English

Heavy-Impact Vibrational Excitation and Dissociation Processes in CO$_2$

Chemical Physics 2021-09-15 v2

Abstract

A heavy-impact vibrational excitation and dissociation model for CO2_2 is presented. This state-to-state model is based on the Forced Harmonic Oscillator (FHO) theory which is more accurate than current state of the art kinetic models of CO2_2 based on First Order Perturbation Theory. The first excited triplet state 3^{3}B2_{2} of CO2_2, including its vibrational structure, is considered in our model, and a more consistent approach to CO2_2 dissociation is also proposed. The model is benchmarked against a few academic 0D cases and compared to decomposition time measurements in a shock tube. Our model is shown to have reasonable predictive capabilities, and the CO2_2 ++ O \leftrightarrow CO ++ O2_2 is found to have a key influence on the dissociation dynamics of CO2_2 shocked flows, warranting further theoretical studies. We conclude this study with a discussion on the theoretical improvements that are still required for a more consistent analysis of the vibrational dynamics of CO2_2, discussing the concept of vibrational chaos and its possible application to CO2_2. The necessity for further experimental works to calibrate such state-to-state models is also discussed, with a proposed roadmap for novel experiments in shocked flows.

Keywords

Cite

@article{arxiv.2006.10426,
  title  = {Heavy-Impact Vibrational Excitation and Dissociation Processes in CO$_2$},
  author = {João Vargas and Bruno Lopez and Mário Lino da Silva},
  journal= {arXiv preprint arXiv:2006.10426},
  year   = {2021}
}

Comments

73 pages, 23 figures