Preprints
https://doi.org/10.5194/acp-2022-200
https://doi.org/10.5194/acp-2022-200
 
18 Mar 2022
18 Mar 2022
Status: this preprint is currently under review for the journal ACP.

Secondary aerosol formation in marine Arctic environments: A model measurement comparison at Ny-Ålesund

Carlton Xavier1, Metin Baykara1,2, Robin Wollesen de Jonge3, Barbara Altstädter4, Petri Clusius1, Ville Vakkari5,6, Roseline Thakur1, Lisa Beck1, Silvia Becagli7, Mirko Severi7, Rita Traversi7, Birgit Wehner8, Mikko Sipilä1, Markku Kulmala1, Michael Boy1, and Pontus Roldin3 Carlton Xavier et al.
  • 1Institute for Atmospheric and Earth Systems Research, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland
  • 2Climate and Marine Sciences Department, Eurasia Institute of Earth Sciences, Istanbul Technical University, Maslak 34469, Istanbul, Turkey
  • 3Division of Nuclear Physics, Department of Physics, Lund University, P. O. Box 118 SE-221 00 Lund, Sweden
  • 4Institute of Flight Guidance, Technische Universität Braunschweig, 38108 Braunschweig, Germany
  • 5Atmospheric Chemistry Research Group, Chemical Resource Beneficiation, North-West University, Potchefstroom, South Africa
  • 6Finnish Meteorological Institute, POBox 503, FI-00101 Helsinki, Finland
  • 7Department of Chemistry, University of Florence, Sesto Fiorentino, 50019 Florence, Italy
  • 8Institute of Tropospheric Research, 04318 Leipzig, Germany

Abstract. In this study, we modeled the aerosol particle formation along air mass trajectories arriving at the remote Arctic research stations Gruvebadet (67 m a.s.l) and Zeppelin (474 m a.s.l), Ny-Ålesund during May 2018. The aim of this study was to improve our understanding of processes governing secondary aerosol formation in remote Arctic marine environments. We run the Lagrangian chemistry transport model ADCHEM, along air mass trajectories generated with FLEXPART v10.4. The air masses arriving at Ny-Ålesund spend most of their time over the open ice-free ocean. In order to capture the secondary aerosol formation from the DMS emitted by phytoplankton on the ocean surface, we implemented a recently developed comprehensive DMS and halogen multi-phase oxidation chemistry scheme, coupled with the widely used Master Chemical Mechanism (MCM).

The modeled median particle number size distributions are in close agreement with the observations in the marine influenced boundary layer at near sea surface Gruvebadet site. However, while the model reproduces the accumulation mode particle number concentrations at Zeppelin, it overestimates the Aitken mode particle number concentrations by a factor of ~5.5. We attribute this to the deficiency of the model to capture the complex orographic effects on the boundary layer dynamics at Ny-Ålesund. The model also reproduces the average vertical particle number concentration profiles within the boundary layer (0–600 m a.s.l.) above Gruvebadet, as measured with Condensation Particle Counters (CPCs) on board an Unmanned Aircraft Systems (UAS).

The model successfully reproduces the observed Hoppel minima, often seen in particle number size distributions at Ny-Ålesund. The model also supports the previous experimental findings that ion mediated H2SO4-NH3 nucleation can explain the observed new particle formation in the marine Arctic boundary layer in the vicinity of Ny-Ålesund. Precursors resulting from gas and aqueous phase DMS chemistry contribute to the subsequent growth of the secondary aerosols. The growth of particles is primarily driven via H2SO4 condensation and formation of methane sulfonic acid (MSA) through the aqueous-phase ozonolysis of methane sulfinic acid (MSIA) in cloud and deliquescent droplets.

Carlton Xavier 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-2022-200', Anonymous Referee #1, 28 Apr 2022
  • RC2: 'Comment on acp-2022-200', Anonymous Referee #2, 29 Apr 2022

Carlton Xavier et al.

Carlton Xavier et al.

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Short summary
The focus of this work is to study and improve our understanding of processes involved in the formation and growth of new particle in remote Arctic marine environment. We run the 1-D model ADCHEM, along air mass trajectories arriving at Ny-Ålesund during May 2018. The model finds that ion mediated H2SO4-NH3 nucleation can explain the observed new particle formation at Ny-Ålesund. The growth of particles is driven via H2SO4 condensation and formation of methane sulfonic acid in aqueous phase.
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