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Discussion papers
https://doi.org/10.5194/acp-2019-102
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-102
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 18 Mar 2019

Submitted as: research article | 18 Mar 2019

Review status
This discussion paper is a preprint. A revision of the manuscript is under review for the journal Atmospheric Chemistry and Physics (ACP).

Using airborne observations to improve estimates of short-lived halocarbon emissions during summer from Southern Ocean

Elizabeth Asher1, Rebecca S. Hornbrook2, Britton B. Stephens1, Doug Kinnison1, Eric J. Morgan5, Ralph F. Keeling5, Elliot L. Atlas6, Sue M. Schauffler1, Simone Tilmes1, Eric A. Kort2, Martin S. Hoecker-Martínez3, Matt C. Long1, Jean-François Lamarque1, Alfonso Saiz-Lopez4,1, Kathryn McKain7,8, Colm Sweeney8, Alan J. Hills1, and Eric C. Apel1 Elizabeth Asher et al.
  • 1National Center for Atmospheric Research, Boulder, Colorado, USA
  • 2University of Michigan, Climate and Space Sciences and Engineering, Ann Arbor, Michigan, USA
  • 3University of Redlands, Physics Department, Redlands, California, USA
  • 4Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Madrid, Spain
  • 5Scripps Institution of Oceanography, University of California, San Diego, California, USA
  • 6University of Miami, Department of Atmospheric Sciences, Miami, Florida, USA
  • 7Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado, USA
  • 8National Oceanic and Atmospheric Administration, Boulder, Colorado, USA

Abstract. We present observations of CHBr3, CH2Br2, CH3I, CHClBr2, and CHBrCl2 from the Trace Gas Organic Analyzer (TOGA) during the O2/N2 Ratio and CO2 Airborne Southern Ocean (ORCAS) study and the 2nd Atmospheric Tomography mission (ATom-2), in January and February of 2016 and 2017. We also use CH3Br from the University of Miami Advanced Whole Air Sampler (AWAS) on ORCAS and from the UC Irvine Whole Air Sampler (WAS) on ATom-2. We compare our observations with simulations from the Community Atmosphere Model with Chemistry (CAM-Chem). We report regional enrichment ratios of CHBr3 and CH2Br2 to O2 of 0.19 ± 0.01, and 0.07 ± 0.004 pmol : mol, poleward of 60° S between 180° W and 55° W, and of 0.32 ± 0.02, 0.07 ± 0.004 pmol : mol over the Patagonian Shelf, between 40° S and 55° S and between 70° W and 55° W where we also report enrichment ratios of CH3I to O2 of 0.38 ± 0.03 pmol : mol and of CH2ClBr2 to O2 of 0.19 ± 0.04 pmol: mol. Using the Stochastic Time-Inverted Lagrangian Transport (STILT) particle dispersion model, we use correlations between halogenated hydrocarbon mixing ratios and the upwind influences of chlorophyll a, sea ice, solar radiation, and dissolved organic material to investigate previously hypothesized sources of halogenated volatile organic compounds (HVOCs) in the southern high latitudes. Our results are consistent with a biogenic regional source of CHBr3, and both non-biological and biological sources of CH3I over these regions, but do not corroborate a regional sea-ice source of HVOCs in January and February. Based on these relationships, we estimate the average two-month (Jan.-Feb.) emissions poleward of 60° S between 180° W and 55° W of CHBr3, CH2Br2, CH3I, and CHClBr2 to be 91 ± 8, 31 ± 17, 35 ± 29, and 11 ± 4 pmol m−2 hr−1, and regional emissions of these gases over the Patagonian Shelf to be 329 ± 23, 69 ± 5, 392 ± 32, 24 ± 4 pmol m−2 hr−1 respectively.

Elizabeth Asher et al.
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Elizabeth Asher et al.
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Short summary
Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer, and compares them to a global climate model simulation. In addition, we evaluate hypothesized regional sources and estimate emissions of these trace gases through their relationships to additional aircraft observations.
Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere,...
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