Abstract

Abstract. The variability of the relative sensitivity of photochemical ozone formation to volatile organic compounds (VOC) and NOx emissions, the chemical regime, over Europe during summers 2001 to 2003 is simulated with a regional scale transport-chemistry model. The robustness and variability of chemical regimes is shown. A VOC sensitive regime over North-Western Europe and a mainly NOx sensitive regime over the Mediterranean basin and Eastern Europe are found, confirming earlier published results. The chemical regime time variability, its robustness with respect to several environmental factors (seasonality, interannual variability) and with respect to model uncertainty are thoroughly analysed. For the regions with well pronounced chemical regimes over North-Western Europe and the Mediterranean, the chemical regime occurrence only slightly depends on the ozone target considered – daily ozone or Ox (= O3 + NO2) maximum or mean, AOT's, SOMO35, .... For these regions, differences between particular years and summer months are weak, day to day variability is significant but does not change the occurrence of one or another chemical regime. On the contrary, over North-Eastern Germany, the chemical regime changes form one day to another and is also dependent on the ozone target chosen. Expected decreases in anthropogenic NOx emissions over Europe since the last and for the next few decades have shifted and will shift chemical regimes to more NOx sensitive. The predictive skill of chemical regime indicator species is made evident at continental scale, extending their spatial range of applicability with respect to earlier studies. Several sensitivity tests were performed in order to account for major sources of model uncertainty. With the exception of regions near ship tracks over the Mediterranean basin, the spatial pattern of chemical regimes appears to be robust with respect to model uncertainty for all cases tested.

Highlights

  • The relation between pollutant emissions and concentrations of gases and aerosols affecting health and ecosystems is nonlinear

  • Chemical regimes have been defined relating ozone concentrations to upwind precursor emissions: in the “nitrogen oxides (NOx) sensitive chemical regime”, NOx anthropogenic emission reductions are more efficient to reduce ozone levels than volatile organic carbon species (VOC) anthropogenic emission reductions (Sillman et al, 1995), and the reverse occurs in the “VOC sensitive chemical regime”

  • Kleinman et al (1997) defined chemical regimes in terms of sensitivity of local photochemical ozone production (PO3) with respect to NOx and VOC concentrations. They showed theoretically that a locally VOC sensitive chemical regime is related to a dominant odd hydrogen (HOx) radical loss through reactions between NOx and HOx species, whereas a NOx sensitive chemical regime is related to dominant loss through HOx recombination reactions

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Summary

Introduction

The relation between pollutant emissions and concentrations of gases and aerosols affecting health and ecosystems is nonlinear. Kleinman et al (1997) defined chemical regimes in terms of sensitivity of local photochemical ozone production (PO3) with respect to NOx and VOC concentrations (instead of emissions). They showed theoretically that a locally VOC sensitive chemical regime is related to a dominant odd hydrogen (HOx) radical loss through reactions between NOx and HOx species, whereas a NOx sensitive chemical regime is related to dominant loss through HOx recombination reactions

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