New Methodology Shows Short Atmospheric Lifetimes of Oxidized Sulfur and Nitrogen due to Dry Deposition

Abstract. The atmospheric lifetimes of pollutants determine their impacts on human health, ecosystems and climate and yet pollutant lifetimes due to dry deposition over large regions have not been determined from measurements. Here, a new methodology based on aircraft observations is used to determine the lifetimes of oxidized sulfur and nitrogen due to dry deposition over (3–6) × 103 km2 of boreal forest in Canada. Dry deposition fluxes decreased exponentially with distance, resulting in lifetimes of 2.2–26 hours. Fluxes were 2–14 and 1–18 times higher than model estimates for oxidized sulfur and nitrogen, respectively, indicating dry deposition velocities which were 1.2–5.4 times higher than those computed for models. A Monte-Carlo analysis with five commonly used inferential dry deposition algorithms indicates that such model underestimates of dry deposition velocity are typical. These findings indicate that deposition to vegetation surfaces are likely under-estimated in regional and global chemical transport models regardless of the model algorithm used. The model-observation gaps may be reduced if surface pH, and quasi-laminar and aerodynamic resistances in algorithms are optimized as shown in the Monte-Carlo analysis. Assessing the air quality and climate impacts of atmospheric pollutants on regional and global scales requires improved measurement-based understanding of atmospheric lifetimes of these pollutants.