Formation and Stabilization of Ground and Excited-State Singlet O₂ upon Recombination of ³P Oxygen on Amorphous Solid...

The recombination dynamics of ³P oxygen atoms on cold amorphous solid water to form triplet and singlet molecular oxygen (O₂) is investigated under conditions representative of cold clouds. Reactive molecular dynamics simulations including Landau-Zener-based hopping to account for nonadiabatic transitions find that both ground-state (X³Σ^-) O₂ and molecular oxygen in the two lowest singlet states (a¹Δ and b¹Σ⁺) can be formed and the molecular species stabilize through vibrational relaxation. The relative populations of the species are approximately 1:1:1. These results also agree qualitatively with a kinetic model based on simplified wavepacket simulations. The presence and stabilization of higher electronic states of O₂ are expected to modify the chemical evolution of cold interstellar (T ∼ 10-50 K) and warmer noctilucent (T ∼ 100 K) clouds.