We employ the numerically exact hierarchical equations of motion (HEOM) method to perform benchmark tests for the popular modified Redfield method in calculating linear and nonlinear spectroscopic signals of molecular aggregates in photosynthetic light harvesting complexes. It is currently well known that the perturbative and Markovian approximations involved in the modified Redfield equation may give inappropriate description of the excitation energy transfer processes in the intermediate coupling regime. An interesting topic is thus to test the validity of the modified Redfield method in calculating various types of spectroscopic signals. By using model dimers with different sets of parameters and a model of the Fenna-Matthews-Olson complex, we calculate and compare the absorption, emission, and 2D spectra using the modified Redfield and HEOM methods. It is found that results from the modified Redfield method agree well with the HEOM ones in a wide range of parameter regimes. The comparison also helps to understand the quantum beating signals in the 2D spectra of the photosynthetic light harvesting complexes.
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August 2015
Research Article|
August 27 2015
Linear and Nonlinear Spectra in Photosynthetic Light Harvesting Complexes: Benchmark Tests of Modified Redfield Method†
Yuan-yuan Jing;
Yuan-yuan 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
, Beijing 100190, China
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Kai Song;
Kai Song
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species,
Institute of Chemistry, Chinese Academy of Sciences
, Beijing 100190, China
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Shu-ming Bai;
Shu-ming Bai
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species,
Institute of Chemistry, Chinese Academy of Sciences
, Beijing 100190, China
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*
Author to whom correspondence should be addressed. E-mail: qshi@iccas.ac.cn
†
Dedicated to Professor Qing-shi Zhu on the occasion of his 70th birthday.
Chin. J. Chem. Phys. 28, 431–439 (2015)
Article history
Received:
June 17 2015
Accepted:
July 13 2015
Citation
Yuan-yuan Jing, Kai Song, Shu-ming Bai, Qiang Shi; Linear and Nonlinear Spectra in Photosynthetic Light Harvesting Complexes: Benchmark Tests of Modified Redfield Method. Chin. J. Chem. Phys. 27 August 2015; 28 (4): 431–439. https://doi.org/10.1063/1674-0068/28/cjcp1506126
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