Atmos. Chem. Phys. Discuss., 3, 5919-5976, 2003
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
The nitrate aerosol field over Europe: simulations with an atmospheric chemistry-transport model of intermediate complexity
M. Schaap1, M. van Loon2, H. M. ten Brink3, F. J. Dentener4, and P. J. H. Builtjes1,2
1University of Utrecht, Institute of Marine and Atmospheric Science, PO Box 80005, 3508 TA, Utrecht, The Netherlands
2TNO institute of Environmental Sciences, Energy and Process Innovation, PO Box 342, 7300 AH Apeldoorn, The Netherlands
3Netherlands Energy Research Foundation (ECN), PO Box 1, 1755 LE Petten, The Netherlands
4Joint Research Centre (JRC), Institute for Environment and Sustainability, 21020 Ispra, Italy

Abstract. Nitrate is an important component of fine aerosols in Europe. We present a model simulation for the year 1995 in which we account for the formation of the ammonium nitrate, a semi volatile component. For this purpose, LOTOS, a chemistry-transport model of intermediate complexity, was extended with a thermodynamic equilibrium module and additional relevant processes to account for aerosol formation and deposition. Our earlier analysis of data on (ammonium) nitrate in Europe was used for model evaluation. During winter, fall and especially spring high nitrate levels are projected over north western, central and eastern Europe. During winter nitrate concentrations are highest in the Po valley, Italy. This is in accordance with the field that was constructed from the data. In winter nitric acid, the precursor for aerosol nitrate, is formed through heterogeneous reactions on the surface of aerosols. Appreciable ammonium nitrate concentrations in summer are limited to those areas with high ammonia emissions, e.g. The Netherlands, since high ammonia concentrations are necessary to stabilise this aerosol component at high temperatures. Averaged over all stations the model reproduces the measured concentrations for NO3, SO4, NH4, TNO3, TNH4 and SO2 within 20%. The daily variation is captured well, albeit that the model does not always represents the amplitude of single events. The model underestimates wet deposition which was attributed to the crude representation of cloud processes. The treatment of ammonia was found to be the major source for uncertainties in the model representation of secondary aerosols. Also, inclusion of sea salt is necessary to properly assess the nitrate and nitric acid levels in marine areas.

Over Europe the annual forcing by nitrate is calculated to be 25% of that by sulphate. In summer nitrate is found to be regionally important, e.g. in The Netherlands, where the forcing of nitrate and sulphate are calculated to be equal. In winter, spring and fall the nitrate forcing over Europe is about half that by sulphate. Over north western Europe and the alpine region the forcing by nitrate was calculated to be similar to that of sulphate. Overall, nitrate forcing is significant and should be taken into account to estimate the impact of regional climate change in Europe.

Citation: Schaap, M., van Loon, M., ten Brink, H. M., Dentener, F. J., and Builtjes, P. J. H.: The nitrate aerosol field over Europe: simulations with an atmospheric chemistry-transport model of intermediate complexity, Atmos. Chem. Phys. Discuss., 3, 5919-5976, doi:10.5194/acpd-3-5919-2003, 2003.
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