Comprehensive \textsl{Ab Initio}~Calculations of \ce{CO2-H2} and \ce{CO2-He} Collisional Properties
Abstract
We present comprehensive \textsl{ab initio} calculations of CO-H and CO-He collisional properties from first principles, employing CCSD(T), potential calculations together with close-coupling dynamical scattering in the \YUMI~framework. We derive (in)elastic cross sections, rate coefficients, and pressure-broadening parameters -- incl., their rotational dependence up to , and temperature dependence over the range of 100-800 K. We provide Pad\'e fits for the broadening coefficients as a function of rotational quantum number, enabling extrapolation of the results and integration into spectroscopic databases, including HITRAN and HITEMP. The computed potentials for both CO-H and CO-He have a sub-percent precision, and the dynamics-solving code YUMI ultimately yields the collisional parameters. Among these, the scaled pressure broadening experimental values meet the 10\% precision requirement for exoplanetary sciences with \textit{JWST}. This contrasts with the parameters available before the present calculations, which at higher temperatures (T400 K) deviate as much as 5 from the desired precision requirement. All derivations and collisional properties are provided with this manuscript, establishing the first of such a comprehensive ab initio foundation for collisional systems with a target molecule having more than two atoms.
Cite
@article{arxiv.2510.03327,
title = {Comprehensive \textsl{Ab Initio}~Calculations of \ce{CO2-H2} and \ce{CO2-He} Collisional Properties},
author = {Prajwal Niraula and Laurent Wiesenfeld and Nejmeddine Jaïdane and Julien de Wit and Robert J. Hargreaves and Jeremy Kepner and Deborah Woods and Cooper Loughlin and Iouli E. Gordon},
journal= {arXiv preprint arXiv:2510.03327},
year = {2025}
}
Comments
Submitted. Comments welcome. Data available at zenodo: https:/zenodo.org/records/17161891