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首页> 外文期刊>The Journal of Chemical Physics >Four-dimensional coherent electronic Raman spectroscopy
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Four-dimensional coherent electronic Raman spectroscopy

机译：四维相干电子拉曼光谱

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摘要

The correlations between different quantum-mechanical degrees of freedom of molecular species dictate their chemical and physical properties. Generally, these correlations are reflected in the optical response of the system but in low-order or low-dimensionality measurement the signals are highly averaged. Here, we describe a novel four-dimensional coherent spectroscopic method that directly correlates within and between the manifold of electronic and vibrational states. The optical response theory is developed in terms of both resonant and non-resonant field-matter interactions. Using resonance to select coherences on specific electronic states creates opportunities to directly distinguish coherent dynamics on the ground and electronically excited potentials. Critically, this method is free from lower-order signals that have plagued other electronically non-resonant vibrational spectroscopies. The theory presented here compliments recent work on the experimental demonstration of the 4D spectroscopic method described. We highlight specific means by which non-trivial effects such as anharmonicity (diagonal and off-diagonal), mode-specific vibronic coupling, and curvature of the excited states manifest in different projections of the 4D spectrum. Published by AIP Publishing.
机译：不同量子机械分子物种自由度之间的相关性决定了它们的化学和物理性质。通常，这些相关性反映在系统的光学响应中，但是以低阶或低维度测量，信号高度平均。这里，我们描述了一种新的四维相干光谱方法，其直接相关在电子和振动状态的歧管内和之间。在谐振和非共振场 - 物质相互作用方面开发了光学响应理论。利用谐振选择特定电子国家的一致性，会产生直接区分地面和电子兴奋电位的相干动态的机会。批判性地，该方法没有损坏其他电子非共振振动谱的低位信号。这里介绍了近期关于所描述的4D光谱法的实验证明的工作的恭维。我们突出了特定的方法，通过其中诸如Anharmonicity（对角线和非对角线），模式特定的振动耦合和在4D光谱的不同投影中突出的兴奋状态的抗谐波耦合和曲率。通过AIP发布发布。

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