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Charge transfer through a cytochrome multiheme chain: Theory and simulation

Burggraf, Fabian and Koslowski, Thorsten (2014) Charge transfer through a cytochrome multiheme chain: Theory and simulation. Biochimica et Biophysica Acta - Bioenergetics, 1837 (1), pp. 186-192. Elsevier. ISSN 0005-2728

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Abstract

We study sequential charge transfer within a chain of four heme cofactors located in the c-type cytochrome subunit of the photoreaction center of Rhodopseudomonas viridis from a theoretical perspective. Molecular dynamics simulations of the thermodynamic integration type are used to compute two key energies of Marcus' theory of charge transfer, the driving force ΔG and the reorganization energy λ. Due to the small exposure of the cofactors to the solvent and to charged amino acids, the outer sphere contribution to the reorganization energy almost vanishes. Interheme effective electronic couplings are estimated using ab initio wave functions and a well-parameterized semiempirical scheme for long-range interactions. From the resulting charge transfer rates, we conclude that at most the two heme molecules closest to themembrane participate in a fast recharging of the photoreaction center, whereas the remaining hemes are likely to have a different function, such as intermediate electron storage. Finally, we suggest means to verify or falsify this hypothesis.

Item URL in elib:https://elib.dlr.de/91890/
Document Type:Article
Title:Charge transfer through a cytochrome multiheme chain: Theory and simulation
Authors:
AuthorsInstitution or Email of AuthorsAuthors ORCID iD
Burggraf, FabianDLRUNSPECIFIED
Koslowski, ThorstenInstitut für Physikalische Chemie 2, Albert-Ludwigs-Universität FreiburgUNSPECIFIED
Date:January 2014
Journal or Publication Title:Biochimica et Biophysica Acta - Bioenergetics
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:1837
Page Range:pp. 186-192
Publisher:Elsevier
Series Name:Biochimica et Biophysica Acta
ISSN:0005-2728
Status:Published
Keywords:Ladungstransfer, Photosynthese, Marcus Theorie, Su-Schrieffer-Heeger Modell, Cytochrom c, Thermodynamische Integration, Häm,
HGF - Research field:Energy
HGF - Program:Efficient Energy Conversion and Use (old)
HGF - Program Themes:Fuel Cells (old)
DLR - Research area:Energy
DLR - Program:E EV - Energy process technology
DLR - Research theme (Project):E - Electrochemical Processes (old)
Location: Stuttgart
Institutes and Institutions:Institute of Engineering Thermodynamics > Electrochemical Energy Technology
Deposited By: Burggraf, Fabian
Deposited On:19 Nov 2014 14:51
Last Modified:19 Nov 2014 14:51

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