A new methodology to assess the performance and uncertainty of source apportionment models II: The results of two European intercomparison exercises
Résumé
In this work, impact of aerosol solar extinction on the photochemistry over eastern Europe during the 2010 wildfires episode is discussed for the period from 5 to 12 August 2010, which coincides to the peak of fire activity. The methodology is based on an online coupling between the chemistry-transport model CHIMERE (extended by an aerosol optical module) and the radiative transfer code TUV. Results of simulations indicate an important influence of the aerosol solar extinction, in terms of intensity and spatial extent, with a reduction of the photolysis rates of NO2 and O-3 up to 50% (in daytime average) along the aerosol plume transport. At a regional scale, these changes in photolysis rates lead to a 3-15% increase in the NO2 daytime concentration and to an ozone reduction near the surface of 1-12 %. The ozone reduction is shown to occur over the entire boundary layer, where aerosols are located. Also, the total aerosol mass concentration (PM10) is shown to be decreased by 1-2 %, on average during the studied period, caused by a reduced formation of secondary aerosols such as sulfates and secondary organics (4-10 %) when aerosol impact on photolysis rates is included. In terms of model performance, comparisons of simulations with air quality measurements at Moscow indicate that an explicit representation of aerosols interaction with photolysis rates tend to improve the estimation of the near-surface concentration of ozone and nitrogen dioxide as well as the formation of inorganic aerosol species such as ammonium, nitrates and sulfates.
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