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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Determination of Surface Preference Using Heterospectral Surface-Bulk Correlation Spectroscopy
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Determination of Surface Preference Using Heterospectral Surface-Bulk Correlation Spectroscopy

机译：使用异晶体表面堆积相关光谱法测定表面偏好

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摘要

We outline a method by which the surface preference of a species in a multicomponent mixture may be obtained using surface-specific visible-infrared sum frequency generation (SFG) spectroscopy combined with bulk infrared absorption and/or Raman data. In general, the problem is complicated by the fact that the SFG signal is a function of both the surface coverage and the structure of the molecules. Two-dimensional correlation analysis can be used to reveal which spectral features are changing synchronously, that is, in phase with each other, and which ones are evolving in a manner that is phase-shifted by 90 degrees (asynchronous correlation) as a function of the bulk composition. We provide a framework for determining the surface preference from the correlations between the vibrational modes in the SFG spectra and between the modes from SFG and bulk infrared and/or Raman spectra. When compared to the equivalent analysis performed using the SFG spectra alone, this method can be used with the data obtained using a single-beam polarization and in congested spectral regions where fitting to isolate the behavior of individual vibrational modes is not robust.
机译：我们概述了一种方法，通过该方法，可以使用与散装红外吸收和/或拉曼数据结合的表面特异性可见红外和频率产生（SFG）光谱来获得多组分混合物中物种的表面偏好。通常，问题的情况是SFG信号是表面覆盖的函数和分子的结构的函数。二维相关性分析可用于揭示哪些频谱特征是同步改变的，即相位彼此相位，并且哪些是以相移为90度（异步相关性）的方式发展散装组成。我们提供了一种用于确定表面偏好从SFG光谱中的振动模式和来自SFG和散装红外线和/或拉曼光谱之间的模式之间的相关性的框架。与单独使用SFG光谱执行的等效分析相比，该方法可以与使用单束偏振的数据和拥挤的光谱区域一起使用，其中拟合隔离单独振动模式的行为是不稳健的。

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