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Discussion papers
https://doi.org/10.5194/acp-2019-866
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-866
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 16 Oct 2019

Submitted as: research article | 16 Oct 2019

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Missing OH Reactivity in the Global Marine Boundary Layer

Alexander B. Thames1, William H. Brune1, David O. Miller1, Hannah M. Allen4, Eric C. Apel2, Donald R. Blake15, T. Paul Bui8, Roisin Commane14, John D. Crounse4, Bruce C. Daube13, Glenn S. Diskin5, Joshua P. DiGangi5, James W. Elkins10, Samuel R. Hall2, Thomas F. Hanisco6, Reem A. Hannun6,7, Eric Hintsa10,12, Rebecca S. Hornbrook2, Michelle J. Kim3, Kathryn McKain10,12, Fred L. Moore10,12, Julie M. Nicely6,7, Jeffrey Peischl10,11, Thomas B. Ryerson11, Jason M. St. Clair6,7, Colm Sweeney9, Alex Teng4, Chelsea R. Thompsona,11,12, Kirk Ullmann2, Paul O. Wennberg3, and Glenn M. Wolfe6,7 Alexander B. Thames et al.
  • 1Department of Meteorology and Atmospheric Science, The Pennsylvania State University, University Park, PA, USA
  • 2Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
  • 3Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
  • 4Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA, USA
  • 5Chemistry and Dynamics Branch, NASA Langley Research Center, Hampton, VA, USA
  • 6Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, MD, USA
  • 7Joint Center for Earth Systems Technology, University of Maryland, Baltimore County, Catonsville, MD, USA
  • 8Earth System Science Interdisciplinary Center, University of Maryland, College Park, MD, USA
  • 9Earth Science Division, NASA Ames Research Center, Moffett Field, CA, USA
  • 10Global Monitoring Division, NOAA Earth System Research Laboratory, Boulder, CO, USA
  • 11Chemical Sciences Division, NOAA Earth System Research Laboratory, Boulder, CO, USA
  • 12Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • 13Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA
  • 14Department of Earth and Environmental Sciences, Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY, USA
  • 15Departmentof Chemistry, University of California, Irvine, CA, USA
  • anow at: Scientific Aviation, Boulder, CO, USA

Abstract. The hydroxyl radical (OH) reacts with thousands of chemical species in the atmosphere, initiating their removal and the chemical reaction sequences that produce ozone, secondary aerosols, and gas-phase acids. OH reactivity, which is the inverse of OH lifetime, influences the OH abundance and the ability of OH to cleanse the atmosphere. The NASA Atmospheric Tomography (ATom) campaign used instruments on the NASA DC-8 aircraft to measure OH reactivity and more than 100 trace chemical species. ATom presented a unique opportunity to test the completeness of the OH reactivity calculated from the chemical species measurements by comparing it to the measured OH reactivity over two oceans across four seasons. Although the calculated OH reactivity was below the OH reactivity instrument's limit-of-detection for much of the free troposphere, the OHR instrument was able to measure the OH reactivity in and just above the marine boundary layer. The average measured value of OH reactivity in the marine boundary layer across all latitudes and all ATom phases was 1.9 s−1, which 0.5 s−1 larger than the average calculated OH reactivity. Concurrently, missing OH reactivity, the difference between the measured and calculated OH reactivity, was measured to be ~ 0.5–2.0 s−1 at some locations in the tropics and midlatitudes. Correlations of missing OH reactivity with formaldehyde, dimethyl sulfide, butanal, and sea surface temperature suggest the presence of unmeasured or unknown volatile organic compounds or oxygenated volatile organic compounds associated with ocean emissions.

Alexander B. Thames et al.
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Short summary
Oceans and the atmosphere exchange volatile gases that react with the hydroxyl radical (OH). During a NASA airborne study, measurements of the total frequency of OH reactions, called the OH reactivity, were made in the marine boundary layer of the Atlantic and Pacific Oceans. The measured OH reactivity often exceeded the OH reactivity calculated from measured chemical species. This missing OH reactivity appears to be from unmeasured volatile organic compounds coming out of the ocean.
Oceans and the atmosphere exchange volatile gases that react with the hydroxyl radical (OH)....
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