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  14 Jan 2021

14 Jan 2021

Review status: this preprint is currently under review for the journal ACP.

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

Katherine Hayden1, Shao-Meng Li1,2, Paul Makar1, John Liggio1, Samar G. Moussa1, Ayodeji Akingunola1, Robert McLaren3, Ralf M. Staebler1, Andrea Darlington1, Jason O'Brien1, Junhua Zhang1, Mengistu Wolde4, and Leiming Zhang1 Katherine Hayden et al.
  • 1Air Quality Research Division, Environment and Climate Change Canada, Toronto, Ontario, Canada, M3H 5T4
  • 2College of Environmental Science and Engineering, Peking University, Beijing 100871 China
  • 3Center for Atmospheric Chemistry, York University, 4700 Keele Street, Toronto, Ontario, Canada
  • 4National Research Council Canada, Flight Research Laboratory, Ottawa, Canada K1A 0R6

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.

Katherine Hayden et al.

Status: open (until 11 Mar 2021)

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Katherine Hayden et al.

Katherine Hayden et al.


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