Reactive uptake of N₂O₅ by atmospheric aerosol is dominated by interfacial processes

Nitrogen oxides are removed from the troposphere through the reactive uptake of N₂O₅ into aqueous aerosol. This process is thought to occur within the bulk of an aerosol, through solvation and subsequent hydrolysis. However, this perspective is difficult to reconcile with field measurements and cannot be verified directly because of the fast reaction kinetics of N₂O₅ Here, we use molecular simulations, including reactive potentials and importance sampling, to study the uptake of N₂O₅ into an aqueous aerosol. Rather than being mediated by the bulk, uptake is dominated by interfacial processes due to facile hydrolysis at the liquid-vapor interface and competitive reevaporation. With this molecular information, we propose an alternative interfacial reactive uptake model consistent with existing experimental observations.