A quasi-classical study of energy transfer in collisions of hyperthermal H atoms with SO2 molecules

作者：da Silva Ramon S; Garrido Juan D; Ballester Maikel Y^*

来源：Journal of Chemical Physics, 2017, 147(8): 084308.

DOI：10.1063/1.4991699

A deep understanding of energy transfer processes in molecular collisions is at central attention in physical chemistry. Particularly vibrational excitation of small molecules colliding with hot light atoms, via a metastable complex formation, has shown to be an efficient manner of enhancing reactivity. A quasi-classical trajectory study of translation-to-vibration energy transfer (T-V ET) in collisions of hyperthermal H(S-2) atoms with SO2((X) over tilde (1)A') molecules is presented here. For such a study, a double many-body expansion potential energy surface previously reported for HSO2((2)A) is used. This work was motivated by recent experiments by Ma et al. studying collisions of H + SO2 at the translational energy of 59 kcal/mol [J. Ma et al., Phys. Rev. A 93, 040702 (2016)]. Calculations reproduce the experimental evidence that during majority of inelastic non-reactive collision processes, there is a metastable intermediate formation (HOSO or HSO2). Nevertheless, the analysis of the trajectories shows that there are two distinct mechanisms in the T-V ET process: direct and indirect. Direct T-V processes are responsible for the high population of SO2 with relatively low vibrational excitation energy, while indirect ones dominate the conversion from translational energy to high values of the vibrational counterpart. Published by AIP Publishing.

• 出版日期2017-8-28