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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article
03 Jul 2017
Review status
This discussion paper is a preprint. A revision of this manuscript was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.
Ozone Impacts of Gas-Aerosol Uptake in Global Chemistry Transport Models
Scarlet Stadtler1, David Simpson2,3, Sabine Schröder1, Domenico Taraborrelli1, Andreas Bott4, and Martin Schultz1 1Institut für Energie- und Klimaforschung, IEK-8, Forschungszentrum Jülich, Germany
2EMEP MSC-W, Norwegian Meteorological Institute, Oslo, Norway
3Dept. Space, Earth & Environment, Chalmers University of Technology, Gothenburg, Sweden
4Meteorological Institute University Bonn, Bonn, Germany
Abstract. The impact of six heterogeneous gas-aerosol uptake reactions on tropospheric ozone and nitrogen species was studied using two chemical transport models, EMEP MSC-W and ECHAM-HAMMOZ. Species undergoing heterogeneous reactions in both models include N2O5, NO3, NO2, O3, HNO3 and HO2. Since heterogeneous reactions take place at the aerosol surface area, the modeled surface area density Sa of both models was compared to a satellite product retrieving the surface area. This comparison shows a good agreement in global pattern and especially the capability of both models to capture the extreme aerosol loadings in East Asia.

The impact of the heterogeneous reactions was evaluated by the simulation of a reference run containing all heterogeneous reactions and several sensitivity runs. One reaction was turned off in each sensitivity run to compare it with the reference run. The analysis of the sensitivity runs confirms that the globally most important heterogeneous reaction is the one of N2O5. Nevertheless, NO2, HNO3 and HO2 heterogeneous reaction gain relevance particularly in East Asia due to the presence of high NOx concentrations and high Sa in the same region, although ECHAM-HAMMOZ showed much stronger responses than EMEP in this respect. The heterogeneous reaction of O3 itself on dust is of minor relevance compared to the other heterogeneous reactions. The impacts of the N2O5 reactions show strong seasonal variations, with biggest impacts on O3 in spring time when photochemical reactions are active and N2O5 levels still high. Evaluation of the models with northern hemispheric ozone surface observations yields a better agreement of the models with observations in terms of concentration levels, variability, and temporal correlations at most sites when the heterogeneous reactions are incorporated.

Citation: Stadtler, S., Simpson, D., Schröder, S., Taraborrelli, D., Bott, A., and Schultz, M.: Ozone Impacts of Gas-Aerosol Uptake in Global Chemistry Transport Models, Atmos. Chem. Phys. Discuss.,, in review, 2017.
Scarlet Stadtler et al.
Interactive discussionStatus: closed
AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment
Printer-friendly Version - Printer-friendly version      Supplement - Supplement
RC1: 'Review comment', Anonymous Referee #1, 17 Jul 2017 Printer-friendly Version 
AC1: 'Reply to Referee #1', Scarlet Stadtler, 30 Nov 2017 Printer-friendly Version Supplement 
RC2: 'Referee comment', Anonymous Referee #2, 16 Sep 2017 Printer-friendly Version 
AC2: 'Reply to Referee #2', Scarlet Stadtler, 30 Nov 2017 Printer-friendly Version Supplement 
Scarlet Stadtler et al.
Scarlet Stadtler et al.


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