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Title: Dynamics of a Chlorophyll Dimer in Collective and Local Thermal Environments

Abstract

Here we present a theoretical analysis of exciton transfer and decoherence effects in a photosynthetic dimer interacting with collective (correlated) and local (uncorrelated) protein-solvent environments. Our approach is based on the framework of the spin-boson model. We derive explicitly the thermal relaxation and decoherence rates of the exciton transfer process, valid for arbitrary temperatures and for arbitrary (in particular, large) interaction constants between the dimer and the environments. We establish a generalization of the Marcus formula, giving reaction rates for dimer levels possibly individually and asymmetrically coupled to environments. We identify rigorously parameter regimes for the validity of the generalized Marcus formula. The existence of long living quantum coherences at ambient temperatures emerges naturally from our approach.

Authors:
 [1];  [2];  [3];  [2];  [4];  [5];  [6]
  1. Memorial Univ. of Newfoundland, St. John’s, NL (Canada). Dept. of Mathematics and Statistics
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Biological Division
  4. Memorial Univ. of Newfoundland, St. Johnas, NL (Canada). Dept. of Mathematics and Statistics; Univ. Stuttgart, Stuttgart (Germany). Fachbereich Mathematik
  5. CUCEI: Universidad de Guadalajara
  6. Tianjin University of Technology
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1338732
Report Number(s):
LA-UR-15-29509
Journal ID: ISSN 0259-9791
Grant/Contract Number:  
AC52-06NA25396; 15349
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Mathematical Chemistry
Additional Journal Information:
Journal Volume: 54; Journal Issue: 4; Journal ID: ISSN 0259-9791
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 54 ENVIRONMENTAL SCIENCES; Biological Science; Light-harvesting photosynthetic complex; Photosynthetic dimer; Exciton transfer; Transfer rate; Relaxation rate; Decoherence rate; Marcus formula; Local environment; Collective environment; Strong environment coupling; Open quantum systems; Dynamical quantum resonance theory

Citation Formats

Merkli, M., Berman, Gennady Petrovich, Sayre, Richard Thomas, Gnanakaran, Sandrasegaram, Konenberg, M., Nesterov, A.I., and Song, H.. Dynamics of a Chlorophyll Dimer in Collective and Local Thermal Environments. United States: N. p., 2016. Web. https://doi.org/10.1007/s10910-016-0593-z.
Merkli, M., Berman, Gennady Petrovich, Sayre, Richard Thomas, Gnanakaran, Sandrasegaram, Konenberg, M., Nesterov, A.I., & Song, H.. Dynamics of a Chlorophyll Dimer in Collective and Local Thermal Environments. United States. https://doi.org/10.1007/s10910-016-0593-z
Merkli, M., Berman, Gennady Petrovich, Sayre, Richard Thomas, Gnanakaran, Sandrasegaram, Konenberg, M., Nesterov, A.I., and Song, H.. Sat . "Dynamics of a Chlorophyll Dimer in Collective and Local Thermal Environments". United States. https://doi.org/10.1007/s10910-016-0593-z. https://www.osti.gov/servlets/purl/1338732.
@article{osti_1338732,
title = {Dynamics of a Chlorophyll Dimer in Collective and Local Thermal Environments},
author = {Merkli, M. and Berman, Gennady Petrovich and Sayre, Richard Thomas and Gnanakaran, Sandrasegaram and Konenberg, M. and Nesterov, A.I. and Song, H.},
abstractNote = {Here we present a theoretical analysis of exciton transfer and decoherence effects in a photosynthetic dimer interacting with collective (correlated) and local (uncorrelated) protein-solvent environments. Our approach is based on the framework of the spin-boson model. We derive explicitly the thermal relaxation and decoherence rates of the exciton transfer process, valid for arbitrary temperatures and for arbitrary (in particular, large) interaction constants between the dimer and the environments. We establish a generalization of the Marcus formula, giving reaction rates for dimer levels possibly individually and asymmetrically coupled to environments. We identify rigorously parameter regimes for the validity of the generalized Marcus formula. The existence of long living quantum coherences at ambient temperatures emerges naturally from our approach.},
doi = {10.1007/s10910-016-0593-z},
journal = {Journal of Mathematical Chemistry},
number = 4,
volume = 54,
place = {United States},
year = {2016},
month = {1}
}

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