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二维瞬态光谱的全局动力学分析揭示了紫色细菌光捕获复合物中的能量转移途径。

Energy transfer pathways in light-harvesting complexes of purple bacteria as revealed by global kinetic analysis of two-dimensional transient spectra.

机构信息

Department of Chemistry, University of Toronto , 80 St. George Street, Toronto, Ontario, M5S 3H6, Canada.

出版信息

J Phys Chem B. 2013 Sep 26;117(38):11349-62. doi: 10.1021/jp403028x. Epub 2013 Jul 18.

DOI:10.1021/jp403028x
PMID:23865801
Abstract

Excited state dynamics in LH2 complexes of two purple bacterial species were studied by broad-band two-dimensional electronic spectroscopy. The optical response was measured in the 500-600 nm spectral region on the 0-400 fs time scale. Global target analysis of two-dimensional (2D) transient spectra revealed the main energy transfer pathways between carotenoid S2, 1Bu(-) and S1 states and bacteriochlorophyll Qx state. Global analysis ascertained the evolutionary and vibration-associated spectra, which also indicated the presence of a higher-lying vibrational level in the carotenoid S1 state. The estimation of the spectral overlap between the 1Bu(-) state and the Qx state indicated a significant contribution of the 1Bu(-) state to the overall S2-to-Qx excitation energy transfer.

摘要

通过宽带二维电子光谱研究了两种紫色细菌 LH2 复合物的激发态动力学。在 0-400 fs 的时间尺度上,在 500-600nm 的光谱区域测量了光响应。二维(2D)瞬态光谱的全局目标分析揭示了类胡萝卜素 S2、1Bu(-) 和 S1 态与细菌叶绿素 Qx 态之间的主要能量转移途径。全局分析确定了进化和振动相关的光谱,这也表明类胡萝卜素 S1 态中存在更高的振动能级。对 1Bu(-)态和 Qx 态之间的光谱重叠的估计表明,1Bu(-)态对 S2 到 Qx 激发能量转移的整体贡献显著。

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