Primary versus secondary contributions to particle number concentrations in the European boundary layer
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.
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Citation proposal
Carly L. Reddington (Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds,) - Ken S. Carslaw (Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds,) - Dominick V. Spracklen (Institute for Climate and Atmospheric Science, School of Earth and Environment) - L. Collins (Institute for Climate and Atmospheric Science, School of Earth and Environment) - J. Merikanto (Institute for Climate and Atmospheric Science, School of Earth and Environment) - M. Grazia Frontoso (C2SM , ETH) - Markku Kulmala (University of Helsinki, Dept of Physics,Division of Atmospheric Sciences,) - Pasi Aalto (University of Helsinki, Dept of Physics,Division of Atmospheric Sciences,) - Andreas Minikin (Institute of Atmospheric Physics,) - Thomas Hamburger (Institute of Atmospheric Physics,) - Hugh Coe (School of Earth, Atmospheric and Environmental Sciences, University of Manchester,) - Harald Flentje (Deutscher Wetterdienst,Meteorological Observatory Hohenpeissenberg) - Christian Plass-Dülmer (Deutscher Wetterdienst,Meteorological Observatory Hohenpeissenberg) - Wolfram Birmili (Leibniz Institute for Tropospheric Research) - Alfred Wiedensohler (Leibniz Institute for Tropospheric Reseach) - Birgit Wehner (Leibniz Institute for Tropospheric Reseach) - Thomas Tuch (Leibniz Institute for Tropospheric Research,) - Andre Sonntag (Leibniz Institute for Tropospheric Research,) - Colin D. O'Dowd (School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway) - S.Gerard Jennings (School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway) - Regis Dupuy (School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway) - Urs Baltensperger (Paul Scherrer Institut, Laboratory of Atmospheric Chemistry,) - Ernest Weingartner (Paul Scherrer Institute, Laboratory of Atmospheric Chemistry,) - Hans-Christen Hansson (Institute for Applied Environmental Research, Stockholm University,) - Peter Tunved (Institute for Applied Environmental Research, Stockholm University,) - Paolo Laj (CNRS Laboratory of Meteorology Physics - Laboratory of Glaciology) - Karine Sellegri (Université Blaise Pascal, CNRS,) - Julien Boulon (Physical Laboratory of Meteorology, University Blaise Pascal,CNRS) - Jean Philippe Putaud (European Commission, Joint Research Centre, Institute for Environment and Sustainability,) - Carsten Gruening (European Commission, Joint Research Centre, Institute for Environment and Sustainability,) - Erik Swietlicki (Division of Nuclear Physics, Lund University,) - Pontus Roldin (Division of Nuclear Physics, Lund University,) - J. S. Henzing (TNO—Netherlands Organization for Applied Scientific Research,) - Marcel Moerman (Netherlands Organisation for Applied Scientific Research, TNO,) - Nikolaos Mihalopoulos (Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete,) - Giorgios Kouvarakis (Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete) - Vladimír Ždímal (Institute of Chemical Process Fundamentals of the AS CR,) - Nadežda Zíková (Institute of Chemical Process Fundamentals of the AS CR,) - Angela Marinoni (Institute of Atmospheric Sciences and Climate (ISAC) - CNR) - Paolo Bonasoni (Institute of Atmospheric Sciences and Climate (ISAC) - CNR) - Rocco Duchi (Institute of Atmospheric Sciences and Climate (ISAC) - CNR) (2011) . Primary versus secondary contributions to particle number concentrations in the European boundary layer. Copernicus GmbH (Copernicus Publications) https://geoportal.mountaingenius.org/geonetwork/srv/api/records/8796a712-80a0-4b91-99cf-a5f451516215 |
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- European Integrated Project , Air Quality Interactions (EUCAARI) , Aerosol , Cloud , Climate
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- Europe
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- particle number concentrations , boundary layer , primary particles , secondary particles
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"Primary versus secondary contributions to particle number concentrations in the European boundary layer".
