Preprints
https://doi.org/10.5194/egusphere-2022-887
https://doi.org/10.5194/egusphere-2022-887
 
23 Sep 2022
23 Sep 2022

Measurement Report: Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes

Wiebke Scholz1,, Jiali Shen2,, Diego Aliaga2, Cheng Wu3,10, Samara Carbone5, Isabel Moreno4, Qiaozhi Zha2, Wei Huang2, Liine Heikkinen2,3, Jean Luc Jaffrezo6, Gaelle Uzu6, Eva Partoll1, Markus Leiminger1, Fernando Velarde4, Paolo Laj6,2, Patrick Ginot6, Paolo Artaxo7, Alfred Wiedensohler8, Markku Kulmala2, Claudia Mohr3, Marcos Andrade4,9, Victoria Sinclair2, Federico Bianchi2, and Armin Hansel1 Wiebke Scholz et al.
  • 1Institute for Ion and Applied Physics, University of Innsbruck, Innsbruck, Austria
  • 2Institute for Atmospheric and Earth System Research /Physics, University of Helsinki, Helsinki, Finland
  • 3Department of Environmental Science and Bolin Centre for Climate Research, Stockholm University, Stockholm, Sweden
  • 4Laboratory for Atmospheric Physics, Institute for Physics Research, Universidad Mayor de San Andrés, La Paz, Bolivia
  • 5Federal University of Uberlândia, Uberlândia, MG, Brazil
  • 6University Grenoble Alpes, CNRS, IRD, INP-G, IGE (UMR 5001), 38000 Grenoble, France
  • 7Institute of Physics, University of Sao Paulo, Sao Paulo, SP, Brazil
  • 8Experimental Aerosol and Cloud Microphysics, Leibniz Institute for Tropospheric Research, Leipzig, Germany
  • 9Department of Atmospheric and Oceanic Sciences, University of Maryland, College Park, MD 20742
  • 10Department of Chemistry and Molecular Biology, Atmospheric Science, University of Gothenburg, SE-412 96 Gothenburg, Sweden
  • These authors contributed equally to this work.

Abstract. Dimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products H2SO4, MSA, DMSO, DMSO2, MSIA, MTF, CH3S(O)2OOH and CH3SOH in the gas-phase as well as measurements of the sulfate and methane- sulfonate aerosol mass fractions at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240 m above sea level (a.s.l.).

DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000–8000 m a.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs dimethyl sulfone (DMSO2) in the gas phase and methanesulfonate (MS) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethyl sulfoxide, and methane sulfinic acid. Also for this event, backtrajectory calculations show, that the air masses came from above the ocean (distance >330 km) with no local sur- face contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.

Journal article(s) based on this preprint

19 Jan 2023
Measurement report: Long-range transport and the fate of dimethyl sulfide oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023,https://doi.org/10.5194/acp-23-895-2023, 2023
Short summary

Wiebke Scholz et al.

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • AC1: 'Comment on egusphere-2022-887', Wiebke Scholz, 28 Sep 2022
  • RC1: 'Referee comment on egusphere-2022-887', Anonymous Referee #1, 05 Oct 2022
    • AC2: 'reply to RC1 - discussing open questions', Wiebke Scholz, 10 Oct 2022
  • RC2: 'Comment on egusphere-2022-887', Anonymous Referee #2, 29 Nov 2022

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • AC1: 'Comment on egusphere-2022-887', Wiebke Scholz, 28 Sep 2022
  • RC1: 'Referee comment on egusphere-2022-887', Anonymous Referee #1, 05 Oct 2022
    • AC2: 'reply to RC1 - discussing open questions', Wiebke Scholz, 10 Oct 2022
  • RC2: 'Comment on egusphere-2022-887', Anonymous Referee #2, 29 Nov 2022

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision
AR by Wiebke Scholz on behalf of the Authors (13 Dec 2022)  Author's response    Author's tracked changes    Manuscript
ED: Publish as is (22 Dec 2022) by Marc von Hobe

Journal article(s) based on this preprint

19 Jan 2023
Measurement report: Long-range transport and the fate of dimethyl sulfide oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023,https://doi.org/10.5194/acp-23-895-2023, 2023
Short summary

Wiebke Scholz et al.

Data sets

Data and Code for figures of "Long-range transport and fate of DMS-oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes" Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean-Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, Armin Hansel https://doi.org/10.5281/zenodo.6866115

Wiebke Scholz et al.

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Short summary
Dimethyl sulfide (DMS), emitted from the ocean, is the most abundant biogenic sulfur emission into the atmosphere. OH radicals, among others, can oxidize DMS to sulfuric and methanesulfonic acid, which are relevant for aerosol formation. We quantified DMS and nearly all DMS oxidation products with novel mass spectrometric instruments for gas and particle phase at the high mountain station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes in free tropospheric air after long-range transport.