State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, 116023, P. R. China.
Science. 2011 Jul 22;333(6041):440-2. doi: 10.1126/science.1205770.
Quantum dynamical theories have progressed to the stage in which state-to-state differential cross sections can now be routinely computed with high accuracy for three-atom systems since the first such calculation was carried out more than 30 years ago for the H + H(2) system. For reactions beyond three atoms, however, highly accurate quantum dynamical calculations of differential cross sections have not been feasible. We have recently developed a quantum wave packet method to compute full-dimensional differential cross sections for four-atom reactions. Here, we report benchmark calculations carried out for the prototypical HD + OH → H(2)O + D reaction on an accurate potential energy surface that yield differential cross sections in excellent agreement with those from a high-resolution, crossed-molecular beam experiment.
量子动力学理论已经发展到可以为三原子系统常规地高精度计算态态微分截面的阶段，自从 30 多年前首次对 H+H(2)系统进行这样的计算以来。然而，对于超过三个原子的反应，高精度的量子动力学微分截面计算是不可行的。我们最近开发了一种量子波包方法来计算四原子反应的全维微分截面。在这里，我们报告了在精确势能表面上为原型 HD+OH→H(2)O+D 反应进行的基准计算，得到的微分截面与高分辨率的分子束交叉实验结果非常吻合。
