An advanced method of contributing emissions to short-lived chemical species (OH and HO 2): the TAGGING 1.1 submodel based on the Modular Earth Submodel System (MESSy 2.53)

Rieger, Vanessa S.; Mertens, Mariano; Grewe, Volker

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 inline-formulaHO2 is important as they play a crucial role for atmospheric chemistry. This study presents an advanced version of a tagging method for OH and inline-formulaHO2 (inline-formulaHOx) which attributes inline-formulaHOx 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 inline-formulaHOx chemistry in the stratosphere are also regarded (in total 27 reactions). To fully take into account the main inline-formulaHO2 source by the reaction of H and inline-formulaO2, 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 inline-formulaHOx production and loss. This closes the budget between the sum of all contributions and the total concentration. The contributions to OH and inline-formulaHO2 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 inline-formulaHO2, the contributions differ strongly in the categories biogenic emissions and methane decomposition. As inline-formulaHOx reacts with ozone (inline-formulaO3), carbon monoxide (CO), reactive nitrogen compounds (inline-formulaNOy), non-methane hydrocarbons (NMHCs) and peroxyacyl nitrates (PAN), the contributions to these species are also modified by the advanced inline-formulaHOx tagging method V1.1. The contributions to inline-formulaNOy, NMHC and PAN show only little change, whereas inline-formulaO3 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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Rieger, Vanessa S. / Mertens, Mariano / Grewe, Volker: 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). 2018. Copernicus Publications.

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Rechteinhaber: Vanessa S. Rieger et al.

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