Atmospheric Chemistry and Physics, Volume 11, Issue 23, 2011, pp.12007-12036.
Reddington, C.L., Carslaw, K.S., Spracklen, D.V., Frontoso, M.G., Collins, L., Merikanto, J., Minikin, A., Hamburger, T., Coe, H., Kulmala, M., Aalto, P., Flentje, H., Plass-Dülmer, C., Birmili, W., Wiedensohler, A., Wehner, B., Tuch, T., Sonntag, A., O'Dowd, C.D., Jennings, S.G., Dupuy, R., Baltensperger, U., Weingartner, E., Hansson, H.-C., Tunved, P., Laj, P., Sellegri, K., Boulon, J., Putaud, J.-P., Gruening, C., Swietlicki, E., Roldin, P., Henzing, J.S., Moerman, M., Mihalopoulos, N., Kouvarakis, G., Ždímal, V., Zíková, N., Marinoni, A., Bonasoni, P., Duchi, R.
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- ear3clsr@leeds.ac.uk
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- Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds,
- lecksc@ds.leeds.ac.uk
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- Institute for Climate and Atmospheric Science, School of Earth and Environment
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- Institute for Climate and Atmospheric Science, School of Earth and Environment
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- Institute for Climate and Atmospheric Science, School of Earth and Environment
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- C2SM , ETH
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- pasi.p.aalto@helsinki.fi
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- Institute of Atmospheric Physics,
- Andreas.Minikin@dlr.de
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- Institute of Atmospheric Physics,
- thomas.hamburger@dlr.de
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- School of Earth, Atmospheric and Environmental Sciences, University of Manchester,
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- Deutscher Wetterdienst,Meteorological Observatory Hohenpeissenberg
- harald.flentje@dwd.de
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- Deutscher Wetterdienst,Meteorological Observatory Hohenpeissenberg
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- Leibniz Institute for Tropospheric Research
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- Leibniz Institute for Tropospheric Reseach
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- Leibniz Institute for Tropospheric Reseach
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- Leibniz Institute for Tropospheric Research,
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- Leibniz Institute for Tropospheric Research,
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- School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway
- colin.odowd@nuigalway.ie
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- School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway
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- School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway
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- Institute for Applied Environmental Research, Stockholm University,
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- CNRS Laboratory of Meteorology Physics - Laboratory of Glaciology
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- Université Blaise Pascal, CNRS,
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- Physical Laboratory of Meteorology, University Blaise Pascal,CNRS
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- European Commission, Joint Research Centre, Institute for Environment and Sustainability,
- jean.putaud@jrc.it
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- European Commission, Joint Research Centre, Institute for Environment and Sustainability,
- carsten.gruening@jrc.it
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- Division of Nuclear Physics, Lund University,
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- Division of Nuclear Physics, Lund University,
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- TNO—Netherlands Organization for Applied Scientific Research,
- bas.henzing@tno.nl
- Organisation name
- Netherlands Organisation for Applied Scientific Research, TNO,
- moerman@fel.tno.nl
- Organisation name
- Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete,
- mihalo@chemistry.uoc.gr
- Organisation name
- Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete
- Organisation name
- Institute of Chemical Process Fundamentals of the AS CR,
- zdimal@icpf.cas.cz
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- Institute of Chemical Process Fundamentals of the AS CR,
