Preprints
https://doi.org/10.5194/acp-2021-1063
https://doi.org/10.5194/acp-2021-1063
 
19 Jan 2022
19 Jan 2022
Status: a revised version of this preprint is currently under review for the journal ACP.

Investigation of New Particle Formation mechanisms and aerosol processes at the Marambio Station, Antarctic Peninsula

Lauriane L. J. Quéléver1, Lubna Dada1,2,3, Eija Asmi4,5, Janne Lampilahti1, Tommy Chan1, Jonathan E. Ferrara4, Gustavo E. Copes4, German Pérez-Fogwill4, Luis Barreira5, Minna Aurela5, Douglas R. Worsnop1,6, Tuija Jokinen1,7, and Mikko Sipila1 Lauriane L. J. Quéléver et al.
  • 1Institute for Atmospheric and Earth System Research/INAR-Physics, P.O. Box 64, FI-00014 University of Helsinki, Finland
  • 2Extreme Environments Research Laboratory, École Polytechnique Fédérale de Lausanne (EPFL) Valais, Sion, 1951, Switzerland
  • 3Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
  • 4Servicio Meteorológico Nacional/SMN, Av. Dorrego, 4019, Buenos Aires, Argentina
  • 5Finnish Meteorological Institute/FMI, Erik Palmenin aukio 1, FI-00560 Helsinki, Finland
  • 6Aerodyne Research, Inc. Billerica, MA 01821, USA
  • 7The Cyprus Institute, The Climate & Atmosphere Research Centre (CARE-C), P.O. Box 27456 Nicosia, Cyprus

Abstract. Understanding chemical processes leading to the formation of atmospheric aerosol particles is crucial to improve our capabilities in predicting the future climate. However, those mechanisms are still inadequately characterized, especially in polar regions, which are typically representative of the pre-industrial era in climate models. In this study, we report observations of neutral and charged aerosol precursor molecules and chemical clusters composition (qualitatively and quantitatively), as well as air ions and aerosol particle number concentrations and size distributions from the Marambio research station (64°15'S–56°38'W), located North of the Antarctic Peninsula. We conducted measurements during the austral summer, between 15 January and 25 February 2018. The scope of this study is to characterize New Particle Formation (NPF) event parameters and connect our observations of gas phase compounds with the formation of secondary aerosols to resolve the nucleation mechanisms at the molecular scale. NPF occurred on 40% of measurement days (i.e., 13 NPF events were recorded during 35 days). All NPF events were observed during sunny days (i.e., sufficient radiation), mostly with above freezing temperatures and low relative humidity (RH < 80 %). The averaged formation rate for 3 nm particles (J3) was 0.686 cm−3 s−1 and the average particle growth rate (GR 3.8–12 nm) was 4.2 nm h−1. Analysis of neutral aerosol precursor molecules showed measurable concentrations of iodic acid (IA), sulfuric acid (SA) and methane sulfonic acid (MSA) throughout the entire measurement period with average concentrations of 5.17 × 105, 1.18 × 106, 2.06 × 105 molecules cm−3, respectively. MSA and SA concentrations significantly increased during NPF events. We highlight SA as a key contributor to NPF processes, while IA and MSA would likely only contribute to particle growth. Mechanistically, anion clusters of dimethylamine (DMA)-bisulfate (2SA) as well as numerous ammonium-(bi)sulfate clusters were identified, with the latter at mass-to-charge ratios (m/z) larger than 1000 Th. All of which suggests elevated concentration of both ammonia and amines in the atmosphere. Those species are likely contributing to NPF events since SA alone is not sufficient to explain observed nucleation rates. Here, we provide evidence of the marine origin of the measured chemical precursors and discuss their potential contribution to the aerosol phase. Our observations highlight the importance of the Antarctic Ocean, water, and ice ecosystems interacting with the land-fauna – the plausible sources of the principal precursor molecules hereby investigated – for secondary aerosol formation.

Lauriane L. J. Quéléver 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-2021-1063', Anonymous Referee #1, 14 Mar 2022
    • AC1: 'Reply on RC1', Lauriane L. J. Quéléver, 11 May 2022
  • RC2: 'Comment on acp-2021-1063', Farahnaz Khosrawi, 21 Mar 2022
    • AC2: 'Reply on RC2', Lauriane L. J. Quéléver, 11 May 2022
  • RC3: 'Comment on acp-2021-1063', Anonymous Referee #3, 01 Apr 2022
    • AC3: 'Reply on RC3', Lauriane L. J. Quéléver, 11 May 2022

Lauriane L. J. Quéléver et al.

Lauriane L. J. Quéléver et al.

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Short summary
Understanding how aerosol form is crucial to correctly model the climate and improve future predictions. This work provides an extensive analysis of aerosol particles and their precursors at the Marambio research Station, Antarctic Peninsula. We show that Sulfuric Acid, Ammonia and Dimethyl amine are key contributors for the frequent new particle formation events observed at site. We discuss nucleation mechanisms and highlight the need of targeted measurement to fully understand these processes.
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