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.
|
|
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 |
Simple
- Alternate title
- ACP - Special Issue
- Date ( Publication )
- 2011-12-05T00:00:00
- Edition
- Presentation form
- Hardcopy document
- Presentation form
- Digital document
- Name
- Atmospheric Chemistry and Physics, Volume 11,
- Issue identification
- 23
- Page
- 12007-12036
- Other citation details
- Atmospheric Chemistry and Physics, Volume 11, Issue 23, 2011, pp.12007-12036
- Collective title
- European Integrated Project on Aerosol-Cloud-Climate and Air Quality Interactions (EUCAARI)
- ISBN
- ISSN
- 1680-7316
- Purpose
- Status
- Completed
Publisher
Author
Author
Author
Author
Institute for Climate and Atmospheric Science, School of Earth and Environment
-
L. Collins
( )
Leeds
LS2 9JT
United Kingdom
- Website
- www.leeds.ac.uk
Author
Institute for Climate and Atmospheric Science, School of Earth and Environment
-
J. Merikanto
( )
Leeds
LS2 9JT
United Kingdom
- Website
- http://www.see.leeds.ac.uk
Author
Author
University of Helsinki, Dept of Physics,Division of Atmospheric Sciences,
-
Markku Kulmala
( )
P.O. Box 64
Helsinki
FI-00014
Finland
Author
University of Helsinki, Dept of Physics,Division of Atmospheric Sciences,
-
Pasi Aalto
( )
P.O. Box 64
Helsinki
FI-00014
Finland
Author
Institute of Atmospheric Physics,
-
Andreas Minikin
( )
Münchner Strasse 20
Oberpfaffenhofen-Wessling
82230
Germany
Author
Institute of Atmospheric Physics,
-
Thomas Hamburger
( )
Münchner Strasse 20
Oberpfaffenhofen-Wessling
82230
Germany
- Website
- http://www.dlr.de/pa
Author
School of Earth, Atmospheric and Environmental Sciences, University of Manchester,
-
Hugh Coe
( )
Williamson Building Oxford Road
Manchester
M13 9PL
United Kingdom
Author
Deutscher Wetterdienst,Meteorological Observatory Hohenpeissenberg
-
Harald Flentje
( )
Frankfurter Strasse 135
Offenbach
63067
Germany
Author
Deutscher Wetterdienst,Meteorological Observatory Hohenpeissenberg
-
Christian Plass-Dülmer
( )
Frankfurter Strasse 135
Offenbach
63067
Germany
- Website
- http://www.dwd.de/gaw
Author
Leibniz Institute for Tropospheric Research
-
Wolfram Birmili
( )
Permoserstrasse 15
Leipzig, Germany
04318
Germany
Author
Leibniz Institute for Tropospheric Reseach
-
Alfred Wiedensohler
( )
Permoserstrasse 15
Leipzig
04318
Germany
Author
Leibniz Institute for Tropospheric Reseach
-
Birgit Wehner
( )
Permoserstrasse 15
Leipzig
04318
Germany
Author
Leibniz Institute for Tropospheric Research,
-
Thomas Tuch
( )
Permoserstrasse 15
Leipzig
04318
Germany
- Website
- www.tropos.de
Author
Leibniz Institute for Tropospheric Research,
-
Andre Sonntag
( )
Permoserstrasse 15
Leipzig
04318
Germany
- Website
- http://www.tropos.de
Author
Author
Author
School of Physics & Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway
-
Regis Dupuy
( )
University Road
Galway
Galway
Ireland
Author
Author
Author
Institute for Applied Environmental Research, Stockholm University,
-
Hans-Christen Hansson
( )
ITM, Stockholm University,
Stockholm
SE-106 91
Sweden
Author
Institute for Applied Environmental Research, Stockholm University,
-
Peter Tunved
( )
ITM, Stockholm University,
Stockholm
SE-106 91
Sweden
Author
CNRS Laboratory of Meteorology Physics - Laboratory of Glaciology
-
Paolo Laj
( )
Avenue des Landais
