Vibration-rotation spectra of HCl in rare-gas liquid mixtures: Molecular dynamics simulations of Q-branch absorption
Vibration-rotation spectra of HCl in rare-gas liquid mixtures: Molecular dynamics simulations of Q-branch absorption
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稀有气体液体混合物中 HCl 的振动-旋转光谱：Q 支链吸收的分子动力学模拟
DOI：
10.1063/1.1454994
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发表时间：
2002
影响因子：
4.4
通讯作者：
B. Veken
中科院分区：
文献类型：
--
作者：
A. Medina;J. Roco;A. Hernández;S. Velasco;M. Bulanin;W. Herrebout;B. Veken
本文介绍了HCl溶于纯Ar和Ar掺杂Kr和Ar的红外光谱基本带形的新实验结果。在掺杂溶液的光谱中观察到中心Q支范围内的吸收的强烈增强。用（12-6）Lennard-Jones位-位相互作用势对谱带轮廓进行了半经典分子动力学模拟。通过拟合已有的各向异性相互作用曲面，推导出模型势的参数，准确描述了稀有气体-HCl货车van der Waals二元络合物的结构.模拟逼真地再现了所观察到的三重态能带结构及其随热力学条件变化的演化。各向异性相互作用对溶质取向动力学和取向依赖的径向分布函数的影响的分析揭示了有助于出现的Q-分支的机制。结果表明，长寿命溶质-溶剂空间相关性是一个重要的研究方向。
New experimental results are presented on the fundamental IR band shape of HCl dissolved in neat liquid Ar and Ar doped with Kr and Xe. A strong enhancement of the absorption in the range of a central Q-branch is observed in the spectra of doped solutions. Semiclassical molecular dynamics simulations of the spectral band profile are carried out using (12-6) Lennard-Jones site–site interaction potentials. The parameters of these model potentials were deduced by fitting the available anisotropic interaction surfaces, accurately describing the structure of binary rare-gas-HCl van der Waals complexes. Simulations realistically reproduce the observed triplet band structure and its evolution with changing thermodynamic conditions. The analysis of the influence of anisotropic interactions on the orientational dynamics of solutes and orientation-dependent radial distribution functions reveals the mechanisms that contribute to appearance of the Q-branches. It is shown that long-living solute-solvent spatial correl...