Collisional O₂+ N₂State-Selected Cross Sections for Open Science Cloud Reuse

Abstract

In this paper, we report a quasi-classical trajectory study of the internal energy state specificity of dissociative O2 + N2 collision rates computed at high temperatures on an accurate potential energy surface (PES). This paper analyzes the outcomes of the trajectory calculations performed by explicitly considering the rotational state of the reactants and compares them with those of a previous study carried out by assuming a thermal rotational distribution. In particular, in order to quantify the deviation of the rotationally thermalized rates from the rotationally state-selected ones, we discuss here the properties of the corresponding state-specific and state-to-state cross sections with the support of both internuclear distance and bond-order reduced dimensionality representations of the isoenergetic contours of the PES. This allows us to single out a suitable bond-order-like process coordinate useful for modeling detailed dissociation cross sections and rate coefficients and relating them, as well, to some specific features of the PES. Furthermore, this is also shown to be useful for structuring data repositories of the molecular section of the European Open Science Cloud Project so as to obtain collaborative production, validation, reuse, and dissemination of chemical processes’ knowledge and efficiency parameters.

Global and Full-Dimensional Potential Energy Surfaces of the N2 + O2 Reaction for Hyperthermal Collisions

“…For this PES, 54,046 data points were computed at the multi-state complete-active-space second-order perturbation theory (MS-CASPT2) − level with the minimally augmented correlation-consistent polarized valence triple-zeta (maug-cc-pVTZ) basis set. − The energies of these data were then dynamically scaled with the dynamically scaled external correlation (DSEC) method to recover a larger fraction of the external correlation and fitted to the many-body (MB) function form with the four-body component represented by the permutationally invariant polynomial (PIP) in terms of bond-order functions of the six interatomic distances. The resulting PES, abbreviated as the MB-PIP PES, has been widely used for kinetic and dynamic simulations. − The MB-PIP PES played a crucial role in the development of high-temperature aerothermodynamics. Our understanding and prediction ability have been significantly improved, and the simulated results were generally consistent with available experiments.…”