N atoms recombination on a silica surface: A global theoretical approach

The paper reports on a semiclassical dynamics study about N2 formation after nitrogen atom recombination on a silica surface via the Eley–Rideal collisional mechanism at T = 1000 K. The molecular dynamics study was carried out using a fitted potential energy surface based on new density functional computations on clusters cleaved from the β-cristobalite unit cell. The B3LYP results obtained using silica clusters of increasing dimensions (up to Si7O14H14) show that only atomic nitrogen is adsorbed (binding energy Eb ≅ 2.7–2.8 eV). Then, the obtained potential energy surface has been used in a time-dependent semiclassical collisional method which is able to describe, at a very detailed level, the recombination of N atoms on the surface assisted by the phonon excitation mechanism of the substrate. combination coefficient γ of the Eley–Rideal recombination mechanism was calculated together with the reaction energetics.