Sun Zhigang, Lin Xin, Lee Soo-Y, Zhang Dong H
Division of Physics & Applied Physics, School of Physical & Mathematical Sciences, Nanyang Technological University, Singapore.
J Phys Chem A. 2009 Apr 23;113(16):4145-54. doi: 10.1021/jp810512j.
A new time-dependent wavepacket method is developed to study the A + BC --> AB + C, AC + B reaction at the state-to-state level. The method only requires propagation of the wavepacket in reactant Jacobi coordinates by extracting S-matrix information on a dividing surface right before the absorption potential in the product region. It has particular advantages for reactions with deep wells and long-range attractive interactions in the product channels in which the wavepacket in the product channels can only be absorbed sufficiently far away from the interaction potential. Demonstration made on the benchmark H + H(2) reaction shows that the method is rather efficient in dealing with a direct reaction at high collision energy. The method is applied to study the very challenging H + O(2) (nu(0) = 0, j(0) = 0, 1) reaction, with state-to-state differential cross sections obtained for the first time for collision energies up to 1.1 eV. The calculations not only show the power and accuracy of the new approach in dealing with complex-forming reactions but also shed light on the dynamics of the H + O(2) reaction.
开发了一种新的含时波包方法，用于在态-态水平上研究A + BC --> AB + C、AC + B反应。该方法仅需在反应物雅可比坐标中传播波包，通过在产物区域吸收势之前的分割面上提取S矩阵信息来实现。对于产物通道中存在深势阱和长程吸引相互作用的反应，该方法具有独特优势，因为在这种情况下，产物通道中的波包只能在远离相互作用势的足够远处被吸收。对基准反应H + H(2)的演示表明，该方法在处理高碰撞能量下的直接反应时相当有效。该方法被应用于研究极具挑战性的H + O(2)（ν(0) = 0，j(0) = 0，1）反应，首次获得了碰撞能量高达1.1 eV时的态-态微分截面。计算结果不仅展示了这种新方法在处理形成复合物反应方面的能力和准确性，还为H + O(2)反应的动力学提供了新的见解。
