Dynamics of the mixed exciton and charge-transfer states in light-harvesting complex Lhca4: Hierarchical equation approach

Vladimir I. Novoderezhkin, Roberta Croce, Rienk van Grondelle

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

We model the energy transfer dynamics in the Lhca4 peripheral antenna of photosystem I from higher plants. Equilibration between the bulk exciton levels of the antenna and the red-shifted charge-transfer (CT) states is described using the numerically inexpensive Redfield-Förster approach and exact hierarchical equation (HEOM) method. We propose a compartmentalization scheme allowing a quantitatively correct description of the dynamics with the Redfield-Förster theory, including the exciton-type relaxation within strongly coupled compartments and hopping-type migration between them. The Redfield-Förster method gives the kinetics close to the HEOM solution when treating the CT state as dynamically localized. We also demonstrate that the excited states strongly coupled with the CT should be considered as localized as well.

Original languageEnglish
Pages (from-to)655-665
Number of pages11
JournalBiochimica et Biophysica Acta - Bioenergetics
Volume1859
Issue number9
Early online date5 Jul 2018
DOIs
Publication statusPublished - Sep 2018

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Charge transfer
Photosystem I Protein Complex
Light
Energy Transfer
Antennas
Excited states
Energy transfer
Kinetics
LDS 751
HEOM

Keywords

  • Charge-transfer states
  • Exciton states
  • Förster theory
  • Hierarchical equation of motion
  • Lhca4
  • Light-harvesting complex
  • Redfield theory

Cite this

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abstract = "We model the energy transfer dynamics in the Lhca4 peripheral antenna of photosystem I from higher plants. Equilibration between the bulk exciton levels of the antenna and the red-shifted charge-transfer (CT) states is described using the numerically inexpensive Redfield-F{\"o}rster approach and exact hierarchical equation (HEOM) method. We propose a compartmentalization scheme allowing a quantitatively correct description of the dynamics with the Redfield-F{\"o}rster theory, including the exciton-type relaxation within strongly coupled compartments and hopping-type migration between them. The Redfield-F{\"o}rster method gives the kinetics close to the HEOM solution when treating the CT state as dynamically localized. We also demonstrate that the excited states strongly coupled with the CT should be considered as localized as well.",
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Dynamics of the mixed exciton and charge-transfer states in light-harvesting complex Lhca4 : Hierarchical equation approach. / Novoderezhkin, Vladimir I.; Croce, Roberta; van Grondelle, Rienk.

In: Biochimica et Biophysica Acta - Bioenergetics, Vol. 1859, No. 9, 09.2018, p. 655-665.

Research output: Contribution to JournalArticleAcademicpeer-review

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T1 - Dynamics of the mixed exciton and charge-transfer states in light-harvesting complex Lhca4

T2 - Hierarchical equation approach

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