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Electron Transfer Model for the Electric Field Effect on Quantum Yield of Charge Separation in Bacterial Photosynthetic Reaction Centers

Tanaka, Shigenori and Marcus, R. A. (1997) Electron Transfer Model for the Electric Field Effect on Quantum Yield of Charge Separation in Bacterial Photosynthetic Reaction Centers. Journal of Physical Chemistry B, 101 (25). pp. 5031-5045. ISSN 1089-5647. https://resolver.caltech.edu/CaltechAUTHORS:20150513-153233889

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Abstract

The effect of an electric field on a photoinduced charge separation process is treated theoretically. The system considered is a reaction center (RC) of photosynthetic bacteria, involving an electron transfer (ET) from the electronically excited singlet state of the bacteriochlorophyll dimer (P) to the bacteriopheophytin (H) and quinone (Q). In contrast to formulations which focus only on the forward steps and do not explain the major effect on the quantum yield of P^+Q^- or, in Q-depleted samples, of P^+H^-, the present study includes the effect on the back reactions, an effect which we find to be large. The low-frequency medium and high-frequency intramolecular vibrational modes are included in the calculation of the various ET rates. Recent experimental results on the ET energetics, including the estimated effect of static heterogeneity in RCs, are incorporated. The rate equations for the population densities of distinct states are solved for both oriented and randomly oriented (isotropic) RC samples, and the results are compared with experimental data for the field-induced reduction of the quantum yield of formation of charge-separated state P^+Q^-. A simple (quasi-equilibrium) model calculation illustrates the essential features of this analysis of the electric field effect and compares reasonably well with these numerical results of the more detailed model. The question of the electric field effect on the fluorescence quantum yield is also addressed, and a suggestion is made for consistency with the data on the formation of P^+Q^-.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp9632854DOIArticle
http://pubs.acs.org/doi/abs/10.1021/jp9632854PublisherArticle
ORCID:
AuthorORCID
Marcus, R. A.0000-0001-6547-1469
Additional Information:© 1997 American Chemical Society. Received October 22, 1996; In Final Form April 11, 1997. We thank Yuri Georgievskii, Antonio Hidalgo García, and Xueyu Song for useful discussions and Chao-Ping Hsu, Aseem Mehta, and Bryan Hathorn for their help in the preparation of the manuscript and the figures. S.T. acknowledges the financial support provided by Toshiba Corp. during his stay at the California Institute of Technology. We are indebted to the National Science Foundation and the Office of Naval Research for the support of this research.
Funders:
Funding AgencyGrant Number
Toshiba CorporationUNSPECIFIED
NSFUNSPECIFIED
Office of Naval Research (ONR)UNSPECIFIED
Issue or Number:25
Record Number:CaltechAUTHORS:20150513-153233889
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20150513-153233889
Official Citation:Tanaka, S., & Marcus, R. A. (1997). Electron Transfer Model for the Electric Field Effect on Quantum Yield of Charge Separation in Bacterial Photosynthetic Reaction Centers. The Journal of Physical Chemistry B, 101(25), 5031-5045. doi: 10.1021/jp9632854
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:57512
Collection:CaltechAUTHORS
Deposited By: Joanne McCole
Deposited On:13 May 2015 23:23
Last Modified:22 Nov 2019 09:58

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