1. Primary versus secondary contributions to particle number concentrations in the European boundary layer
- Author
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Karine Sellegri, Nadezda Zikova, Kenneth S. Carslaw, Ernest Weingartner, Angela Marinoni, Thomas Hamburger, Thomas Tuch, Paolo Bonasoni, Joonas Merikanto, Urs Baltensperger, A. Sonntag, Marcel M. Moerman, M. G. Frontoso, Colin D. O'Dowd, Vladimír Ždímal, Pasi Aalto, Pontus Roldin, J. Boulon, L. Collins, Carly Reddington, Birgit Wehner, Hugh Coe, Wolfram Birmili, J. P. Putaud, Andreas Minikin, R. Duchi, Christian Plass-Dülmer, Hans-Christen Hansson, Régis Dupuy, Carsten Gruening, Paolo Laj, Markku Kulmala, Peter Tunved, J. S. Henzing, Dominick V. Spracklen, Alfred Wiedensohler, Nikos Mihalopoulos, Erik Swietlicki, S. G. Jennings, Giorgos Kouvarakis, Harald Flentje, Institute for Climate and Atmospheric Science [Leeds] (ICAS), School of Earth and Environment [Leeds] (SEE), University of Leeds-University of Leeds, C2SM, Department of Physics [Helsinki], Falculty of Science [Helsinki], Helsingin yliopisto = Helsingfors universitet = University of Helsinki-Helsingin yliopisto = Helsingfors universitet = University of Helsinki, DLR Institut für Physik der Atmosphäre (IPA), Deutsches Zentrum für Luft- und Raumfahrt [Oberpfaffenhofen-Wessling] (DLR), School of Earth, Atmospheric and Environmental Sciences [Manchester] (SEAES), University of Manchester [Manchester], Deutscher Wetterdienst [Offenbach] (DWD), Leibniz Institute for Tropospheric Research (TROPOS), Centre for Climate and Air Pollution Studies [Galway] (C-CAPS), National University of Ireland [Galway] (NUI Galway), School of Physics [NUI Galway], Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Institute for Applied Environmental Research [Stockholm], Stockholm University, Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), JRC Institute for Environment and Sustainability (IES), European Commission - Joint Research Centre [Ispra] (JRC), Division of Nuclear Physics, Lund University [Lund], Netherlands Organization for Applied Scientific Research (TNO), TNO Science and Industry, Environmental Chemical Processes Laboratory [Heraklion] (ECPL), Department of Chemistry [Heraklion], University of Crete [Heraklion] (UOC)-University of Crete [Heraklion] (UOC), Institute of Chemical Process Fundamentals of the AS CR, CNR Institute of Atmospheric Sciences and Climate (ISAC), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), NERC ADIENT, University of Helsinki-University of Helsinki, Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Consiglio Nazionale delle Ricerche (CNR), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), and Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)
- Subjects
Atmospheric Science ,Particle number ,010504 meteorology & atmospheric sciences ,aerosol particles ,Aerosol radiative forcing ,Earth & Environment ,Nucleation ,[SDU.STU]Sciences of the Universe [physics]/Earth Sciences ,boundary layer ,Environment ,010501 environmental sciences ,Atmospheric sciences ,01 natural sciences ,resolved aerosol microphysics ,lcsh:Chemistry ,Primary (astronomy) ,ion-induced nucleation ,instrumental development ,Cloud condensation nuclei ,0105 earth and related environmental sciences ,particulate matter ,size distributions ,Atmosphärische Spurenstoffe ,Particulates ,lcsh:QC1-999 ,Aerosol ,on-road ,Europe ,Boundary layer ,carbonaceous aerosol ,lcsh:QD1-999 ,13. Climate action ,UES - Urban Environment & Safety ,Environmental science ,emission factors ,atmospheric sulfuric-acid ,off-line model ,EELS - Earth, Environmental and Life Sciences ,lcsh:Physics - 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 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., JRC.H.2-Air and Climate
- Published
- 2011
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