Aubiere Cedex
63177
France
Author
Author
Physical Laboratory of Meteorology, University Blaise Pascal,CNRS
-
Julien Boulon
( )
24,avenue des Landais
Aubière
63177
France
Author
European Commission, Joint Research Centre, Institute for Environment and Sustainability,
-
Jean Philippe Putaud
( )
Via E. Fermi 2749
Ispra
VA
21027
Italy
Author
European Commission, Joint Research Centre, Institute for Environment and Sustainability,
-
Carsten Gruening
( )
Via E. Fermi 2749
Ispra
VA
21027
Italy
Author
Author
- Website
- http://www.lth.se
Author
TNO—Netherlands Organization for Applied Scientific Research,
-
J. S. Henzing
( )
Princetonlaan 6
Utrecht
7334 DT
Netherlands
Author
Netherlands Organisation for Applied Scientific Research, TNO,
-
Marcel Moerman
( )
P.O. Box 96864
The Hague
JG
2509
Netherlands
- Website
- http://www.tno.nl
Author
Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete,
-
Nikolaos Mihalopoulos
( )
POBox 2208
Heraklion
Crete
71003
Greece
Author
Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete
-
Giorgios Kouvarakis
( )
POBox 2208
Heraklion
Crete
71003
Greece
Author
Institute of Chemical Process Fundamentals of the AS CR,
-
Vladimír Ždímal
( )
Rozvojová 135/1
Prague
Praha-Lysolaje
165 02
Czech Republic
Author
Institute of Chemical Process Fundamentals of the AS CR,
-
Nadežda Zíková
( )
Rozvojová 135/1
Prague
Praha-Lysolaje
165 02
Czech Republic
Author
Institute of Atmospheric Sciences and Climate (ISAC) - CNR
-
Angela Marinoni
( )
Via Gobetti,101
Bologna
BO
40129
Italy
Author
Institute of Atmospheric Sciences and Climate (ISAC) - CNR
-
Paolo Bonasoni
( )
Via Gobetti,101
Bologna
BO
40129
Italy
Author
Institute of Atmospheric Sciences and Climate (ISAC) - CNR
-
Rocco Duchi
( )
Via Gobetti,101
Bologna
BO
40129
Italy
- Website
- www.isac.cnr.it
- Maintenance and update frequency
- As needed
- Keywords ( Theme )
-
- SHARE
- Keywords
-
- European Integrated Project , Air Quality Interactions (EUCAARI) , Aerosol , Cloud , Climate
- Keywords ( Place )
-
- Europe
- Keywords
-
- particle number concentrations , boundary layer , primary particles , secondary particles
- Access constraints
- Copyright
- Use constraints
- Copyright
- Other constraints
- Metadata language
- eng
- Character set
- UTF8
- Topic category
-
- Climatology, meteorology, atmosphere
- Environment
N
S
E
W
))
- Distribution format
-
- ( )
- OnLine resource
-
Abstract:"Primary versus secondary contributions to particle number concentrations in the European boundary layer."
Abstract:"Primary versus secondary contributions to particle number concentrations in the European boundary layer."
- OnLine resource
-
acp-11-12007-2011.pdf
Full Text(pdf):"Primary versus secondary contributions to particle number concentrations in the European boundary layer."
- Hierarchy level
- Series
- Dataset
- Statement
-
"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.
gmd:MD_Metadata
- File identifier
- 8796a712-80a0-4b91-99cf-a5f451516215 XML
- Metadata language
- eng
- Character set
- UTF8
- Date stamp
- 2012-03-15T17:24:28
- Metadata standard name
- ISO 19115:2003/19139
- Metadata standard version
- 1.0
Point of contact
Overviews
thumbnail
Provided by
Views
8796a712-80a0-4b91-99cf-a5f451516215
Access to the portal
Read here the full details and access to the data.
Associated resources
Not available