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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >A Proposed Method to Obtain Surface Specificity with Pump-Probe and 2D Spectroscopies
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A Proposed Method to Obtain Surface Specificity with Pump-Probe and 2D Spectroscopies

机译：提出的方法以泵探针和2D光谱获得表面特异性

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摘要

Surfaces and interfaces are ubiquitous in nature. From cell membranes, to photovoltaic thin films, surfaces have important function in both biological and materials systems. Spectroscopic techniques have been developed to probe systems like these, such as sum frequency generation (SFG) spectroscopies. The advantage of SFG spectroscopy, a second-order spectroscopy, is that it can distinguish between signals produced from molecules in the bulk versus on the surface. We propose a polarization scheme for third-order spectroscopy experiments, such as pump-probe and 2D spectroscopy, to select for surface signals and not bulk signals. This proposed polarization condition uses one pulse perpendicular compared to the other three to isolate cross-peaks arising from molecules with polar and uniaxial (i.e., biaxial) order at a surface, while removing the signal from bulk isotropic molecules. In this work, we focus on two of these cases: XXXY and YYYX, which differ by the sign of the cross-peak they create. We compare this technique to SFG spectroscopy and vibrational circular dichroism to provide insight to the behavior of the cross-peak signal. We propose that these singularly cross- polarized schemes provide odd-ordered spectroscopies the surface-specificity typically associated with even-ordered techniques.
机译：表面和界面在自然界中普遍存在。从细胞膜，到光伏薄膜，表面在两个生物和材料系统中具有重要的功能。已经开发了光谱技术，用于探测器系统，例如和频率产生（SFG）光谱。 SFG光谱法，二阶光谱学的优点是它可以区分从散装与表面上的分子产生的信号。我们提出了一种用于三阶光谱实验的偏振方案，例如泵探针和2D光谱，以选择表面信号而不是批量信号。与其他三个相比，该提出的偏振条件使用一个脉冲垂直，以分离在表面处的极性和单轴（即双轴）顺序产生的横峰，同时从散装各向同性分子中除去信号。在这项工作中，我们专注于其中的两个案例：XXXY和YYYX，它因他们创造的跨峰的标志而异。我们将该技术与SFG光谱和振动圆形二色性的比较，为交叉峰值信号的行为提供了洞察。我们提出这些奇异的交叉极化方案提供奇数有序的光谱仪，所述表面特异性通常与偶令技术相关联。

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