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https://doi.org/10.5194/acp-2020-636
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-636
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  10 Sep 2020

10 Sep 2020

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This preprint is currently under review for the journal ACP.

Investigation of several proxies to estimate sulfuric acid concentration in volcanic plume conditions

Clémence Rose1, Matti P. Rissanen2,3, Siddharth Iyer2, Jonathan Duplissy3,4, Chao Yan3, John B. Nowak5, Aurélie Colomb1, Régis Dupuy1, Xu-Cheng He3, Janne Lampilahti3, Yee Jun Tham3, Daniela Wimmer3, Jean-Marc Metzger6, Pierre Tulet7, Jérôme Brioude7, Céline Planche1, Markku Kulmala3, and Karine Sellegri1 Clémence Rose et al.
  • 1Université Clermont Auvergne, CNRS, Laboratoire de Météorologie Physique (LaMP), F-63000 Clermont-Ferrand, France
  • 2Aerosol Physics Laboratory, Physics Unit, Tampere University, Tampere, Finland
  • 3Institute for Atmospheric and Earth System Research INAR/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
  • 4Helsinki Institute of Physics, University of Helsinki, Helsinki, Finland
  • 5Chemistry and Dynamics Branch, NASA Langley Research Center, Hampton, VA 23681, USA
  • 6Observatoire des Sciences de l'Univers de La Réunion, UMS 3365 (CNRS, Université de La Réunion, Météo-France), 97744 Saint Denis de La Réunion, France
  • 7LACy, Laboratoire de l'Atmosphère et des Cyclones, UMR8105 (CNRS, Université de La Réunion, Météo-France), Saint-Denis de la Réunion, France

Abstract. Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation (NPF). However, direct measurements of [H2SO4] remain challenging, thus preventing the determination of this important quantity, and, consequently, a complete understanding of its contribution to the NPF process. Several proxies have been developed to bridge the gaps, but their ability to predict [H2SO4] in very specific conditions such as those encountered in volcanic plumes (including in particular high sulphur dioxide mixing ratios) has not been evaluated so far. In this context, the main objective of the present study was to develop new proxies for daytime [H2SO4] in volcanic plume conditions and compare their performance to that of the proxies available in the literature. In specific, the data collected at Maïdo during the OCTAVE 2018 campaign, in the volcanic eruption plume of the Piton de la Fournaise, were first used to derive seven proxies based on the knowledge of sulphur dioxide (SO2) mixing ratio, global radiation, condensation sink (CS) and relative humidity (RH). In three of the seven proxies (F1–F3), all variables were given equal weight in the prediction of [H2SO4], while adjusted powers were allowed for the different variables in the other four proxies (A1–A4). Proxies A1–A4 were overall found to perform better compared to F1–F3, with, in specific, improved predictive ability for [H2SO4] > 2 × 108 cm−3. The CS was observed to play an important role in regulating [H2SO4], while, in contrast, the inclusion of RH did not improve the predictions. A last expression accounting for an additional sink term related to cluster formation, S1, was also tested and showed a very good predictive ability over the whole range of measured [H2SO4]. The newly developed proxies were in a second step further evaluated using airborne measurements performed in the passive degassing plume of Etna during the STRAP 2016 campaign. Increased correlations between observed and predicted [H2SO4] were obtained when the dependence of predicted [H2SO4] over CS was the lowest, and when the dependence over [SO2] was concurrently the highest. The best predictions were finally retrieved by the simple formulation of F2 (in which [SO2] and radiation alone were assumed to explain the variations of [H2SO4] with equal contributions), with a pre factor adapted to the STRAP data. All in all, our results illustrate the fairly good capacity of the proxy available in the literature to describe [H2SO4] in volcanic plume conditions, but highlight at the same time the benefit of the newly developed proxies for the prediction of the highest concentrations ([H2SO4] > 2–3 × 108 cm−3). Also, the contrasting behaviours of the new proxies in the two investigated datasets indicate that in volcanic plumes like in other environments, the relevance of a proxy can be affected by changes in environmental conditions, and that location specific coefficients do logically improve the predictions.

Clémence Rose et al.

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Short summary
Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, thus motivating the development of proxies. Using data collected in two different volcanic plumes, we show, in these specific conditions, the good performance of a proxy from the literature and highlight as well the benefit of the newly developed proxies for the prediction of the highest [H2SO4] concentrations.
Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle...
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