理论模拟含氢键二次有机气溶胶的振动光谱

项目名称： 理论模拟含氢键二次有机气溶胶的振动光谱

项目编号： No.21273094

项目类型： 面上项目

立项/批准年度： 2013

项目学科： 数理科学和化学

项目作者： 李辉

作者单位： 吉林大学

项目金额： 80万元

中文摘要： 二次有机气溶胶通过凝聚大气中挥发性有机化合物的氧化产物而形成。二次有机气溶胶作为气溶胶的重要组成部分，对气候改变、环境污染、人类健康有很大影响， 备受研究者关注。 二次有机气溶胶的光谱表征是实验研究其成份、结构、大小、形状等内部性质的重要手段。 而由于其内在的复杂性, 给实验科学家的光谱指认造成了巨大的困难。 二次有机气溶胶中常含有大量氢键, 凝聚中容易形成动态氢键网络，具有不可忽视的量子效应。 本项目立足大气化学热点， 以含氢键二次有机气溶胶为研究对象，拟发展量子路径积分分子动力学（PIMD)程序， 应用自己发展的从头算基础的分子内－分子间相关势和力场， 模拟二次有机气溶胶的内部结构和氢键动力学，考察温度相关的量子效应。 结合一次微扰理论和中心分子动力学方法（CMD）， 该项目拟模拟二次有机气溶胶的振动光谱，帮助实验化学家进行光谱指认，为进一步解析卫星遥感光谱信息提供基础数据。

中文关键词： 势能面；振动光谱；分子动力学；气溶胶；分子簇

英文摘要： Secondary organic aerosols are formed in the atmosphere through condensation of oxidation products of volatile organic compounds. Secondary organic aerosols, as an important part of atmospheric aerosol, have great effects on the climate change，environmental pollution and human health, and have been given great attention from research scientists. Spectroscopic characterization of secondary organic aerosols is an important experimental route to investigate their components, architecture, size, shape and other intrinsic particle properties. However, due to the intrinsic complexes of the secondary organic aerosols, the observed experimental spectra are very difficult to be assigned. Most of the secondary organic aerosols have hydrogen bonds, which are easy to form dynamic hydrogen-bond network during their condensation, and have non-negligible nuclear quantum effects. For this research, based on the hot topic of atmospheric chemistry, secondary organic aerosols with hydrogen bonds are selected as our research objects. A path-integral molecular dynamics (PIMD) code will be developed in this project. With our own ab initio-based representation of the underlying inter- and intra- molecular interactions and forces, it will be applied in simulating the structure and dynamics of hydrogen-bond network formed in second or

英文关键词： potential energy surface；vibrational spectra；molecular dynamics；aerosols；molecular clusters