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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Collision energy dependence of the O(D-1)+HCl - OH+Cl(P-2) reaction studied by crossed beam scattering and quasiclassical trajectory calculations on ab initio potential energy surfaces
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Collision energy dependence of the O(D-1)+HCl - OH+Cl(P-2) reaction studied by crossed beam scattering and quasiclassical trajectory calculations on ab initio potential energy surfaces

机译：O（D-1）+ HCl-> OH + Cl（P-2）反应的碰撞能依存关系，其通过从头算势能面上的交叉束散射和准经典轨迹计算来研究

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摘要

The dynamics of the O(D-1) + HCl -> OH + Cl(P-2) reaction are investigated by a crossed molecular beam ion-imaging method and quasiclassical trajectory calculations on the three ab initio potential energy surfaces, the ground 1(1)A' and two excited (1(1)A '' and 2(1)A') states. The scattering experiment was carried out at collision energies of 4.2, 4.5, and 6.4 kcal/mol. The observed doubly differential cross sections (DCSs) for the Cl(P-2) product exhibit almost no collision energy dependence over this inspected energy range. The nearly forward-backward symmetric DCS indicates that the reaction proceeds predominantly on the ground-state potential energy surface at these energies.. Variation of the forward-backward asymmetry with collision energy is interpreted using an osculating complex model. Although the potential energy surfaces obtained by CASSCF-MRCI ab initio calculations exhibit relatively low potential barriers of 1.6 and 6.5 kcal/mol for 1(1)A '' and 2(1)A', respectively, the dynamics calculations indicate that contributions of these excited states are small at the collision energies lower than 15.0 kcal/mol. Theoretical DCSs calculated for the ground-state reaction pathway agree well with the observed ones. These experimental and theoretical results suggest that the titled reaction at collision energies less than 6.5 kcal/mol is predominantly via the ground electronic state.
机译：通过交叉分子束离子成像方法和准经典轨迹计算在三个从头算势能面（地面1）上研究了O（D-1）+ HCl-> OH + Cl（P-2）反应的动力学。 （1）A'和两个激发（1（1）A''和2（1）A'）状态。散射实验是在碰撞能量为4.2、4.5和6.4 kcal / mol的条件下进行的。 Cl（P-2）产物的观察到的双微分截面（DCSs）在此检查的能量范围内几乎没有碰撞能量依赖性。几乎向前-向后对称的DCS表示，在这些能量下，反应主要在基态势能表面上进行。使用紧密复合模型解释了向前向后不对称性与碰撞能量的变化。尽管通过CASSCF-MRCI从头计算获得的势能面分别显示出1（1）A''和2（1）A'的势垒较低，分别为1.6和6.5 kcal / mol，但动力学计算表明在低于15.0 kcal / mol的碰撞能量下，这些激发态很小。为基态反应路径计算的理论DCS与观察到的DCS吻合良好。这些实验和理论结果表明，在碰撞能量小于6.5 kcal / mol时的标题反应主要是通过基态电子引起的。

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