Investigation of New Particle Formation mechanisms and aerosol processes at the Marambio Station, Antarctic Peninsula
- 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
- 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.
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Lauriane L. J. Quéléver et al.
Status: final response (author comments only)
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RC1: 'Comment on acp-2021-1063', Anonymous Referee #1, 14 Mar 2022
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2021-1063/acp-2021-1063-RC1-supplement.pdf
- AC1: 'Reply on RC1', Lauriane L. J. Quéléver, 11 May 2022
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RC2: 'Comment on acp-2021-1063', Farahnaz Khosrawi, 21 Mar 2022
Editor review on the paper “Investigations of New Particle Formation mechanisms and aerosol processes at the Marambio Station, Antarctic Peninsula” by Quéléver et al.
Since the second referee report is still missing, I will provide a review so that the open discussion can be closed. Quéléver et al. present an extensive study on new particle formation using data derived during a measurement campaign at Marambio station in 2018. The paper is generally well written and I only have suggestions for minor revisions.
Generally:
For the next submission it would be good if you could use the ACP manuscript style (line spacing, font size etc. See templates on the ACP webpage: https://www.atmospheric-chemistry-and-physics.net/submission.html#manuscriptcomposition). The manuscript was as it was published as preprint quite difficult to read (e.g. too small font).
Line numbering: On the first few pages you start numbering again with each page, but the second half of the manuscript the numbering continues until the end. Should be done one or the other way, but not mixed. Also here I would suggest to check the ACP guidelines which is the correct style.
Specific comments:
Abstract: The abstract is quite long and my impression is that you go between L36 and L41 too much into detail. I am not sure if it is really necessary to list here all the numbers. I would suggest to rather do that in the summary and shorten these lines here in the abstract.
P3, L21: “sufficiently away from the station…….”. Add here why. I assume it’s to avoid that the measurements are affected by the station. Would be good to clearly state this.
P5, L12: Add here “by collision and coalescence”, so that it reads ”are lost to pre-existing particles by collision and coalescence” to be more precise.
P5, L24: Also here I would suggest to add bit more information. How accurate is the approach by Kulmala et al. (2022)?
P7, L28: Why these numbers? Why do you pick these size ranges? An explanation/justification is missing.
P8, L10-11: Sentence not clear. Please rephrase.
P13, Fig. 6 and according text: This kind of analyses is new for me and I could not follow what actually the mass defect is and would you try to extract from it. Some more motivation/explanations are required.
P14, L116: I have difficulties to follow you. To what is the “high intensity” referring to?
P14, L133: orange dots? To which figure are you referring to? Figure 6?
P14, L140: Yellow and green dots? Same here. To which figure are you referring to?
P14, L143-147: Sentence not clear. Please rephrase. Maybe it’s better to split this sentence into two and check the grammar.
P15, L162: Add “aerosols” so that it reads “sea salt aerosols”?
Technical corrections:
P2, L4: Ipcc → IPCC
P2, L5: Add a reference?
P2, L28ff: To my knowledge this are not the only references on these aerosol compositions, thus I would suggest to add “e.g.” before the references.
P3, L1-10: I would suggest to add here references to the respective chapters.
P5, L49: aera → area
P7, Fig 2 caption: here “a)” etc in bold face instead of “(a)” as normal text. Be consistent and check ACP guidelines for which way of writing should be used.
P7, L23: changed → changes
P7, L25: appear → appeared
P8, L33: particle → particles
P11, L39: concentration → concentrations
P11, L42: add “is” so that it reads “that IA is even anticorrelated with…...”
P11, L46: concentration → concentrations
P11, L47: concentration → concentrations
P11, 3.3.2 Header: Study case of → case study on
P13, L104: noise to signal → signal to noise
P14, L124: rate → rates
P14, L134: Add “the” → have shown the possible roles
P15, L192: Add “the” → in the Supplementary
P16, L213: concentration → concentrations
P17, L221: emission → emissions
P17, L236: study case → case study
P17, L238: pathway proceeds → pathways proceeds
P17, L240: than negative → than the negative
P17, L241: should → could
P17, L246: in CLOUD-chamber CERN → in the CLOUD-chamber CERN
P17, L247: Add “that” and use plural: indicate that very high concentrations
P18, L299: in turns → in turn
P18, L299: source → sources
P18, L308: “by key well known”? “key” obsolete?
- AC2: 'Reply on RC2', Lauriane L. J. Quéléver, 11 May 2022
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RC3: 'Comment on acp-2021-1063', Anonymous Referee #3, 01 Apr 2022
I congratulate the authors for the excellent paper, this is a ground breaking paper with lots of excellent measurements.
I suggest publication on ACP following minor revisions:
1) The authors seem not to give importance to sympagic sea ice areas as a source of organic nitrogen, as discussed in Dall´Osto et al (2017), Dall´Osto et al (2019) and Rinaldi et al (2020) - given the fact it is a likely source of an important gaseous precursors, it may be worth to bring it into discussions
2) Following this, I am afraid the discussion on point 4 on page 17 is somehow hard to follow. The authors report 13 nucleation events: event 1 and 3 have high GR, event 6,9,10 have very high J. The authors then decide to reports an important case study for the last day (event 12 and 13). However, the discussion of the wind roses is rather weak. The whole interesting event of the case study event (high organic nitrogen) has the opposite wind roses of the claimed pinguin colonies. Also, event 6,7,8,9 have contrasting wind roses - so there must be some influence from the contrary sector (again coincidentally open pack sea ice regions around Marambio).
Following the points above, please consider to address other possible source regions. On this regards, you may want to consider to run concentration weitghted trajection for particle formation rate or to see where these particles may originate - the dataset is a brilliant one and worth analyzing a bit more in detail. Also, only one mass defect plot is presented (Figure 6). This is unusual, on previous papers (ie Antarctic measurements in Jokinen et al., 2018) mass defect api-tof measurements for each NPF events were presente - may be worth reporting them in supporting information
I congratulate once again for the brilliant dataset produced and the well presented paper, I hope these modifications can be considered before accepting the paper.
- 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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