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首页> 美国卫生研究院文献>Proceedings of the National Academy of Sciences of the United States of America >Multidimensional Ultrafast Spectroscopy Special Feature: Cross-peak-specific two-dimensional electronic spectroscopy
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Multidimensional Ultrafast Spectroscopy Special Feature: Cross-peak-specific two-dimensional electronic spectroscopy

机译：多维超快光谱学特色：跨峰专用二维电子光谱学

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摘要

Intermolecular electronic coupling dictates the optical properties of molecular aggregate systems. Of particular interest are photosynthetic pigment–protein complexes that absorb sunlight then efficiently direct energy toward the photosynthetic reaction center. Two-dimensional (2D) ultrafast spectroscopy has been used widely in the infrared (IR) and increasingly in the visible to probe excitonic couplings and observe dynamics, but the off-diagonal spectral signatures of coupling are often obscured by broad diagonal peaks, especially in the visible regime. Rotating the polarizations of the laser pulses exciting the sample can highlight certain spectral features, and the use of polarized pulse sequences to elucidate cross-peaks in 2D spectra has been demonstrated in the IR for vibrational transitions. Here we develop 2D electronic spectroscopy using cross-peak-specific pulse polarization conditions in an investigation of the Fenna–Matthews–Olson light harvesting complex from green photosynthetic bacteria. Our measurements successfully highlight off-diagonal features of the 2D spectra and, in combination with an analysis based on the signs of features arising from particular energy level pathways and theoretical simulation, we characterize the dominant response pathways responsible for the spectral features. Cross-peak-specific 2D electronic spectroscopy provides insight into the interchromophore couplings, as well as into the energetic pathways giving rise to the signal. With femtosecond resolution, we also observe dynamical processes that depend on these couplings and interactions with the protein environment.
机译：分子间电子耦合决定了分子聚集体系统的光学性质。特别令人感兴趣的是光合色素-蛋白质复合物，该复合物吸收阳光，然后将能量有效地引向光合反应中心。二维（2D）超快光谱已广泛用于红外（IR）中，并越来越多地用于可见光中以探测激子耦合并观察动力学，但耦合的非对角光谱特征通常被宽的对角峰所遮盖，特别是在可见的政权。旋转激发样品的激光脉冲的偏振可以突出某些光谱特征，并且红外中已证明使用偏振脉冲序列来阐明2D光谱中的交叉峰，可以实现振动跃迁。在这里，我们研究了跨峰特定脉冲极化条件下的2D电子光谱，用于研究绿色光合细菌中的Fenna-Matthews-Olson集光复合体。我们的测量成功地突出了2D光谱的非对角线特征，并结合了基于特定能级路径和理论模拟得出的特征符号的分析，从而确定了导致光谱特征的主要响应路径。跨峰特定的2D电子光谱学提供了对发色团间偶联以及产生信号的高能途径的洞察力。在飞秒分辨率下，我们还观察到了取决于这些耦合以及与蛋白质环境相互作用的动力学过程。

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