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Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

Spracklen, D. V. und Carslaw, K. S. und Merikanto, J. und Mann, G. W. und Reddington, C. L. und Pickering, S. und Ogren, J. A. und Andrews, E. und Baltensperger, U. und Weingartner, E. und Boy, M. und Kulmala, M. und Laakso, L. und Lihavainen, H.Finnish Meteorol. Inst., und Kivekäs, N. und Komppula, M. und Mihalopoulos, N. und Kouvarakis, G. und Jennings, S. G. und O'Dowd, C. und Birmili, W. und Wiedensohler, A. und Weller, R. und Gras, J. und Laj, P. und Sellegri, K. und Bonn, B. und Krejci, R. und Laaksonen, A. und Hamed, A. und Minikin, A. und Harrison, R. M. und Talbot, R. und Sun, J. (2010) Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation. Atmospheric Chemistry and Physics, 10, Seiten 4775-4793. DOI: 10.5194/acp-10-4775-2010.

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Offizielle URL: http://www.atmos-chem-phys.net/10/4775/2010/acp-10-4775-2010.html

Kurzfassung

We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300� 2000 cm�3 in the marine boundary layer and free troposphere (FT) and 1000�10 000 cm�3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2�10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=�88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=�25%). Simulated CN concentrations in the continental BL were also biased low (NMB=�74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J , proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.

Dokumentart:Zeitschriftenbeitrag
Titel:Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation
Autoren:
AutorenInstitution oder E-Mail-Adresse der Autoren
Spracklen, D. V.Univ. of Leeds, UK
Carslaw, K. S.Univ. of Leeds, UK
Merikanto, J.Univ. of Leeds, UK
Mann, G. W.Univ. of Leeds, UK
Reddington, C. L.Univ. of Leeds, UK
Pickering, S.Univ. of Leeds, UK
Ogren, J. A.NOAA/ESRL Global Monitoring Division, Boulder, CO, USA
Andrews, E.NOAA/ESRL Global Monitoring Division, Boulder, CO, USA
Baltensperger, U.Lab. of Atmospheric Chemistry, Villigen, CH
Weingartner, E.Lab. of Atmospheric Chemistry, Villigen, CH
Boy, M.Univ. of Helsinki, FIN
Kulmala, M.Univ. of Helsinki, FIN
Laakso, L.Univ. of Helsinki, FIN
Lihavainen, H.Finnish Meteorol. Inst.,Finnish Meteorol. Inst., Helsinki, FIN
Kivekäs, N.Finnish Meteorol. Inst., Helsinki, FIN
Komppula, M.Finnish Meteorol. Inst., Helsinki, FIN
Mihalopoulos, N.Univ. of Crete, Heraklion, GR
Kouvarakis, G.Univ. of Crete, Heraklion, GR
Jennings, S. G.National Univ. of Ireland, Galway, IR
O'Dowd, C.National Univ. of Ireland, Galway, IR
Birmili, W.Leibniz Institute for Tropospheric Research, Leipzig
Wiedensohler, A.Leibniz Institute for Tropospheric Research, Leipzig
Weller, R.Alfred Wegener Institute, Bremerhaven
Gras, J.CSIRO Marine and Atmospheric Research, Aspendale, Victoria, AU
Laj, P.Univ. Grenoble, F
Sellegri, K.Univ. Clermont-Ferrand/CNRS, Clermont-Ferrand, F
Bonn, B.J. W. Goethe Univ., Frankfurt/Main
Krejci, R.Stockholm Univ., S
Laaksonen, A.Finnish Meteorol. Inst., Helsinki, FIN
Hamed, A.Univ. of Eastern Finland, Kuopio, FIN
Minikin, A.andreas.minikin@dlr.de
Harrison, R. M.Univ. of Birmingham, UK
Talbot, R.Univ. of New Hampshire, Durham, NH, USA
Sun, J.Chinese Academy of Meteoroi. Sciences, Beijing, CHN
Datum:26 Mai 2010
Erschienen in:Atmospheric Chemistry and Physics
Referierte Publikation:Ja
In Open Access:Ja
In SCOPUS:Ja
In ISI Web of Science:Ja
Band:10
DOI :10.5194/acp-10-4775-2010
Seitenbereich:Seiten 4775-4793
Status:veröffentlicht
Stichwörter:aerosol, troposphere, CN, particle formation
HGF - Forschungsbereich:Verkehr und Weltraum (alt)
HGF - Programm:Weltraum (alt)
HGF - Programmthema:W EO - Erdbeobachtung
DLR - Schwerpunkt:Weltraum
DLR - Forschungsgebiet:W EO - Erdbeobachtung
DLR - Teilgebiet (Projekt, Vorhaben):W - Vorhaben Atmosphären- und Klimaforschung (alt)
Standort: Oberpfaffenhofen
Institute & Einrichtungen:Institut für Physik der Atmosphäre > Atmosphärische Spurenstoffe
Hinterlegt von: Dr.rer.nat. Andreas Minikin
Hinterlegt am:01 Jun 2010 13:45
Letzte Änderung:12 Dez 2013 20:57

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