Parameterization of plume chemistry into large-scale atmospheric models: Application to aircraft NOx emissions

A method is presented to parameterize the impact of the nonlinear chemical reactions occurring in the plume generated by concentrated NO_x sources into large-scale models. The resulting plume parameterization is implemented into global models and used to evaluate the impact of aircraft emissions on the atmospheric chemistry. Compared to previous approaches that rely on corrected emissions or corrective factors to account for the nonlinear chemical effects, the present parameterization is based on the representation of the plume effects via a fuel tracer and a characteristic lifetime during which the nonlinear interactions between species are important and operate via rates of conversion for the NO_x species and an effective reaction rates for O₃. The implementation of this parameterization insures mass conservation and allows the transport of emissions at high concentrations in plume form by the model dynamics. Results from the model simulations of the impact on atmospheric ozone of aircraft NO_x emissions are in rather good agreement with previous work. It is found that ozone production is decreased by 10 to 25% in the Northern Hemisphere with the largest effects in the north Atlantic flight corridor when the plume effects on the global-scale chemistry are taken into account. These figures are consistent with evaluations made with corrected emissions, but regional differences are noticeable owing to the possibility offered by this parameterization to transport emitted species in plume form prior to their dilution at large scale. This method could be further improved to make the parameters used by the parameterization function of the local temperature, humidity and turbulence properties diagnosed by the large-scale model. Further extensions of the method can also be considered to account for multistep dilution regimes during the plume dissipation. Furthermore, the present parameterization can be adapted to other types of point-source NO_x emissions that have to be introduced in large-scale models, such as ship exhausts, provided that the plume life cycle, the type of emissions, and the major reactions involved in the nonlinear chemical systems can be determined with sufficient accuracy.