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  Chemical composition and source attribution of submicron aerosol particles in the summertime Arctic lower troposphere

Köllner, F., Schneider, J., Willis, M. D., Schulz, H., Kunkel, D., Bozem, H., et al. (2020). Chemical composition and source attribution of submicron aerosol particles in the summertime Arctic lower troposphere. Atmospheric Chemistry and Physics Discussions, 20. doi:10.5194/acp-2020-742.

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Köllner, Franziska1, Author              
Schneider, Johannes1, Author              
Willis, Megan D., Author
Schulz, Hannes, Author
Kunkel, Daniel, Author
Bozem, Heiko, Author
Hoor, Peter, Author
Klimach, Thomas2, Author              
Helleis, Frank3, Author              
Burkart, Julia, Author
Leaitch, W. Richard, Author
Alibadi, Amir A., Author
Abbatt, Jonathan P. D., Author
Herber, Andreas B., Author
Borrmann, Stephan1, Author              
Affiliations:
1Particle Chemistry, Max Planck Institute for Chemistry, Max Planck Society, ou_1826291              
2Multiphase Chemistry, Max Planck Institute for Chemistry, Max Planck Society, ou_1826291              
3Max Planck Institute for Chemistry, Max Planck Society, ou_1826284              

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 Abstract: We use airborne measurements of aerosol particle composition to demonstrate the strong contrast between particle sources and composition within and above the summertime Arctic boundary layer. In-situ measurements from two complementary aerosol mass spectrometers, the ALABAMA and the HR-ToF-AMS, with black carbon measurements from an SP2 are presented. Particle composition analysis was complemented by trace gas measurements, satellite data, and air mass history modeling to attribute particle properties to particle origin and air mass source regions. Particle composition above the summertime Arctic boundary layer was dominated by chemically aged particles, containing elemental carbon, nitrate, ammonium, sulfate, and organic matter. From our analysis, we conclude that the presence of these particles was driven by transport of aerosol and precursor gases from mid-latitudes to Arctic regions. Particularly, elevated concentrations of nitrate, ammonium, and organic matter coincided with time spent over vegetation fires in northern Canada. In parallel, those particles were largely present in high CO environments (> 90 ppbv). Additionally, we observed that the organic-to-sulfate ratio was enhanced with increasing influence from these fires. Besides vegetation fires, particle sources in mid-latitudes further include anthropogenic emissions in Europe, North America, and East Asia. The presence of particles in the Arctic lower free troposphere correlated with time spent over populated and industrial areas in these regions. Further, the size distribution of free tropospheric particles containing elemental carbon and nitrate was shifter to larger diameters compared to particles present within the boundary layer. Moreover, our analysis suggests that organic matter when present in the Arctic free troposphere can partly be identified as low-molecular weight dicarboxylic acids (oxalic, malonic, and succinic acid). Particles containing dicarboxylic acids were largely present when the residence time of air masses outside Arctic regions was high. In contrast, particle composition within the marine boundary layer was largely driven by Arctic regional processes. Air mass history modeling demonstrated that alongside primary sea spray particles, marine-biogenic sources contributed to secondary aerosol formation by trimethylamine, methanesulfonic acid, sulfate, and other organic species.

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Language(s): eng - English
 Dates: 2020-08-03
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: No review
 Identifiers: DOI: 10.5194/acp-2020-742
 Degree: -

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Title: Atmospheric Chemistry and Physics Discussions
  Abbreviation : Atmos. Chem. Phys. Discuss.
Source Genre: Journal
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Publ. Info: Katlenburg-Lindau, Germany : European Geophysical Society, Copernicus Publ.
Pages: 39 Volume / Issue: 20 Sequence Number: - Start / End Page: - Identifier: ISSN: 1680-7367
CoNE: https://pure.mpg.de/cone/journals/resource/111076360006006