Direct time delay computation applied to the O + O2 exchange reaction at low energy: Lifetime spectrum of O3 species

• Published in: The Journal of chemical physics 2021-03, Vol.154 (10), p.104303-104303
• Main Authors: Privat, Erwan, Guillon, Grégoire, Honvault, Pascal
• Format: Article
• Language: English
• Subjects: Angular momentum; Mathematical analysis; Metastable state; Reagents; Resonance scattering; Time lag
• ISSN: 0021-9606; 1089-7690
• DOI: 10.1063/5.0040717

We report full quantum dynamical calculations for lifetimes of scattering resonances, among which are true metastable states, of the intermediate heavy ozone complex 50O3* of the 18O + 16O16O reaction, for any value of the total angular momentum quantum number J. We show that computations for nonzero values of J are mandatory in order to properly analyze resonances and time delays, with a view to establish a somewhat comprehensive eigenlife spectrum of the complex O3*. Calculations have been performed in a given low to moderate energy range, including the interval between zero-point energies (ZPEs) of reagents and product species. Quasi-bound states tend to be more numerous, and eigenlifetimes themselves are seen to increase with J, reaching unusually large values for J = 30. A very dense forest of O3* species is pictured already for J greater than 20, especially at the highest energies considered, leading to a quasi-continuum of metastable states. On the contrary, they appear as rather sparse and isolated at J = 0 and lower energies, including the domain between 18O16O and 16O16O ZPEs, embedded among many overlapping resonances that turn out to be not long-lived enough to be associated with genuine metastable states.