We challenge the misconception that Bloch-Redfield equations are a less powerful tool than phenomenological Lindblad equations for modeling exciton transport in photosynthetic complexes. This view predominantly originates from an indiscriminate use of the secular approximation. We provide a detailed description of how to model both coherent oscillations and several types of noise, giving explicit examples. All issues with non-positivity are overcome by a consistent straightforward physical noise model. Herein also lies the strength of the Bloch-Redfield approach because it facilitates the analysis of noise-effects by linking them back to physical parameters of the noise environment. This includes temporal and spatial correlations and the strength and type of interaction between the noise and the system of interest. Finally, we analyze a prototypical dimer system as well as a 7-site Fenna-Matthews-Olson complex in regards to spatial correlation length of the noise, noise strength, temperature, and their connection to the transfer time and transfer probability.
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14 February 2015
Research Article|
February 10 2015
Bloch-Redfield equations for modeling light-harvesting complexes
Jan Jeske;
Jan Jeske
1Chemical and Quantum Physics, School of Applied Sciences,
RMIT University
, Melbourne 3001, Australia
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David J. Ing;
David J. Ing
1Chemical and Quantum Physics, School of Applied Sciences,
RMIT University
, Melbourne 3001, Australia
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Martin B. Plenio;
Martin B. Plenio
2Institut für Theoretische Physik, Albert-Einstein-Allee 11,
Universität Ulm
, D-89069 Ulm, Germany
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Susana F. Huelga;
Susana F. Huelga
2Institut für Theoretische Physik, Albert-Einstein-Allee 11,
Universität Ulm
, D-89069 Ulm, Germany
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Jared H. Cole
Jared H. Cole
1Chemical and Quantum Physics, School of Applied Sciences,
RMIT University
, Melbourne 3001, Australia
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J. Chem. Phys. 142, 064104 (2015)
Article history
Received:
August 05 2014
Accepted:
January 21 2015
Citation
Jan Jeske, David J. Ing, Martin B. Plenio, Susana F. Huelga, Jared H. Cole; Bloch-Redfield equations for modeling light-harvesting complexes. J. Chem. Phys. 14 February 2015; 142 (6): 064104. https://doi.org/10.1063/1.4907370
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