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Volume 11, issue 6 | Copyright

Special issue: The Modular Earth Submodel System (MESSy) (ACP/GMD inter-journal...

Geosci. Model Dev., 11, 2049-2066, 2018
https://doi.org/10.5194/gmd-11-2049-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Development and technical paper 05 Jun 2018

Development and technical paper | 05 Jun 2018

An advanced method of contributing emissions to short-lived chemical species (OH and HO2): the TAGGING 1.1 submodel based on the Modular Earth Submodel System (MESSy 2.53)

Vanessa S. Rieger1,a, Mariano Mertens1, and Volker Grewe1,a Vanessa S. Rieger et al.
  • 1Deutsches Zentrum für Luft- und Raumfahrt, Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany
  • aalso at: Delft University of Technology, Aerospace Engineering, Section Aircraft Noise and Climate Effects, Delft, the Netherlands

Abstract. To mitigate the human impact on climate change, it is essential to determine the contribution of emissions to the concentration of trace gases. In particular, the source attribution of short-lived species such as OH and HO2 is important as they play a crucial role for atmospheric chemistry. This study presents an advanced version of a tagging method for OH and HO2 (HOx) which attributes HOx concentrations to emissions. While the former version (V1.0) only considered 12 reactions in the troposphere, the new version (V1.1), presented here, takes 19 reactions in the troposphere into account. For the first time, the main chemical reactions for the HOx chemistry in the stratosphere are also regarded (in total 27 reactions). To fully take into account the main HO2 source by the reaction of H and O2, the tagging of the H radical is introduced. In order to ensure the steady-state assumption, we introduce rest terms which balance the deviation of HOx production and loss. This closes the budget between the sum of all contributions and the total concentration. The contributions to OH and HO2 obtained by the advanced tagging method V1.1 deviate from V1.0 in certain source categories. For OH, major changes are found in the categories biomass burning, biogenic emissions and methane decomposition. For HO2, the contributions differ strongly in the categories biogenic emissions and methane decomposition. As HOx reacts with ozone (O3), carbon monoxide (CO), reactive nitrogen compounds (NOy), non-methane hydrocarbons (NMHCs) and peroxyacyl nitrates (PAN), the contributions to these species are also modified by the advanced HOx tagging method V1.1. The contributions to NOy, NMHC and PAN show only little change, whereas O3 from biogenic emissions and methane decomposition increases in the tropical troposphere. Variations for CO from biogenic emissions and biomass burning are only found in the Southern Hemisphere.

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To reduce the climate impact of human activities, it is crucial to attribute changes in atmospheric gases to anthropogenic emissions. We present an advanced method to determine the contribution of emissions to OH and HO2 concentrations. Compared to the former version, it contains the main reactions of the OH and HO2 chemistry in the troposphere and stratosphere, introduces the tagging of the H radical and closes the budget of the sum of all contributions and the total concentration.
To reduce the climate impact of human activities, it is crucial to attribute changes in...
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