Primary versus secondary contributions to particle number concentrations in the European boundary layer
Lade...
Autor:in (Körperschaft)
Publikationsdatum
05.12.2011
Typ der Arbeit
Studiengang
Typ
01A - Beitrag in wissenschaftlicher Zeitschrift
Herausgeber:innen
Herausgeber:in (Körperschaft)
Betreuer:in
Übergeordnetes Werk
Atmospheric Chemistry and Physics
Themenheft
DOI der Originalpublikation
Link
Reihe / Serie
Reihennummer
Jahrgang / Band
11
Ausgabe / Nummer
23
Seiten / Dauer
12007-12036
Patentnummer
Verlag / Herausgebende Institution
Copernicus
Verlagsort / Veranstaltungsort
Göttingen
Auflage
Version
Programmiersprache
Abtretungsempfänger:in
Praxispartner:in/Auftraggeber:in
Zusammenfassung
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.
Schlagwörter
Fachgebiet (DDC)
550 - Geowissenschaften
Veranstaltung
Startdatum der Ausstellung
Enddatum der Ausstellung
Startdatum der Konferenz
Enddatum der Konferenz
Datum der letzten Prüfung
ISBN
ISSN
1680-7324
1680-7316
1680-7316
Sprache
Englisch
Während FHNW Zugehörigkeit erstellt
Nein
Publikationsstatus
Veröffentlicht
Begutachtung
Peer-Review der ganzen Publikation
Open Access-Status
Gold
Zitation
REDDINGTON, Carly L., Ken S. CARSLAW, Dominick V. SPRACKLEN, Maria Grazia FRONTOSO, Lisa M. COLLINS, Joonas MERIKANTO, Andreas MINIKIN, Thomas HAMBURGER, Hugh COE, Markku KULMALA, Pasi Pekka AALTO, Harald FLENTJE, Christian PLASS-DÜLMER, Wolfram BIRMILI, Alfred WIEDENSOHLER, Birgit WEHNER, Thomas TUCH, Alfred SONNTAG, Collin D. O’DOWD, Stephen G. JENNINGS, Regis DUPUY, Urs BALTENSPERGER, Ernest WEINGARTNER, Hans-Christen HANSSON, Peter TUNVED, Paolo LAJ, Karine SELLEGRI, Julien BOULON, Jean-Philippe PUTAUD, Carsten GRUENING, Erik SWIETLICKI, Pontus ROLDIN, J.S. HENZING, Marcel MOERMAN, Nikolaos MIHALOPOULOS, Giorgos KOUVARAKIS, Vladimir ŽDÍMAL, Nadezda ZÍKOVÁ, Angela MARINONI, Paolo BONASONI und Rocco DUCHI, 2011. Primary versus secondary contributions to particle number concentrations in the European boundary layer. Atmospheric Chemistry and Physics. 5 Dezember 2011. Bd. 11, Nr. 23, S. 12007–12036. DOI 10.5194/acp-11-12007-2011. Verfügbar unter: https://doi.org/10.26041/fhnw-9661