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Primary versus secondary contributions to particle number concentrations in the European boundary layer

C.L. Reddington 1 K. S. Carslaw 1 D. V. Spracklen 1 M. G. Frontoso 2 L. Collins 1 J. Merikanto 1, 3 A. Minikin 4 T. Hamburger 4 H. Coe 5 M. Kulmala 3 P. Aalto 3 H. Flentje 6 C. Plass-Dülmer 6 W. Birmili 7 A. Wiedensohler 7 B. Wehner 7 T. Tuch 7 A. Sonntag 7 C. D. O'Dowd 8, 9 S. G. Jennings 8, 9 R. Dupuy 8, 9 Urs Baltensperger 10 E. Weingartner 10 H.-C. Hansson 11 P. Tunved 11 Paolo Laj 12 K. Sellegri 13 J. Boulon 13 J.-P. Putaud 14 C. Gruening 14 E. Swietlicki 15 P. Roldin 15 J. S. Henzing 16 M. Moerman 16 N. Mihalopoulos 17 G. Kouvarakis 17 V. Zdímal 18 N. Zikova 18 A. Marinoni 19 P. Bonasoni 19 R. Duchi 19 
Abstract : It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous par- ticles at small sizes (as recommended by the Aerosol Inter- comparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with di- ameter >50 nm (N50) and>100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18 % for N50 and −1 % forN100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB =−52 % and −29 %), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
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C.L. Reddington, K. S. Carslaw, D. V. Spracklen, M. G. Frontoso, L. Collins, et al.. Primary versus secondary contributions to particle number concentrations in the European boundary layer. Atmospheric Chemistry and Physics, European Geosciences Union, 2011, 11, pp.12007- 12036. ⟨10.5194/acp-11-12007-2011⟩. ⟨insu-00843532⟩



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