Gamallo Pablo, Huarte-Larrañaga Fermín, González Miguel
Departament de Química Física and IQTC, Universitat de Barcelona , C/Martí i Franqués 1, 08028 Barcelona, Spain.
J Phys Chem A. 2013 Jul 3;117(26):5393-400. doi: 10.1021/jp402400g. Epub 2013 Jun 24.
We investigated the oscillations found in the integral cross section of the title reaction, which are particularly evident for Ne + H2(+)(v0 = 2,j0 = 1) [essentially isoenergetic with NeH(+)(v' = 0,j' = 0) + H] at low collision energy (Ecol < 0.30 eV). We employed mainly an exact time-independent (TI) quantum dynamics method and used the best potential energy surface available. From analysis of TI initial state selected to all integral cross sections, state-to-state integral cross sections, and the corresponding differential cross sections (DCSs), we showed that the oscillations correspond to resonances. They arise from the influence of the global Ne-H-H (collinear) minimum on dynamics and probably correspond to Feshbach resonances. Besides, the forward-backward peaking DCS (which oscillates with Ecol) behavior observed could be a signature for this type of resonances. Finally, as most data on resonances in bimolecular reactions correspond to neutral systems, we hope that the present results will encourage experimentalists to re-examine this benchmark system.
我们研究了标题反应积分截面中发现的振荡，这在低碰撞能量（Ecol < 0.30 eV）下对于Ne + H2(+)(v0 = 2,j0 = 1) [与NeH(+)(v' = 0,j' = 0) + H基本等能] 尤为明显。我们主要采用了精确的与时间无关（TI）量子动力学方法，并使用了现有的最佳势能面。通过对TI初始态选择的所有积分截面、态-态积分截面以及相应的微分截面（DCSs）的分析，我们表明这些振荡对应于共振。它们源于全局Ne-H-H（共线）最小值对动力学的影响，可能对应于费什巴赫共振。此外，观察到的前向-后向峰值DCS（随Ecol振荡）行为可能是这类共振的一个特征。最后，由于双分子反应中共振的大多数数据对应于中性系统，我们希望目前的结果将促使实验人员重新审视这个基准系统。
