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Ultrabroadband 2D electronic spectroscopy as a tool for direct visualization of pathways of energy flow

机译:超宽带2D电子光谱学作为直接可视化能流路径的工具

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Two-dimensional electronic spectroscopy (2DES) has emerged as an incisive tool for mapping out energy relaxation pathways in complex molecular systems by determining correlation maps between the excitation and emission frequencies. Its enhanced spectral as well as temporal resolution offer new insights into coupling and energy transfer between closely-spaced energy states, which are often hidden in a one-dimensional transient spectrum. However, a major drawback of the current 2DES technique is that the spectral window of detection is directly limited to the laser bandwidth used, which leads to an incomplete visualization of the full energy landscape of the system. As a solution to this limitation, we present an ultrabroadband 2DES apparatus utilizing a 8-fs, 185-nm bandwidth supercontinuum that covers the entire visible region. We demonstrate the utility of our setup by measuring the 2D spectra of laser dyes absorbing at different regions of the laser spectrum, and the major light-harvesting complex of spinach.
机译:二维电子光谱(2DES)已成为一种通过确定激发和发射频率之间的相关图来绘制复杂分子系统中能量弛豫途径的敏锐工具。其增强的光谱和时间分辨率为近距离能量状态之间的耦合和能量转移提供了新的见解,这些能量状态通常隐藏在一维瞬态光谱中。但是,当前的2DES技术的主要缺点是检测的光谱窗口直接受限于所使用的激光带宽,这导致系统的整个能量分布图不完整。作为解决此限制的方法,我们提出了一种超宽带2DES装置,该装置利用覆盖整个可见光区域的8-fs,185 nm带宽超连续谱。我们通过测量在激光光谱的不同区域吸收的激光染料的2D光谱以及菠菜的主要光吸收复合物来证明我们的设置的实用性。

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