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Linear and Nonlinear Spectra in Photosynthetic Light Harvesting Complexes: Benchmark Tests of Modi ed Red eld Method
Yuan-yuan Jing,Kai Song,Shu-ming Bai,Qiang Shi*
Author NameAffiliationE-mail
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  
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  
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  
Qiang Shi* 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 qshi@iccas.ac.cn 
Abstract:
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.
Key words:  Linear spectra, Nonlinear spectra, Light harvesting complexes, Modified Redfield method
FundProject:
光合作用体系捕光复合物线性和非线性光谱的理论研究:修正的Redfield方法的验证
景圆圆,宋凯,白书明,史强*
摘要:
使用数值精确的级联方程方法对其计算可靠性进行了验证.目前已知,修正的Redfield方法所用的微扰和马尔科夫近似,在中间耦合区对激发态能量转移会给出不正确的描述.因此研究其在计算各 种光谱信号时是否仍然有效有重要意义.利用不同参数下的二聚体模型和Fenna-Matthews-Olson复合物模型,使用级联方程方法和修正的Redfield方法,计算并比较了它们的吸收谱、发射谱和二维电子相干光谱.研究发现在较大的参数范围内两种方法给出一致的结果,这两种方法的对比也增进了对光合作用捕光复合物的2D光谱中量子拍频信号来源的认识.
关键词:  光合作用体系,捕光复合物,光谱,修正的Redfield方法
DOI:10.1063/1674-0068/28/cjcp1506126
分类号: