We apply the Liouville space hierarchical equations of motion method to calculate the linear and two-dimensional (2D) electronic spectra of the Fenna-Matthews-Olson (FMO) protein complex from Chlorobium tepidum, using a widely used model Hamiltonian. The absorption and linear dichroism spectra of the FMO complex, as well as the main features of the 2D spectra are well reproduced. However, comparison with the recent experimental 2D spectra reveals several limitations of the current model: (1) The homogeneous and inhomogeneous broadening seems to be overestimated for the first exciton peak, but may be underestimated for several other exciton peaks. (2) The calculated oscillations of the diagonal and off-diagonal peaks in the 2D spectra are much weaker than the experimental observations, which indicates that an improved model is needed for the excitonic dynamics of the FMO complex.
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21 May 2011
Research Article|
May 19 2011
Simulation of the two-dimensional electronic spectra of the Fenna-Matthews-Olson complex using the hierarchical equations of motion method
Liping Chen;
Liping Chen
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry,
Chinese Academy of Sciences
, Zhongguancun, Beijing 100190, China
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Renhui Zheng;
Renhui Zheng
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry,
Chinese Academy of Sciences
, Zhongguancun, Beijing 100190, China
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Yuanyuan Jing;
Yuanyuan Jing
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry,
Chinese Academy of Sciences
, Zhongguancun, Beijing 100190, China
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a)
Author to whom correspondence should be addressed. Electronic mail: [email protected].
J. Chem. Phys. 134, 194508 (2011)
Article history
Received:
October 15 2010
Accepted:
April 21 2011
Citation
Liping Chen, Renhui Zheng, Yuanyuan Jing, Qiang Shi; Simulation of the two-dimensional electronic spectra of the Fenna-Matthews-Olson complex using the hierarchical equations of motion method. J. Chem. Phys. 21 May 2011; 134 (19): 194508. https://doi.org/10.1063/1.3589982
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