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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Adding a dimension to the infrared spectra of interfaces using heterodyne detected 2D sumfrequency generation (HD 2D SFG) spectroscopy
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Adding a dimension to the infrared spectra of interfaces using heterodyne detected 2D sumfrequency generation (HD 2D SFG) spectroscopy

机译：使用外差检测2D和频生成（HD 2D SFG）光谱为界面的红外光谱添加尺寸

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摘要

In the last ten years, two-dimensional infrared spectroscopy has become an important technique for studying molecular structures and dynamics. We report the implementation of heterodyne detected two-dimensional sum-frequency generation (HD 2D SFG) spectroscopy, which is the analog of 2D infrared (2D IR) spectroscopy, but is selective to noncentrosymmetric systems such as interfaces. We implement the technique using mid-IR pulse shaping, which enables rapid scanning, phase cycling, and automatic phasing. Absorptive spectra are obtained, that have the highest frequency resolution possible, from which we extract the rephasing and nonrephasing signals that are sometimes preferred. Using this technique, we measure the vibrational mode of CO adsorbed on a polycrystalline Pt surface. The 2D spectrum reveals a significant inhomogenous contribution to the spectral line shape, which is quantified by simulations. This observation indicates that the surface conformation and environment of CO molecules is more complicated than the simple "atop" configuration assumed in previous work. Our method can be straightforwardly incorporated into many existing SFG spectrometers. The technique enables one to quantify inhomogeneity, vibrational couplings, spectral diffusion, chemical exchange, and many other properties analogous to 2D IR spectroscopy, but specifically for interfaces.
机译：在过去的十年中，二维红外光谱已成为研究分子结构和动力学的重要技术。我们报告了外差检测二维和频生成（HD 2D SFG）光谱的实现，这是2D红外（2D IR）光谱的模拟，但对非中心对称系统（例如界面）具有选择性。我们使用中红外脉冲整形技术来实现该技术，该技术可实现快速扫描，相位循环和自动定相。获得具有尽可能高的频率分辨率的吸收光谱，从中我们提取出有时最好的定相和非定相信号。使用这种技术，我们测量了吸附在多晶Pt表面上的CO的振动模式。 2D光谱显示出对光谱线形状的显着不均匀贡献，这可以通过模拟进行量化。该观察结果表明，CO分子的表面构象和环境比先前工作中假定的简单“顶部”构型更为复杂。我们的方法可以直接集成到许多现有的SFG光谱仪中。该技术使人们能够量化不均匀性，振动耦合，光谱扩散，化学交换和许多其他类似于2D IR光谱学的特性，但专门针对界面。

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