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

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

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Offizielle URL: http://www.atmos-chem-phys.net/11/12007/2011/acp-11-12007-2011.html

Kurzfassung

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.

Dokumentart:Zeitschriftenbeitrag
Titel:Primary versus secondary contributions to particle number concentrations in the European boundary layer
Autoren:
AutorenInstitution oder E-Mail-Adresse der Autoren
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
Datum:5 Dezember 2011
Erschienen in:Atmospheric Chemistry and Physics
Referierte Publikation:Ja
In Open Access:Ja
In SCOPUS:Ja
In ISI Web of Science:Ja
Band:11
DOI :10.5194/acp-11-12007-2011
Seitenbereich:Seiten 12007-12036
Status:veröffentlicht
Stichwörter:aerosol particles, Europe, boundary layer
HGF - Forschungsbereich:Luftfahrt, Raumfahrt und Verkehr
HGF - Programm:Raumfahrt
HGF - Programmthema:Erdbeobachtung
DLR - Schwerpunkt:Raumfahrt
DLR - Forschungsgebiet:R EO - Erdbeobachtung
DLR - Teilgebiet (Projekt, Vorhaben):R - Vorhaben Atmosphären- und Klimaforschung
Standort: Oberpfaffenhofen
Institute & Einrichtungen:Institut für Physik der Atmosphäre > Atmosphärische Spurenstoffe
Hinterlegt von: Dr.rer.nat. Andreas Minikin
Hinterlegt am:06 Dez 2011 13:09
Letzte Änderung:12 Dez 2013 21:27

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