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Preprints
https://doi.org/10.5194/acp-2020-284
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-284
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 22 Jun 2020

Submitted as: research article | 22 Jun 2020

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This preprint is currently under review for the journal ACP.

Halogen activation in the plume of Masaya volcano: field observations and box model investigations

Julian Rüdiger1,2, Alexandra Gutmann1, Nicole Bobrowski3,4, Marcello Liotta5, J. Maarten de Moor6, Rolf Sander4, Florian Dinger3,4, Jan-Lukas Tirpitz3, Martha Ibarra7, Armando Saballos7, María Martínez6, Elvis Mendoza7, Arnoldo Ferrufino7, John Stix8, Juan Valdés9, Jonathan M. Castro10, and Thorsten Hoffmann1 Julian Rüdiger et al.
  • 1Institute of Inorganic and Analytical Chemistry, Johannes Gutenberg-University, Mainz, Germany
  • 2Chair of Environmental Chemistry and Air Research, Technical University Berlin, Berlin, Germany
  • 3Institute for Environmental Physics, University of Heidelberg, Heidelberg, Germany
  • 4Max-Planck Institute for Chemistry, Mainz, Germany
  • 5Istituto Nazionale di Geofisica e Vulcanologia, Sezione di Palermo, Italy
  • 6Observatorio Vulcanológico y Sismológico de Costa Rica Universidad Nacional, Heredia, Costa Rica
  • 7Instituto Nicaragüense de Estudios Territoriales, Nicaragua
  • 8Department of Earth and Planetary Sciences, McGill University, Montreal, Canada
  • 9Laboratorio de Química de la Atmósfera, Universidad Nacional, Heredia, Costa Rica
  • 10Institute of Geosciences, Johannes Gutenberg University Mainz, Mainz, Germany

Abstract. Volcanic emissions are a source of halogens to the atmosphere. Rapid reactions convert the initially emitted hydrogen halides (HCl, HBr, HI) into reactive species e.g. BrO, Br2, BrCl, ClO, OClO and IO. The activation reaction mechanisms in the plume consume ozone (O3), which is entrained by in-mixed ambient air. In this study, we present observations of the oxidation of bromine, chlorine and iodine during the first 11 minutes after emission, investigating the plume of Santiago Crater of Masaya volcano in Nicaragua. Two field campaigns were conducted, in July 2016 and September 2016. The sum of the reactive species of the respective halogens were determined by gas diffusion denuder sampling followed by GC-MS analysis, while the total amounts of halogens and sulfur amounts were obtained by alkaline trap sampling with subsequent IC and ICP-MS measurements. Both ground and airborne sampling with an unmanned aerial vehicle (including a denuder sampler in combination with an electrochemical SO2 sensor) was performed at different distances from the crater rim. The in-situ measurements were accompanied by remote sensing observations (DOAS). For bromine, the reactive fraction increased from 0.20 ± 0.13 at the crater rim to 0.76 ± 0.26 at 2.8 km downwind, while chlorine showed an increase of the reactive fraction from (2.7 ± 0.7) × 10−4 to (11 ± 3) × 10−4 in the first 750 m. Additionally, a reactive iodine fraction of 0.3 at the crater rim and 0.9 at 2.8 km was measured. No significant increase in BrO / SO2 molar ratios was observed with the estimated age of the observed plume ranging from 1.4 min to 11.1 min. This study presents a comprehensive gas diffusion denuder data set on reactive halogen species and compares BrO / SO2 ratios with the sum of all reactive Br species. With the observed field data, a chemistry box model (CAABA/MECCA) enabled the reproduction of the observed progression of the reactive bromine to total bromine ratio. An observed contribution of BrO to the reactive bromine fraction of about 10 % was reproduced in the first minutes of the model run. The model results emphasize the importance of ozone entrainment into the plume for the reproduction of the measured reactive bromine formation and the dependence on the availability of HXOY and NOX.

Julian Rüdiger et al.

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Short summary
We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in Nicaragua. An unique data set was collected by employing multiple techniques, including drones. This data enabled us to determine the fraction of activation of the respective halogens at various plume ages, where in-mixing of ambient air causes chemical reactions. An atmospheric chemistry box model was employed to further examine the field results and help our understanding of volcanic plume chemistry.
We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in...
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