Theoretical Descriptions of Molecular Dynamics and Spectroscopy in Condensed and Gas Phases

凝聚相和气相分子动力学和光谱学的理论描述

基本信息

批准号：
0615165
负责人：
Edwin Sibert
金额：
$ 39万
依托单位：
University of Wisconsin-Madison
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2006
资助国家：
美国
起止时间：
2006-08-01 至 2009-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=0615165&HistoricalAwards=false
关键词：
Theoretical Descriptions Molecular Dynamics Spectroscopy

项目摘要

Edwin Sibert of the University of Wisconsin, Madison, is supported by the Theoretical and Computational Chemistry Program to study energy flow in polyatomic molecules in both gas and liquid phases using combined classical and quantum techniques. The research will encompass dynamical events that include vibrational relaxation, proton transfer reactions, and vibrational predissociation in the condensed phase. The objective is to develop robust molecular models of these processes. The model results should be consistent with experimental observations, and are expected to serve as a guide for future experimentation. Mixtures of bromoform and deuterated bromoform will be investigated with the goal of mapping out how energy travels between molecules. As well, formic acid dimer, a prototypical example of double proton transfer, will be studied in the gas and liquid phases. Finally, vibrational predissociation in the condensed phase, and in particular predissociation of hydrogen bonded oligomers, will be investigated.Recent advances in an ultrafast laser spectroscopies enable chemists to probe the unfolding of molecular events with unprecedented time and size resolution. When these experiments are combined with thoughtful theoretical modeling from an atomistic perspective, significant insights are attained on how energy flow is controlled by forces between atoms. This research will make progress toward quantifying these ideas and developing predictive models for the events that occur as a result of these forces. Such models are essential, in the long term, for successful modeling of atmospheric, combustion, and biological processes at a molecular level.

威斯康星大学麦迪逊分校的埃德温·西伯特（Edwin Sibert）得到了理论和计算化学计划的支持，该计划使用合并的经典和量子技术研究了气体和液相的多原子分子中的能量流。该研究将涵盖包括振动弛豫，质子转移反应以及凝结相的振动预性关联的动态事件。目的是开发这些过程的强大分子模型。模型结果应与实验观察结果一致，并有望作为未来实验的指南。将研究溴生型和一个疗程的溴构的混合物，目的是绘制出分子之间的能量如何传播。同样，将在气相和液相中研究甲酸二聚体，这是双质子转移的原型例子。最后，将研究凝结相中的振动预防，尤其是氢键寡聚物的预分离。当这些实验与周到的理论建模相结合时，就可以就原子之间的力控制能量流的方式来获得重要的见解。这项研究将在量化这些想法并为这些力量导致的事件开发预测模型方面取得进展。从长远来看，对于在分子水平上成功建模大气，燃烧和生物过程是必不可少的。