Intra- and interband transfers in the B800-B850 antenna of Rhodospirillum molischianum Redfield theory modeling of polarized pump-probe kinetics

Intra- and interband transfers in the B800-B850 antenna of Rhodospirillum molischianum Redfield theory modeling of polarized pump-probe kinetics
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莫里什红螺菌 B800-B850 天线的带内和带间传输 极化泵浦探针动力学的 Redfield 理论建模

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发表时间:
2003
期刊:
影响因子:
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通讯作者:
R. Grondelle
R. Grondelle
中科院分区:
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文献类型:
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作者:
V. Novoderezhkin;and Markus Wendling;R. Grondelle

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我们使用 Molischianum 红螺菌 B800−B850 LH2 光捕获天线的激子模型来解释吸收、激发波长相关的泵浦探针动力学以及先前报道的 77 K 处的诱导吸收各向异性(Wendling, M.; van Mourik, F.; van Stokkum, I. H. M.; Salverda, J. M.; 米歇尔,H.; van Grondelle, R. 对莫里斯红螺菌 B800 波段的低强度泵浦探针测量。生物物理学。 J. 2003, 84, 440)。使用密度矩阵方程计算非线性响应,相对于外场扩展到三阶,并在激子基础上使用 Redfield 弛豫算子。该模型使我们能够获得数据的同步定量拟合,同时考虑到激子相互作用、静态无序以及声子引起的布居弛豫和单激子流形中的相干性(包括非长期相干转移和布居相干耦合)。激子-光子的谱密度...
We use an exciton model for the B800−B850 LH2 light-harvesting antenna of Rhodospirillum molischianum to explain the absorption, excitation-wavelength-dependent pump−probe kinetics, and induced absorption anisotropy at 77 K reported previously (Wendling, M.; van Mourik, F.; van Stokkum, I. H. M.; Salverda, J. M.; Michel, H.; van Grondelle, R. Low-intensity pump−probe measurements on the B800 band of Rhodospirillum molischianum. Biophys. J. 2003, 84, 440). The nonlinear response was calculated using the density matrix equation, expanded up to the third-order with respect to the external field, with the Redfield relaxation operator in the exciton basis. The model allowed us to obtain a simultaneous and quantitative fit of the data while taking into account the excitonic interactions, the static disorder, and phonon-induced relaxation of populations and coherences in the one-exciton manifold (including a nonsecular coherence transfer and population-coherence coupling). The spectral density of the exciton−pho...