准经典轨线方法研究H(^(2)S)+NO(X^(2)Π)→N(^(4)S)+OH(X^(2)Π)反应动力学

Kinetics and Dynamics of the H(^(2)S)+NO(X^(2)Π)→N(^(4)S)+OH(X^(2)Π) Reaction:A Quasi-classical Trajectory Study

本文基于精确的势能面,采用准经典轨线方法研究了H(^(2)S)+NO(X^(2)Π)→N(^(4)S)+OH(X^(2)Π)反应的动力学.对碰撞能量为2.00~2.80 eV,计算了反应的总反应积分截面,发现它随碰撞能量的增加而单调增加.特别地,在碰撞能为2.40~2.57 eV时,计算的反应截面与实验结果吻合.此外,计算得到的反应速率常数也与实验匹配.在碰撞能为2.57 eV时,通过对反应轨线的分析,发现该反应由非直接反应主导(是直接反应的1.4倍),揭示了反应在高碰撞能量下的反应动力学特性.

A quasi-classical trajectory study of the H(^(2)S)+NO(X^(2)Π)→N(^(4)S)+OH(X^(2)Π) reaction kinetics and dynamics is reported on an accurate potential energy surface.The total integral cross sections of the reaction were calculated at the collision energy ranging from 2.00 e V to 2.80 e V.It was found that the total reaction integral cross section increases monotonically with the collision energy.Specifically at the collision energy range of 2.40-2.57 e V,our calculated results are in reasonably good agreement with the experimental data.The calculated thermal rate constants are in fairly good agreement with available experimental results.Through the trajectory analysis at the collision energy of 2.57 e V,it was found that the title reaction is dominated by the indirect trajectories(1.4 times more compared to the direct trajectories),which sheds light on the reaction dynamics of the title reaction in the high collision energy range.