Regularity and Non-statistical Nature of Transition Dynamics and Chemical Reaction Dynamics Theory

我们分析了6原子Lennard-Jones团簇过渡态区域的局部规律性，以演示如何在相空间中选择一条非重交叉反应路径，沿着该路径，经典反应路径的透射系数从阈值到中等高能量为1，过渡态是混乱的，以及如何描绘非线性，通过将超曲面投影到只有几个维度的空间来划分超曲面的全相空间特征。这些克服了化学反应理论中长期存在的模糊性之一，再交叉问题，直到中等高的能量，并使过渡态理论更一般化，即使在明显的再交叉破坏传统理论的情况下也适用。

We have analyzed local regularities in the regions of transition states of a 6-atom Lennard-Jones cluster to demonstrate how one can choose a non-recrossing reaction path in phase space along which the transmission coefficient for the classical reaction path is unity from threshold up to a moderately high energy, at which the transition state is chaotic, and how one can picture the nonlinear, full-phase-space character of dividing hypersurface by projecting it into spaces of only a few dimensions. These overcome one of the long-standing ambiguities in chemical reaction theories, recrossing problem, up to moderately high energies, and make transition state theory more generalized, applicable even in cases that apparent recrossings spoil the conventional theory.