Cited by 430Spectroscopy and Quantum Chemical StudiesPhotochemistry and Electron Transfer StudiesStrong Light-Matter Interactions

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On the adequacy of the Redfield equation and related approaches to the study of quantum dynamics in electronic energy transfer

Ishizaki, Akihito, Fleming, Graham R.·2009·The Journal of Chemical Physics

DOI 10.1063/1.3155214

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Abstract

The observation of long-lived electronic coherence in photosynthetic excitation energy transfer (EET) by Engel et al. [Nature (London) 446, 782 (2007)] raises questions about the role of the protein environment in protecting this coherence and the significance of the quantum coherence in light harvesting efficiency. In this paper we explore the applicability of the Redfield equation in its full form, in the secular approximation and with neglect of the imaginary part of the relaxation terms for the study of these phenomena. We find that none of the methods can give a reliable picture of the role of the environment in photosynthetic EET. In particular the popular secular approximation (or the corresponding Lindblad equation) produces anomalous behavior in the incoherent transfer region leading to overestimation of the contribution of environment-assisted transfer. The full Redfield expression on the other hand produces environment-independent dynamics in the large reorganization energy region. A companion paper presents an improved approach, which corrects these deficiencies [A. Ishizaki and G. R. Fleming, J. Chem. Phys. 130, 234111 (2009)].

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Authors: Ishizaki, A., & Fleming, G. R.
Affiliations: Lawrence Berkeley National Laboratory (US)
ORCID: Ishizaki, Akihito
Fleming, Graham R.
Venue: The Journal of Chemical Physics
Publisher: AIP Publishing
Published: 2009-06-18
Volume: 130
Issue: 23
Pages: 234110-234110
ISSN: 0021-9606 (ISSN-L)
1089-7690
DOI: 10.1063/1.3155214
OpenAlex: W2009237413
Cited by: 430
References: 60
Citations by year: 2026: 15 · 2025: 19 · 2024: 18 · 2023: 9 · 2022: 21 · 2021: 17 · 2020: 21 · 2019: 32 · 2018: 19 · 2017: 23 · 2016: 22 · 2015: 31 · 2014: 36 · 2013: 25 · 2012: 39
FWCI: 22.64
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: Redfield equation, excitation energy transfer, photosynthetic light harvesting, quantum coherence, secular approximation, Lindblad master equation, reorganization energy, protein environment, quantum dynamics
MeSH terms: Computer Simulation, Electrons, Energy Transfer, Models, Chemical, Quantum Theory

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On the adequacy of the Redfield equation and related approaches to the study of quantum dynamics in electronic energy transfer

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