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Transformation of Aerosol Chemical Properties due to Transport Over a City
Authors:Email author" target="_blank">Gerhard?LammelEmail author  Thomas?Engelhardt  Adrian?Leip  Christian?Neusü?  Andreas?R?hrl  Birgit?Wehner  Alfred?Wiedensohler  Paul?Wieser
Institution:(1) Max Planck Institute for Meteorology, Bundesstr. 53, 20146 Hamburg, Germany;(2) Present address: University of Hamburg, Meteorological Institute, Bundesstr. 55, Hamburg, Germany;(3) University of Hohenheim, Institute for Physics and Meteorology, Garbenstr. 30, Stuttgart, Germany;(4) Leibniz Institute for Tropospheric Research, Permoserstr. 15, Leipzig, Germany;(5) University of Hamburg, Institute for Inorganic and Applied Chemistry, Martin-Luther-King-Pl. 6, Hamburg, Germany;(6) Institute for the Environment and Sustainability, EC Joint Research Center, Ispra, Italy
Abstract:The change of the chemical composition of the near-ground level atmospheric aerosol was studied during two summer episodes by a Lagrangian type of experimental approach. Bulk and single-particle chemical analyses of ions and elements in the particulate phase were deployed. N(-III) and N(V) components were also measured in the gas-phase. The measurements were completed by particle size distributions.Secondary inorganic aerosols (SIA) and fine particles of ≈0.2–0.4 μm size were still elevated 50 km downwind of the city. The direct comparison of transport over the city in contrast to transport over the surrounding areas showed that SIA was formed from emission from the city within less than 3 h. Relative increases, i.e., enrichment during transport were observed for primary and secondary aerosol components. The degree of mixing on the individual particle level increased significantly during transport in the area. In particular, newly emitted carbonaceous particles became internally mixed within hours with pre-existing sulphate particles. Mostly due to secondary aerosol formation the average particle size (mass median diameter) of major constituents of the aerosol was significantly decreased while being transported over 13 h. Given recent insights which link fine particles number and mass concentrations with health risks, the results suggest that rural populations in areas which frequently are located within an urban plume might run an elevated health risk relative to populations in areas not affected by urban plumes.
Keywords:aerosol size distribution  secondary aerosol  single particle analysis  sulphur dioxide oxidation  urban plume
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