Dominated non-statistical behaviors in O+O2 Exchange Reactive Scattering:

Abstract

State-to-state differential and integral cross sections are obtained by accurate quantum dynamics and quasi-classical calculations with the title reaction. The pronounced forward scattering, resulting from the quantum tunneling and slow-down mechanism over the centrifugal barrier, is clearly observed. The collision energies dependent opacity function also exhibits clear non-statistical characteristics. The results are compared with quasi-classical trajectories calculation, which reveals the surprising quantum effects in this system involving such heavy atoms. The special reef structure around the intermediate well of the potential energy surface, which results in effective tunneling penetration with high total angular momentum, and the slow intramolecular energy redistribution of the intermediate O3 complex, which conduces to tuneful quantum resonance states between different partial waves, are explained to account for the significant quantum effects. The strong non-statistical behaviors in the title reaction imply a necessitation of a full quantum description of the isotope effects in an ozone stabilization processes, contrast to the current popular adopted models