Department of Chemistry, Indian Institute of Technology Guwahati, Guwahati, Assam 781039, India.
J Chem Phys. 2010 Jun 7;132(21):214304. doi: 10.1063/1.3429609.
Full dimensional quantum scattering calculations have been carried out for the OH + H(2) --> H(2)O + H reaction on the Walch-Dunning-Schatz-Elgersma and Yang-Zhang-Collins-Lee surfaces employing an exact form of the kinetic energy operator. The multiconfiguration time-dependent Hartree (MCTDH) method has been used to perform the wave packet propagations. The MCTDH method uses relatively little memory and its numerical effort scales much more slowly with the dimensionality of the system compared to conventional propagation methods. The reaction probabilities and cross sections obtained on both the surfaces using the MCTDH method are in good agreement with the previous theoretical results. However, the cross sections on the two surfaces differ significantly as a function of the translational energy of the reagents. The difference in barrier heights for the two surfaces along with the transition state structures account for the different reaction probabilities obtained over the entire energy range considered.
已针对 OH + H(2) --> H(2)O + H 反应在 Walch-Dunning-Schatz-Elgersma 和 Yang-Zhang-Collins-Lee 表面上进行了全维量子散射计算，使用了动能算子的精确形式。多组态含时哈特ree（MCTDH）方法已用于执行波包传播。与传统传播方法相比，MCTDH 方法使用的内存相对较少，并且其数值工作量随系统维数的增加而增加的速度要慢得多。使用 MCTDH 方法在两个表面上获得的反应概率和截面与先前的理论结果吻合良好。然而，两个表面上的截面随试剂的平动能显著不同。两个表面的势垒高度的差异以及过渡态结构解释了在整个考虑的能量范围内获得的不同反应概率。
