11
Volume
133
Issue
18
Pages
184108-184108
ISSN
  • 0021-9606 (ISSN-L)
  • 1089-7690
DOI
10.1063/1.3498901
OpenAlex
W1974038814
Cited by
134
References
68
Citations by year
2026: 2 · 2025: 2 · 2024: 7 · 2023: 3 · 2022: 5 · 2021: 8 · 2020: 11 · 2019: 5 · 2018: 2 · 2017: 5 · 2016: 7 · 2015: 12 · 2014: 14 · 2013: 14 · 2012: 23
FWCI
8.75
Type
journal article
Language
en
Open access
closed
Locations
  • The Journal of Chemical Physics (publishedVersion)
  • PubMed (publishedVersion)
Topics
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
  • Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Strong Light-Matter Interactions
Keywords
photosynthetic light harvesting, green sulfur bacteria, decoherence, energy dissipation, coherent superposition states, exciton delocalization
MeSH terms
Energy Transfer, Markov Chains, Models, Chemical, Monte Carlo Method, Quantum Theory, Chlorobi, Photosynthetic Reaction Center Complex Proteins, Molecular Dynamics Simulation

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