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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Volume 18, issue 19 | Copyright
Atmos. Chem. Phys., 18, 14493-14510, 2018
https://doi.org/10.5194/acp-18-14493-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 10 Oct 2018

Research article | 10 Oct 2018

Atmospheric oxidation in the presence of clouds during the Deep Convective Clouds and Chemistry (DC3) study

William H. Brune1, Xinrong Ren2,3, Li Zhang1, Jingqiu Mao4, David O. Miller1, Bruce E. Anderson5, Donald R. Blake6, Ronald C. Cohen7, Glenn S. Diskin5, Samuel R. Hall8, Thomas F. Hanisco9, L. Gregory Huey10, Benjamin A. Nault11,a, Jeff Peischl12,13, Ilana Pollack12,13,b, Thomas B. Ryerson13, Taylor Shingler14,15, Armin Sorooshian16,17, Kirk Ullmann8, Armin Wisthaler18, and Paul J. Wooldridge7 William H. Brune et al.
  • 1Department of Meteorology and Atmospheric Science, Pennsylvania State University, University Park, PA, USA
  • 2Department of Atmospheric and Oceanic Science, University of Maryland, College Park, MD, USA
  • 3Air Resources Laboratory, National Oceanic and Atmospheric Administration, College Park, MD, USA
  • 4Department of Chemistry and Biochemistry, University of Alaska, Fairbanks, Fairbanks, AK, USA
  • 5Chemistry and Dynamics Branch, NASA Langley Research Center, Hampton, VA, USA
  • 6Department of Chemistry, University of California, Irvine, CA, USA
  • 7Departments of Chemistry and Earth and Planetary Sciences, University of California, Berkeley, Berkeley, CA, USA
  • 8Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
  • 9Atmospheric Chemistry and Dynamics Branch, Goddard Space Flight Center, Greenbelt, MD, USA
  • 10School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
  • 11Department of Earth and Planetary Sciences, University of California, Berkeley, Berkeley, CA, USA
  • 12Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • 13Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
  • 14Science Systems and Applications, Inc., Hampton, VA, USA
  • 15Atmospheric Composition Branch, NASA Langley Research Center, Hampton, VA, USA
  • 16Department of Chemical and Environmental Engineering, University of Arizona, Tucson, AZ, USA
  • 17Department of Hydrology and Atmospheric Sciences, University of Arizona, Tucson, AZ, USA
  • 18Department of Chemistry, University of Oslo, Oslo, Norway
  • anow at: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • bnow at: Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA

Abstract. Deep convective clouds are critically important to the distribution of atmospheric constituents throughout the troposphere but are difficult environments to study. The Deep Convective Clouds and Chemistry (DC3) study in 2012 provided the environment, platforms, and instrumentation to test oxidation chemistry around deep convective clouds and their impacts downwind. Measurements on the NASA DC-8 aircraft included those of the radicals hydroxyl (OH) and hydroperoxyl (HO2), OH reactivity, and more than 100 other chemical species and atmospheric properties. OH, HO2, and OH reactivity were compared to photochemical models, some with and some without simplified heterogeneous chemistry, to test the understanding of atmospheric oxidation as encoded in the model. In general, the agreement between the observed and modeled OH, HO2, and OH reactivity was within the combined uncertainties for the model without heterogeneous chemistry and the model including heterogeneous chemistry with small OH and HO2 uptake consistent with laboratory studies. This agreement is generally independent of the altitude, ozone photolysis rate, nitric oxide and ozone abundances, modeled OH reactivity, and aerosol and ice surface area. For a sunrise to midday flight downwind of a nighttime mesoscale convective system, the observed ozone increase is consistent with the calculated ozone production rate. Even with some observed-to-modeled discrepancies, these results provide evidence that a current measurement-constrained photochemical model can simulate observed atmospheric oxidation processes to within combined uncertainties, even around convective clouds. For this DC3 study, reduction in the combined uncertainties would be needed to confidently unmask errors or omissions in the model chemical mechanism.

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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
Thunderstorms pull in polluted air from near the ground, transport it up through clouds...
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