New Development of Reaction Dynamics Theory based on the Free Energy Gradient Method

在本研究计划中，针对化学反应体系的多维性，开展了以下两方面的研究：(A)它们是依赖时间的化学反应过程；(B)非线性、非平衡和非定常过程：(1)反应能传递机理的分析不仅用多原子分子的Fokker-Planck方程，而且用分子动力学(MD)模拟。(2)我们用分子动力学模拟解释了非平衡动力学中的一些典型特征，并发展了一种新的处理方法来确定自由能超曲面上的临界点，即：(3)研究了上述方法与基于Fokker-Planck方程的模型理论之间的联系，并在中期的研究中，在日本化学会和CSW2004年会上发表了一些关于水溶液中反应能转移的结果。此外，它们被收集并作为几篇研究文章发表，如下一节所述，即参考文献11。

In this Research Program, notifying the multidimensionality of chemically reacting systems, a number of research were executed focusing the following two points : (a)they are time-dependent chemical processes and (b)nonlinear, nonequilibrium and nonstationary processes :(1)The reactive energy transfer mechanism was analyzed by using not only the Fokker-Planck equation for polyatomic molecules but also molecular dynamics(MD) simulation.(2)We explained some typical characteristics in nonequilibrium dynamics by using MD simulation and develpoed a novel treatment to locate critical points on the free energy hypersurface, i.e., free energy gradient method(FEGM).(3)We investigated the connection between the above method and a model theory based on the Fokker-Planck equation.In the middle of the research term, several results with respect to the reactive energy transfer in aqueous solution, were published in the annual meetings of Japan Chemical Society and CSW2004. Further, they were collected and published as several research articles as described in the following section, i.e., 11 REFERENCE.