发展新的波包传播、坐标变换方法研究态态分子反应动力学

项目名称： 发展新的波包传播、坐标变换方法研究态态分子反应动力学

项目编号： No.11304310

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 数理科学和化学

项目作者： 张佩宇

作者单位： 中国科学院大连化学物理研究所

项目金额： 25万元

中文摘要： 态态量子动力学研究给出了最精细的反应动力学实验可观测量。但是，理论计算的计算量仍是一个很大的挑战。我们将发展两种新的方法分别提高态态动力学研究中波包传播效率和反应物产物坐标系之间的变换效率。新的波包传播方法将引入一个分裂算符，显著减少计算节点间的通信，解决并行瓶颈。新的坐标变换方法将变换分成两部分，把一个五重循环变成两个四重循环，减少变换所需的计算量的同时不消耗系统更多的内存。利用新方法，编写一整套态态动力学程序，并实现GPUs/CPUs并行化。与前人的方法进行测试比较，比较各种方案之间的计算量区别以及应用于各种反应体系时不同的适用性。讨论新方法推广到四原子体系的可行性。最后应用程序计算几个典型体系的态态反应几率、积分截面、微分截面等精确定量的动力学结果，研究反应机理。

中文关键词： 反应动力学；含时波包；态态；微分截面；反应机理

英文摘要： State-to-state quantum reaction dynamics study provides the most detailed observable of reaction dynamics experiments. But the theoretical calculations are still a great challenge of amount of the computation.We will develop two methods to raise the efficiencies of the wave-packet propagation and transformation between the reactant and product coordinates, respectively. A new split-operator method is introduced in wave-packet propagation and decreases communication among the computational nodes. Therefore, it solves the bottleneck of the parallelism. A new method separates the coordinate transformation into two parts, and turns the five-loop calculation to two four-loop calculations. It decreases the amount of computation and needs no extra memory. A state-to-state dynamics code will developed with the new methods and parallelly implemented on GPUs/CPUs. The methods will be tested and compared with the previous works in the amount of computation and applicability in different systems. We will discuss the feasibility to extend the new methods to tetratomic systems. At last the code will be applied on several prototype reactions to obtain accurately quantitative results, such as the state-to-state reaction probabilities, integral and differential cross section, to study the mechanism of reaction.

英文关键词： reactive dynamics；time-dependent wave-packet；state-to-state；differential cross-section；reaction mechanism