反应物极化在三原子反应动力学中的作用研究

There are two most persistent goals of scientific investigations of the dynamics of molecular reactions-understanding and control. Nowadays, most studies are strived for a detailed understanding of reaction mechanisms and of the role of energetic and directional factors. The attempt to devise techniques for the control of molecular reactions and particularly, for the selection of desired products is rather too limited. Chemical reactions are intrinsically anisotropic. The anisotropy can be revealed by vector properties. The best known of vector properties is the angular distribution of reaction products, which has been widely studied. The spatial distribtuion (polarization) of the rotational angular momenta of reagents and products is also important, and few researches are concerned with the aspect. There is no significant difference between reactants and products polarization from the theoretical point of view. However, there are differences from a practical point of view. The reagent polarization is determined by the external intervention, whereas the product polarization is determined by the reaction itself. The analysis of the dynamics of controlled reactions can provide important clues about the reaction dynamics. We plan to study the effect of reagent polarization on the triatomic reactions using both quantum mechanical and quasi-classical trajectory methods.

对于分子反应动力学的科学研究有两个持续的目标：一是理解反应机制，二是控制反应本身。目前，大部分研究都侧重于对于反应的理解和能量或者方向因素对于反应的影响。涉及控制分子反应的技术，尤其是对于特定产物的选择，相对而言，这方面的工作比较少。化学反应本质上是各向异性的，可以通过矢量性质表现出来。矢量性质中，最为大家熟悉的是产物的角分布，反应物和产物的转动角动量的空间分布（极化）也是很重要的；对于前者研究的较多，而对于后者的研究相对较少。从理论的角度来看，反应物的极化和产物的极化之间并没有重要的区别。然而，从实用的角度来看，两者是有区别的。反应物的极化由外部干预决定，而产物的极化由反应本身决定。对可操控的反应动力学的分析，能够为反应动力学提供重要的线索。我们计划采用量子力学和准经典轨线两种方法来研究反应物极化在三原子反应中的作用。

对于分子反应动力学的科学研究有两个持续的目标：一是理解反应机制，二是控制反应本身。选取反应体系：O(1D)+HCl-->ClO+H、O(1D)+DCl-->ClO+D、O(1D)+HCl-->OH+Cl和N+NH-->N2+H，我们运用准经典轨线和量子力学两种方法进行了动力学的计算，对反应机制以及反应物极化在三原子反应动力学中的作用进行了研究。近三年来，我们在以下方面取得了进展：（1）通过设定反应物的转动量子数来实现反应物的极化，（2）对积分反应截面、广义的与极化相关的微分散射截面进行了计算，(3) 计算了与反应物极化相关的反应几率，(4) 对产物转动倾斜进行了研究。截止到目前，我们已经发表了3篇被SCI收录的论文。