4.7 Article

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

Journal

ATMOSPHERIC CHEMISTRY AND PHYSICS
Volume 18, Issue 19, Pages 14493-14510

Publisher

COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-18-14493-2018

Keywords

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Funding

  1. U.S. National Science Foundation (NSF)
  2. National Aeronautics and Space Administration (NASA)
  3. National Oceanic and Atmospheric Administration (NOAA)
  4. Deutsches Zentrum fur Luft- und Raumfahrt (DLR)
  5. National Science Foundation
  6. Austrian Federal Ministry for Transport, Innovation, and Technology (BMVIT) through the Austrian Space Applications Programme (ASAP) of the Austrian Research Promotion Agency (FFG)
  7. NASA [NNX12AB84G]
  8. NASA [NNX12AB84G, 30959] Funding Source: Federal RePORTER

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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 air-craft 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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