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- Institute of Atmospheric Sciences and Climate (ISAC) - CNR
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- Institute of Atmospheric Sciences and Climate (ISAC) - CNR
- p.bonasoni@isac.cnr.it
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- Institute of Atmospheric Sciences and Climate (ISAC) - CNR
- R.Duchi@isac.cnr.it
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- info@copernicus.org
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- Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds,
- ear3clsr@leeds.ac.uk
- Organisation name
- Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds,
- lecksc@ds.leeds.ac.uk
- Organisation name
- Institute for Climate and Atmospheric Science, School of Earth and Environment
- Organisation name
- Institute for Climate and Atmospheric Science, School of Earth and Environment
- Organisation name
- Institute for Climate and Atmospheric Science, School of Earth and Environment
- j.merikanto@leeds.ac.uk
- Organisation name
- C2SM , ETH
- Organisation name
- University of Helsinki, Dept of Physics,Division of Atmospheric Sciences,
- Organisation name
- University of Helsinki, Dept of Physics,Division of Atmospheric Sciences,
- pasi.p.aalto@helsinki.fi
- Organisation name
- Institute of Atmospheric Physics,
- Andreas.Minikin@dlr.de
- Organisation name
- Institute of Atmospheric Physics,
- thomas.hamburger@dlr.de
- Organisation name
- School of Earth, Atmospheric and Environmental Sciences, University of Manchester,
- Organisation name
- Deutscher Wetterdienst,Meteorological Observatory Hohenpeissenberg
- harald.flentje@dwd.de
- Organisation name
- Deutscher Wetterdienst,Meteorological Observatory Hohenpeissenberg
- Organisation name
- Leibniz Institute for Tropospheric Research
- birmili@tropos.de
- Organisation name
- Leibniz Institute for Tropospheric Reseach
- Organisation name
- Leibniz Institute for Tropospheric Reseach
- birgit@tropos.de
- Organisation name
- Leibniz Institute for Tropospheric Research,
- tuch@tropos.de
- Organisation name
- Leibniz Institute for Tropospheric Research,
- andre.sonntag@tropos.de
- Organisation name
- School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway
- colin.odowd@nuigalway.ie
- Organisation name
- School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway
- Organisation name
- School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway
- regis.dupuy@nuigalway.ie
- Organisation name
- Paul Scherrer Institut, Laboratory of Atmospheric Chemistry,
- urs.baltensperger@psi.ch
- Organisation name
- Paul Scherrer Institute, Laboratory of Atmospheric Chemistry,
- Organisation name
- Institute for Applied Environmental Research, Stockholm University,
- HC@itm.su.se
- Organisation name
- Institute for Applied Environmental Research, Stockholm University,
- peter.tunved@itm.su.se
- Organisation name
- CNRS Laboratory of Meteorology Physics - Laboratory of Glaciology
- Organisation name
- Université Blaise Pascal, CNRS,
- Organisation name
- Physical Laboratory of Meteorology, University Blaise Pascal,CNRS
- Organisation name
- European Commission, Joint Research Centre, Institute for Environment and Sustainability,
- jean.putaud@jrc.it
- Organisation name
- European Commission, Joint Research Centre, Institute for Environment and Sustainability,
- carsten.gruening@jrc.it
- Organisation name
- Division of Nuclear Physics, Lund University,
- Organisation name
- Division of Nuclear Physics, Lund University,
- Organisation name
- TNO—Netherlands Organization for Applied Scientific Research,
- bas.henzing@tno.nl
- Organisation name
- Netherlands Organisation for Applied Scientific Research, TNO,
- moerman@fel.tno.nl
- Organisation name
- Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete,
- mihalo@chemistry.uoc.gr
- Organisation name
- Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete
- Organisation name
- Institute of Chemical Process Fundamentals of the AS CR,
- zdimal@icpf.cas.cz
- Organisation name
- Institute of Chemical Process Fundamentals of the AS CR,
- zikova@icpf.cas.cz
- Organisation name
- Institute of Atmospheric Sciences and Climate (ISAC) - CNR
- a.marinoni@isac.cnr.it
- Organisation name
- Institute of Atmospheric Sciences and Climate (ISAC) - CNR
- p.bonasoni@isac.cnr.it
- Organisation name
- Institute of Atmospheric Sciences and Climate (ISAC) - CNR
- R.Duchi@isac.cnr.it
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- 2012-03-15T17:24:28
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