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

Reddington, C. L. and Carslaw, K. S. and Spracklen, D. V. and Frontoso, M. G. and Collins, L. and Merikanto, J. and Minikin, Andreas and Hamburger, Thomas and Coe, H. and Kulmala, M. and Aalto, P. and Flentje, H. and Plass-Dülmer, C. and Birmili, W. and Wiedensohler, A. and Wehner, B. and Tuch, T. and Sonntag, A. and O'Dowd, C. D. and Jennings, S. G. and Dupuy, R. and Baltensperger, U. and Weingartner, E. and Hansson, H.-C. and Tunved, P. and Laj, P. and Sellegri, K. and Boulon, J. and Putaud, J.-P. and Gruening, C. and Swietlicki, E. and Roldin, P. and Henzing, J. S. and Moerman, M. and Mihalopoulos, N. and Kouvarakis, G. and Ždímal, V. and Zíková, N. and Marinoni, A. and Bonasoni, P. and Duchi, R. (2011) Primary versus secondary contributions to particle number concentrations in the European boundary layer. Atmospheric Chemistry and Physics, 11, pp. 12007-12036. DOI: 10.5194/acp-11-12007-2011.

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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 particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >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% for N100). 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.

Document Type:Article
Title:Primary versus secondary contributions to particle number concentrations in the European boundary layer
AuthorsInstitution or Email of Authors
Reddington, C. L.Univ. of Leeds, Leeds, UK
Carslaw, K. S.Univ. of Leeds, Leeds, UK
Spracklen, D. V.Univ. of Leeds, Leeds, UK
Frontoso, M. G.ETH Zürich, Zürich, CH
Collins, L.Univ. of Leeds, Leeds, UK
Merikanto, J.Univ. of Leeds, Leeds, UK
Minikin, AndreasDLR
Hamburger, ThomasDLR
Coe, H.Univ. of Manchester, Manchester, UK
Kulmala, M.Univ. of Helsinki, Helsinki, F
Aalto, P.Univ. of Helsinki, Helsinki, F
Flentje, H.DWD, Hohenpeißenberg
Plass-Dülmer, C.DWD, Hohenpeißenberg
Birmili, W.IfT, Leipzig
Wiedensohler, A.IfT, Leipzig
Wehner, B.IfT, Leipzig
Tuch, T.IfT, Leipzig
Sonntag, A.IfT, Leipzig
O'Dowd, C. D.National Univ. of Ireland, Galway, IR
Jennings, S. G.National Univ. of Ireland, Galway, IR
Dupuy, R.National Univ. of Ireland, Galway, IR
Baltensperger, U.Paul Scherrer Instit. Villigen, CH
Weingartner, E.Paul Scherrer Instit. Villigen, CH
Hansson, H.-C.Stockholm Univ., S
Tunved, P.Stockholm Univ., S
Laj, P.CNRS, Grenoble, F
Sellegri, K.Univ. Blaise Pascal, Aubière cedex, F
Boulon, J.Univ. Blaise Pascal, Aubière cedex, F
Putaud, J.-P.IES, Ispra, I
Gruening, C.IES, Ispra, I
Swietlicki, E.Lund Univ., Lund, S
Roldin, P.Lund Univ., Lund, S
Henzing, J. S.TNO, Utrecht, NL
Moerman, M.TNO, Utrecht, NL
Mihalopoulos, N.Univ. of Crete, Heraklion, Crete, GR
Kouvarakis, G.Univ. of Crete, Heraklion, Crete, GR
Ždímal, V.ICPF, Prague, CZ
Zíková, N.ICPF, Prague, CZ
Marinoni, A.CNR, Bologna, I
Bonasoni, P.CNR, Bologna, I
Duchi, R.CNR, Bologna, I
Date:5 December 2011
Journal or Publication Title:Atmospheric Chemistry and Physics
Refereed publication:Yes
In Open Access:Yes
In ISI Web of Science:Yes
Page Range:pp. 12007-12036
Keywords:aerosol particles, Europe, boundary layer
HGF - Research field:Aeronautics, Space and Transport
HGF - Program:Space
HGF - Program Themes:Earth Observation
DLR - Research area:Raumfahrt
DLR - Program:R EO - Erdbeobachtung
DLR - Research theme (Project):R - Vorhaben Atmosphären- und Klimaforschung
Location: Oberpfaffenhofen
Institutes and Institutions:Institute of Atmospheric Physics > Atmospheric Trace Species
Deposited By: Dr.rer.nat. Andreas Minikin
Deposited On:06 Dec 2011 13:09
Last Modified:12 Dec 2013 21:27

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