Simulating ultrafine particle formation in Europe using a regional CTM

Contribution of primary emissions versus secondary formation to aerosol number concentrations

Christos Fountoukis, I. Riipinen, H. A C Denier Van Der Gon, P. E. Charalampidis, C. Pilinis, A. Wiedensohler, C. O'Dowd, J. P. Putaud, M. Moerman, S. N. Pandis

Research output: Contribution to journalArticle

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Abstract

A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS) algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N10) within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N50 levels (up to a factor of 2 increase) mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.

Original languageEnglish
Pages (from-to)8663-8677
Number of pages15
JournalAtmospheric Chemistry and Physics
Volume12
Issue number18
DOIs
Publication statusPublished - 2012
Externally publishedYes

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nucleation
aerosol
parameterization
ammonia
sulfur dioxide
sulfuric acid
particle
Europe
chemical
troposphere
kinetics
prediction
water
effect

ASJC Scopus subject areas

  • Atmospheric Science

Cite this

Simulating ultrafine particle formation in Europe using a regional CTM : Contribution of primary emissions versus secondary formation to aerosol number concentrations. / Fountoukis, Christos; Riipinen, I.; Denier Van Der Gon, H. A C; Charalampidis, P. E.; Pilinis, C.; Wiedensohler, A.; O'Dowd, C.; Putaud, J. P.; Moerman, M.; Pandis, S. N.

In: Atmospheric Chemistry and Physics, Vol. 12, No. 18, 2012, p. 8663-8677.

Research output: Contribution to journalArticle

Fountoukis, C, Riipinen, I, Denier Van Der Gon, HAC, Charalampidis, PE, Pilinis, C, Wiedensohler, A, O'Dowd, C, Putaud, JP, Moerman, M & Pandis, SN 2012, 'Simulating ultrafine particle formation in Europe using a regional CTM: Contribution of primary emissions versus secondary formation to aerosol number concentrations', Atmospheric Chemistry and Physics, vol. 12, no. 18, pp. 8663-8677. https://doi.org/10.5194/acp-12-8663-2012
Fountoukis, Christos ; Riipinen, I. ; Denier Van Der Gon, H. A C ; Charalampidis, P. E. ; Pilinis, C. ; Wiedensohler, A. ; O'Dowd, C. ; Putaud, J. P. ; Moerman, M. ; Pandis, S. N. / Simulating ultrafine particle formation in Europe using a regional CTM : Contribution of primary emissions versus secondary formation to aerosol number concentrations. In: Atmospheric Chemistry and Physics. 2012 ; Vol. 12, No. 18. pp. 8663-8677.
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