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*

*Corresponding author for this work

Research output: Contribution to JournalArticleAcademicpeer-review

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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-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 - Sept 2018

Funding

V.N. was supported by the Russian Foundation for Basic Research (Grant No. 18-04-00105 ). R.C. was supported by the Foundation for Fundamental Research on Matter (FOM) and by the European Research Council via the ERC consolidator grant ASAP ( 281341 ). R. v. G. was supported by the VU University Amsterdam , the Laserlab-Europe Consortium , the TOP grant ( 700.58.305 ) from the Foundation of Chemical Sciences part of NWO , the advanced investigator grant ( 267333 , PHOTPROT) from the European Research Council , and by the EU FP7 project PAPETS ( GA 323901 ), and by his Academy Professor grant from the Netherlands Royal Academy of Sciences ( KNAW ).

FundersFunder number
EU FP7
Laserlab-Europe Consortium
Netherlands Royal Academy of Sciences
PHOTPROT
European Research Council281341
Stichting voor Fundamenteel Onderzoek der Materie
Koninklijke Nederlandse Akademie van Wetenschappen
Vrije Universiteit Amsterdam
Russian Foundation for Basic Research18-04-00105
Nederlandse Organisatie voor Wetenschappelijk Onderzoek267333, 700.58.305
Foundation for Fundamental Research on Matter
Seventh Framework ProgrammeGA 323901

    Keywords

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

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