Preprints
https://doi.org/10.5194/acp-2021-615
https://doi.org/10.5194/acp-2021-615

  06 Aug 2021

06 Aug 2021

Review status: this preprint is currently under review for the journal ACP.

Marine gas-phase sulfur emissions during an induced phytoplankton bloom

Delaney B. Kilgour1, Gordon A. Novak1, Jon S. Sauer2, Alexia N. Moore2, Julie Dinasquet3, Sarah Amiri2, Emily B. Franklin4, Kathryn Mayer2, Margaux Winter5, Clare K. Morris3, Tyler Price2, Francesca Malfatti3,6, Daniel R. Crocker2, Christopher Lee3, Christopher D. Cappa7, Allen H. Goldstein4,8, Kimberly A. Prather2,3, and Timothy H. Bertram1 Delaney B. Kilgour et al.
  • 1Department of Chemistry, University of Wisconsin – Madison, Madison, WI 53706, USA
  • 2Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093, USA
  • 3Scripps Institution of Oceanography, University of California, San Diego, La Jolla, CA 92037, USA
  • 4Department of Civil and Environmental Engineering, University of California, Berkeley, CA 94720, USA
  • 5Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA
  • 6Department of Life Sciences, Universita’ degli Studi di Trieste, Trieste, Italy 34127
  • 7Department of Civil and Environmental Engineering, University of California, Davis, CA 95616, USA
  • 8Department of Environmental Science, Policy and Management, University of California, Berkeley, CA 94720, USA

Abstract. The oxidation of dimethyl sulfide (DMS; CH3SCH3), emitted from the surface ocean, contributes to the formation of Aitken mode particles and their growth to cloud condensation nuclei (CCN) sizes in remote marine environments. It is not clear whether other, less commonly measured marine-derived, sulfur-containing gases share similar dynamics to DMS and contribute to secondary marine aerosol formation. Here, we present measurements of gas-phase volatile organosulfur molecules taken with a Vocus proton transfer reaction high resolution time-of-flight mass spectrometer during a mesocosm phytoplankton bloom experiment using coastal seawater. We show that DMS, methanethiol (MeSH; CH3SH), and benzothiazole (C7H5NS) account for on average over 90 % of total gas-phase sulfur emissions, with non-DMS sulfur sources representing 36.8 ± 7.7 % of sulfur emissions during the first nine days of the experiment in the pre-bloom phase prior to major biological growth, before declining to 14.5 ± 6.0 % in the latter half of the experiment when DMS dominates during the bloom and decay phases. The molar ratio of DMS to MeSH during the pre-bloom phase (DMS : MeSH = 4.60 ± 0.93) was consistent with the range of previously calculated ambient DMS to MeSH sea-to-air flux ratios. As the experiment progressed, the DMS to MeSH emission ratio increased significantly, reaching 31.8 ± 18.7 during the bloom and decay. Measurements of dimethylsulfoniopropionate (DMSP), heterotrophic bacteria, and enzyme activity in the seawater suggest the DMS : MeSH ratio is a sensitive indicator of the bacterial sulfur demand and the composition and magnitude of available sulfur sources in seawater. The evolving DMS : MeSH ratio and the emission of a new aerosol precursor gas, benzothiazole, have important implications for secondary sulfate formation pathways in coastal marine environments.

Delaney B. Kilgour 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-2021-615', Anonymous Referee #1, 10 Sep 2021
  • RC2: 'Comment on acp-2021-615', Anonymous Referee #2, 14 Oct 2021

Delaney B. Kilgour et al.

Delaney B. Kilgour et al.

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Short summary
We report measurements of gas-phase volatile organosulfur molecules made during a mesocosm phytoplankton bloom experiment. Dimethyl sulfide (DMS), methanethiol (MeSH), and benzothiazole accounted for on average over 90 % of total gas-phase sulfur emissions. This work focuses on factors controlling the production and emission of DMS and MeSH and the role of non-DMS molecules (such as MeSH and benzothiazole) in secondary sulfate formation in coastal marine environments.
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