On the initial charge separation in bacterial reaction centers: Long-range electron transfer via an exciton-charge transfer (ECT) coupling mechanism

P. O.J. Scherer; Sighart F. Fischer

doi:10.1016/0009-2614(87)85005-4

On the initial charge separation in bacterial reaction centers: Long-range electron transfer via an exciton-charge transfer (ECT) coupling mechanism

P. O.J. Scherer, Sighart F. Fischer

TUM Emeriti of Excellence

Technical University of Munich

Research output: Contribution to journal › Article › peer-review

28 Scopus citations

Abstract

The low-lying electronically excited states for the reaction center of Rps. viridis are investigated using PPP/CI calculations. The six pigments are treated as three interacting pairs, the symmetric special pair dimer BC_MPBC_LP and the two loosely coupledasymmetric dimers BC_LABP_L and BC_MABP_M. It is shown that the charge transfer state BC_LA⁺BP_L^- can fall below the special pair excitation P* due to partial charge transfer from a histidine to BC_LA and due to stabilization of BP_L^- by a glutamic acid residue. As a result P* can decay in 2.8 ps into BC_LA⁺BP_L^- which goes over into the radical pair P⁺ BP_L^- in less than 1 ps. The first step can be described as an excitonic interaction between P* and BC_LA⁺ BP_L^-.

Original language	English
Pages (from-to)	179-185
Number of pages	7
Journal	Chemical Physics Letters
Volume	141
Issue number	3
DOIs	https://doi.org/10.1016/0009-2614(87)85005-4
State	Published - 6 Nov 1987

Access to Document

10.1016/0009-2614(87)85005-4

Cite this

@article{c5d7e80219f5484885df18896c47778d,

title = "On the initial charge separation in bacterial reaction centers: Long-range electron transfer via an exciton-charge transfer (ECT) coupling mechanism",

abstract = "The low-lying electronically excited states for the reaction center of Rps. viridis are investigated using PPP/CI calculations. The six pigments are treated as three interacting pairs, the symmetric special pair dimer BCMPBCLP and the two loosely coupledasymmetric dimers BCLABPL and BCMABPM. It is shown that the charge transfer state BCLA+BPL- can fall below the special pair excitation P* due to partial charge transfer from a histidine to BCLA and due to stabilization of BPL- by a glutamic acid residue. As a result P* can decay in 2.8 ps into BCLA+BPL- which goes over into the radical pair P+ BPL- in less than 1 ps. The first step can be described as an excitonic interaction between P* and BCLA+ BPL-.",

author = "Scherer, {P. O.J.} and Fischer, {Sighart F.}",

note = "Funding Information: The authors thank Dr. H.P. Braun for the experimental absorption spectra of Rb. sphaeroides and Dr. E.W. Knapp for stimulating discussions. This work was supported by the Deutsche Forschungs-gemeinschaft SFB 143C.",

year = "1987",

month = nov,

day = "6",

doi = "10.1016/0009-2614(87)85005-4",

language = "English",

volume = "141",

pages = "179--185",

journal = "Chemical Physics Letters",

issn = "0009-2614",

publisher = "Elsevier B.V.",

number = "3",

}

TY - JOUR

T1 - On the initial charge separation in bacterial reaction centers

T2 - Long-range electron transfer via an exciton-charge transfer (ECT) coupling mechanism

AU - Scherer, P. O.J.

AU - Fischer, Sighart F.

N1 - Funding Information: The authors thank Dr. H.P. Braun for the experimental absorption spectra of Rb. sphaeroides and Dr. E.W. Knapp for stimulating discussions. This work was supported by the Deutsche Forschungs-gemeinschaft SFB 143C.

PY - 1987/11/6

Y1 - 1987/11/6

N2 - The low-lying electronically excited states for the reaction center of Rps. viridis are investigated using PPP/CI calculations. The six pigments are treated as three interacting pairs, the symmetric special pair dimer BCMPBCLP and the two loosely coupledasymmetric dimers BCLABPL and BCMABPM. It is shown that the charge transfer state BCLA+BPL- can fall below the special pair excitation P* due to partial charge transfer from a histidine to BCLA and due to stabilization of BPL- by a glutamic acid residue. As a result P* can decay in 2.8 ps into BCLA+BPL- which goes over into the radical pair P+ BPL- in less than 1 ps. The first step can be described as an excitonic interaction between P* and BCLA+ BPL-.

AB - The low-lying electronically excited states for the reaction center of Rps. viridis are investigated using PPP/CI calculations. The six pigments are treated as three interacting pairs, the symmetric special pair dimer BCMPBCLP and the two loosely coupledasymmetric dimers BCLABPL and BCMABPM. It is shown that the charge transfer state BCLA+BPL- can fall below the special pair excitation P* due to partial charge transfer from a histidine to BCLA and due to stabilization of BPL- by a glutamic acid residue. As a result P* can decay in 2.8 ps into BCLA+BPL- which goes over into the radical pair P+ BPL- in less than 1 ps. The first step can be described as an excitonic interaction between P* and BCLA+ BPL-.

UR - http://www.scopus.com/inward/record.url?scp=0002654997&partnerID=8YFLogxK

U2 - 10.1016/0009-2614(87)85005-4

DO - 10.1016/0009-2614(87)85005-4

M3 - Article

AN - SCOPUS:0002654997

SN - 0009-2614

VL - 141

SP - 179

EP - 185

JO - Chemical Physics Letters

JF - Chemical Physics Letters

IS - 3

ER -

On the initial charge separation in bacterial reaction centers: Long-range electron transfer via an exciton-charge transfer (ECT) coupling mechanism

Abstract

Access to Document

Other files and links

Fingerprint

Cite this