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相干振动动力学和高分辨非线性光谱学:空气/二甲亚砜液体界面的比较
Luis Velarde,陆洲,王鸿飞*
作者单位E-mail
Luis Velarde 美国能源部西北太平洋国家实验室William R. Wiley环境分子科学研究所华盛顿州里奇兰市99352  
陆洲 美国能源部西北太平洋国家实验室William R. Wiley环境分子科学研究所华盛顿州里奇兰市99352  
王鸿飞* 美国能源部西北太平洋国家实验室William R. Wiley环境分子科学研究所华盛顿州里奇兰市99352 hongfei.wang@pnnl.gov 
摘要:
研究了空气/二甲亚砜界面C?H伸缩振动的自由诱导衰减的相干振动动力学和亚波数高分辨宽带和频振动光谱.对于特定分子体系,频率域光谱测量和时间域动力学测量原则上应获得相同的信息.但对具有耦合或者重叠在一起的若干振动模式的分子体系,通过时域或者频域测量以获取光谱和动力学信息细节均非易事.对于振动光谱并非过于复杂的空气/二甲亚砜界面,基于亚波数高分辨宽带和频振动光谱的频域测量较超快时域测量更有益于获取界面结构和相干动力学定量信
关键词:  和频振动光谱,高分辨宽带和频振动光谱,自由诱导衰减,二甲亚砜,空气/二甲亚砜界面
DOI:10.1063/1674-0068/26/06/710-720
分类号:
基金项目:
Coherent Vibrational Dynamics and High-resolution Nonlinear Spectroscopy: A Comparison with the Air/DMSO Liquid Interface
Luis Velarde,Zhou Lu,Hong-fei Wang*
Abstract:
We present a comparative study on the C-H stretching vibrations at air/DMSO (dimethyl sulfoxide) interface with both the free-induction decay (FID) coherent vibrational dynamics and the sub-wavenumber high resolution sum-frequency generation vibrational spectroscopy measurements. In principle the frequency-domain and time-domain spectroscopic measure-ments should generate identical information for a given molecular system. However, when the molecular systems are with several coupled or overlapping vibrational modes, obtain-ing detailed spectroscopic and coherent dynamics information is not as straightforward and rather difficult from either the time-domain or the frequency domain measurements. For the case of air/DMSO interface that is with moderately complex vibrational spectra, we show that the frequency-domain measurement with sub-wavenumber high-resolution sum-frequency generation vibrational spectroscopy is probably more advantageous than the time-domain measurement in obtaining quantitative understanding of the structure and coherent dynamics of the molecular interface
Key words:  Sum-frequency generation vibrational spectroscopy (SFG-VS), High-resolution broadband SFG-VS, Free-induction decay, Dimethyl sulfoxide, Air/DMSO interface