15 Feb 2022
15 Feb 2022
Status: a revised version of this preprint is currently under review for the journal ACP.

Possible controls on Arctic clouds by natural aerosols from long-range transport of biogenic emissions and ozone depletion events

Rupert Holzinger1, Oliver Eppers2,3, Kouji Adachi4, Heiko Bozem2, Markus Hartmann5,a, Andreas Herber6, Makoto Koike7, Dylan B. Millet8, Nobuhiro Moteki7, Sho Ohata7,b,c, Frank Stratmann5, and Atsushi Yoshida7,d Rupert Holzinger et al.
  • 1Institute for Marine and Atmospheric Research, Utrecht (IMAU), Utrecht University, The Netherlands
  • 2Johannes Gutenberg University of Mainz, Institute for Atmospheric Physics, Mainz, Germany
  • 3Particle Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
  • 4Department of Atmosphere, Ocean, and Earth System Modeling Research, Meteorological Research Institute, Tsukuba, Japan
  • 5Atmospheric Chemistry Department (ACD), Leibniz-Institute for Tropospheric Research (TROPOS), Leipzig, Germany
  • 6Alfred Wegener Institute Helmholtz Centre for Polar and Marine Research (AWI), Bremerhaven, Germany
  • 7Department of Earth and Planetary Science, Graduate School of Science, The University of Tokyo, Tokyo, Japan
  • 8University of Minnesota, Saint Paul, MN, USA
  • anow at: Atmospheric Science, Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden
  • bnow at: Institute for Space–Earth Environmental Research, Nagoya University, Nagoya, Aichi, Japan
  • cnow at: Institute for Advanced Research, Nagoya University, Nagoya, Aichi, Japan
  • dnow at: National Institute of Polar Research, Tokyo, Japan

Abstract. During the PAMARCMiP 2018 campaign (March and April 2018) a proton-transfer-reaction mass spectrometer (PTR-MS) was deployed onboard the POLAR 5 research aircraft and sampled the high Arctic atmosphere under Arctic haze conditions. More than 100 compounds exhibited levels above 1 pmol/mol in at least 25 % of the measurements. We used back trajectories and acetone mixing ratios to identify periods with and without long-range transport from continental sources.

Air masses with continental influence contained elevated levels of compounds associated with aged biogenic emissions and anthropogenic pollution (e.g., methanol, peroxyacetylnitrate (PAN), acetone, acetic acid, methylethylketone (MEK), proprionic acid, and pentanone). Almost half of all positively detected compounds (> 100) in the High Arctic atmosphere can be associated with terpene oxidation products. This may constitute a signature of biogenic terpenes and their oxidation products on the high Arctic atmosphere. Many of these compounds will condense and produce biogenic secondary organic aerosol (SOA) – a natural source of organic aerosol (OA) in addition to the aerosols that can be associated with pollution. Therefore, we hypothesize that biogenic SOA may have exerted significant control over the complex system of aerosols, clouds and longwave radiation in the pre-industrial Arctic winter, even though their role is likely marginal under contemporary polluted Arctic haze conditions. However, biogenic SOA may become an important factor in the futRure again, if biogenic emissions are enhanced due to climate change and if polluting technologies are phased out in the future.

During two flights, surface ozone depletion events (ODE) were observed that coincided with enhanced levels of acetone, and methylethylketone. There is evidence that ODEs may also be associated with the emission of biogenic ice-nucleating particles (INP) because the filter samples taken during these two flights exhibited enhanced levels of highly active INP.

Both these processes, INP production in association with ozone depletion events, and the transport of biogenic SOA could require corrections in estimates of Arctic change. If the preindustrial effects from these natural factors was stronger than is thought, subsequent climate changes over the Arctic may be larger than currently assumed.

Rupert Holzinger et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2022-95', Anonymous Referee #1, 04 Apr 2022
  • RC2: 'Comment on acp-2022-95', Anonymous Referee #2, 15 Apr 2022
  • AC1: 'answer to reviewer comments', Rupert Holzinger, 25 May 2022

Rupert Holzinger et al.

Rupert Holzinger et al.


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Short summary
In spring 2018 the research aircraft Polar 5 conducted flights in the Arctic atmosphere. The flight operation was from Station Nord in Greenland, 1700 km north of the Arctic Circle (81°43'N, 17°47'W). Using a mass spectrometer we measured more than 100 organic compounds in the air. We found a clear signature of natural organic compounds that are transported from forests to the high Arctic. These compounds have the potential to change the cloud cover and energy budget of the Arctic region.