Chemical composition and source attribution of sub-micrometre aerosol particles in the summertime Arctic lower troposphere

• Published in: Atmospheric Chemistry and Physics
• Main Authors: Köllner, F., Schneider, J., Willis, M., Schulz, H., Kunkel, D., Bozem, H., Hoor, P., Klimach, T., Helleis, F., Burkart, J., Leaitch, W., Aliabadi, A., Abbatt, J., Herber, A., Borrmann, S.
• Format: Article in Journal/Newspaper
• Language: unknown
• Published: 2021
• Subjects: Arctic; Canada; Alabama; black carbon
• Online Access: http://hdl.handle.net/21.11116/0000-0008-9EF0-7

Aerosol particles impact the Arctic climate system both directly and indirectly by modifying cloud properties, yet our understanding of their vertical distribution, chemical composition, mixing state, and sources in the summertime Arctic is incomplete. In situ vertical observations of particle properties in the high Arctic combined with modelling analysis on source attribution are in short supply, particularly during summer. We thus 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 Aircraft-based Laser Ablation Aerosol Mass Spectrometer (ALABAMA) and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), are presented alongside black carbon measurements from an single particle soot photometer (SP2). Particle composition analysis was complemented by trace gas measurements, satellite data, and air mass history modelling 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. Specifically, 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 ...