H + DN (v = 0,1; j = 0)→HD + N及其同位素效应的量子和准经典动力学研究

Study on Quantum and Quasi-Classical Dynamics of Reaction H + DN (v = 0,1; j = 0)→HD + N and Its Isotopic Variants

摘要: 本文采用含时波包(TDWP)和准经典轨线(QCT)方法，在反应阈值到1.0 eV的碰撞能量范围内，在4A''态新势能面(PES)上研究了标题反应及其同位素效应。我们考虑了科里奥利耦合(CC)效应，并给出了CC和CS近似计算的结果比较。在不同总角动量J值下，比较了用不同方法得到的反应几率与碰撞能量的关系。CC和CS结果的积分截面有显著差异。在大部分碰撞能量范围内，QCT计算的截面很好地再现了CC结果。此外，还计算了J = 0时标题反应随攻击角变化的反应几率。研究发现，反应几率与攻击角密切相关。此外本文还详细研究了反应物振动激发对依赖攻击角的反应几率的影响。

Abstract: Time-dependent wave packet (TDWP) and quasic-classical trajectory (QCT) methods were employed to study the title reaction and its isotopic variants on a new potential energy surface (PES) of 4A'' state over the range of collision energies starting from the reaction threshold to 1.0 eV. We took the Coriolis coupling (CC) effect into account and presented the comparison between the CC and the centrifugal sudden (CS) approximation calculations. Reaction probabilities obtained using the different methods were thoroughly compared as a function of the collision energy for a series of total angular momentum J values. Significant differences of integral cross section between CC and CS results have been observed. The QCT-calculated cross sections and probabilities reproduced well the CC results over most of the collision energy range. In addition, the attack angle dependent reaction probabilities of the title reaction at J = 0 were calculated. The reaction probabilities were found to be strongly dependent on the attack angle. The influences of the reactant vibration excitation on the attack angle dependent reaction probabilities were also studied in detail.