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 language | English |
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Pages (from-to) | 655-665 |
Number of pages | 11 |
Journal | Biochimica et Biophysica Acta - Bioenergetics |
Volume | 1859 |
Issue number | 9 |
Early online date | 5 Jul 2018 |
DOIs | |
Publication status | Published - 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 ).
Funders | Funder number |
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EU FP7 | |
Laserlab-Europe Consortium | |
Netherlands Royal Academy of Sciences | |
PHOTPROT | |
European Research Council | 281341 |
Stichting voor Fundamenteel Onderzoek der Materie | |
Koninklijke Nederlandse Akademie van Wetenschappen | |
Vrije Universiteit Amsterdam | |
Russian Foundation for Basic Research | 18-04-00105 |
Nederlandse Organisatie voor Wetenschappelijk Onderzoek | 267333, 700.58.305 |
Foundation for Fundamental Research on Matter | |
Seventh Framework Programme | GA 323901 |
Keywords
- Charge-transfer states
- Exciton states
- Förster theory
- Hierarchical equation of motion
- Lhca4
- Light-harvesting complex
- Redfield theory