Journal cover Journal topic
Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
Atmos. Chem. Phys., 14, 10845-10895, 2014
http://www.atmos-chem-phys.net/14/10845/2014/
doi:10.5194/acp-14-10845-2014
© Author(s) 2014. This work is distributed
under the Creative Commons Attribution 3.0 License.
Research article
15 Oct 2014
The AeroCom evaluation and intercomparison of organic aerosol in global models
K. Tsigaridis1,2, N. Daskalakis3,4, M. Kanakidou3, P. J. Adams5,6, P. Artaxo7, R. Bahadur8, Y. Balkanski9, S. E. Bauer1,2, N. Bellouin10,a, A. Benedetti11, T. Bergman12, T. K. Berntsen13,14, J. P. Beukes15, H. Bian16, K. S. Carslaw17, M. Chin18, G. Curci19, T. Diehl18,20, R. C. Easter21, S. J. Ghan21, S. L. Gong22, A. Hodzic23, C. R. Hoyle24,25, T. Iversen11,13,26, S. Jathar5, J. L. Jimenez27, J. W. Kaiser11,28,29, A. Kirkevåg26, D. Koch1,2,b, H. Kokkola12, Y. H Lee5,c, G. Lin30, X. Liu21,d, G. Luo31, X. Ma32,e, G. W. Mann33,34, N. Mihalopoulos3, J.-J. Morcrette11, J.-F. Müller35, G. Myhre14, S. Myriokefalitakis3,4, N. L. Ng36, D. O'Donnell37,f, J. E. Penner30, L. Pozzoli38, K. J. Pringle29,39, L. M. Russell9, M. Schulz26, J. Sciare9, Ø. Seland26, D. T. Shindell1,2,g, S. Sillman30, R. B. Skeie14, D. Spracklen17, T. Stavrakou35, S. D. Steenrod20, T. Takemura40, P. Tiitta15,41, S. Tilmes23, H. Tost42, T. van Noije43, P. G. van Zyl15, K. von Salzen32, F. Yu31, Z. Wang44, Z. Wang45, R. A. Zaveri21, H. Zhang44, K. Zhang21,37, Q. Zhang46, and X. Zhang45 1Center for Climate Systems Research, Columbia University, New York, NY, USA
2NASA Goddard Institute for Space Studies, New York, NY, USA
3Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete, Heraklion, Greece
4Institute of Chemical Engineering, Foundation for Research and Technology Hellas (ICE-HT FORTH), Patras, Greece
5Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, PA, USA
6Department of Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, PA, USA
7University of São Paulo, Department of Applied Physics, Brazil
8Scripps Institution of Oceanography, University of California San Diego, CA, USA
9Laboratoire des Sciences du Climat et de l'Environnement, Gif-sur-Yvette, France
10Met Office Hadley Centre, Exeter, UK
11ECMWF, Reading, UK
12Finnish Meteorological Institute, Kuopio, Finland
13University of Oslo, Department of Geosciences, Oslo, Norway
14Center for International Climate and Environmental Research – Oslo (CICERO), Oslo, Norway
15Environmental Sciences and Management, North-West University, Potchefstroom, South Africa
16University of Maryland, Joint Center for Environmental Technology, Baltimore County, MD, USA
17School of Earth and Environment, University of Leeds, Leeds, UK
18NASA Goddard Space Flight Center, Greenbelt, MD, USA
19Department of Physics CETEMPS, University of L'Aquila, Italy
20Universities Space Research Association, Greenbelt, MD, USA
21Pacific Northwest National Laboratory; Richland, WA, USA
22Air Quality Research Branch, Meteorological Service of Canada, Toronto, Ontario, Canada
23National Center for Atmospheric Research, Boulder, CO, USA
24Paul Scherrer Institute, Villigen, Switzerland
25Swiss Federal Institute for Forest Snow and Landscape Research (WSL) – Institute for Snow and Avalanche Research (SLF), Davos, Switzerland
26Norwegian Meteorological Institute, Oslo, Norway
27University of Colorado, Department of Chemistry & Biochemistry, Boulder, CO, USA
28King's College London, Department of Geography, London, UK
29Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
30Department of Atmospheric, Oceanic, and Space Sciences, University of Michigan, Ann Arbor, MI, USA
31State University of New York, Albany, NY, USA
32Environment Canada, Victoria, Canada
33National Centre for Atmospheric Science, University of Leeds, Leeds, UK
34School of Earth and Environment, University of Leeds, Leeds, UK
35Belgian Institute for Space Aeronomy, Brussels, Belgium
36School of Chemical and Biomolecular Engineering and School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
37Max Planck Institute for Meteorology, Hamburg, Germany
38Eurasia Institute of Earth Sciences, Istanbul Technical University, Turkey
39Institute for Climate and Atmospheric Science, School or Earth and Environment, University of Leeds, Leeds, UK
40Research Institute for Applied Mechanics, Kyushu University, Fukuoka, Japan
41Fine Particle and Aerosol Technology Laboratory, Department of Environmental Science, University of Eastern Finland, Kuopio, Finland
42Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
43Royal Netherlands Meteorological Institute (KNMI), De Bilt, the Netherlands
44Laboratory for Climate Studies, Climate Center, China Meteorological Administration, Beijing, China
45Chinese Academy of Meteorological Sciences, Beijing, China
46Department of Environmental Toxicology, University of California, Davis, CA, USA
anow at: Department of Meteorology, University of Reading, Reading, UK
bnow at: Department of Energy, Office of Biological and Environmental Research, Washington, DC, USA
cnow at: Center for Climate Systems Research, Columbia University, New York, NY, USA and NASA Goddard Institute for Space Studies, New York, NY, USA
dnow at: University of Wyoming, Department of Atmospheric Science, Laramie, WY, USA
enow at: State University of New York, Department of Atmospheric Science, Albany, NY, USA
fnow at: Finnish Meteorological Institute, Helsinki, Finland
gnow at: Nicholas School of the Environment, Duke University, Durham, NC, USA
Abstract. This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models.

The median global primary OA (POA) source strength is 56 Tg a−1 (range 34–144 Tg a−1) and the median SOA source strength (natural and anthropogenic) is 19 Tg a−1 (range 13–121 Tg a−1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a−1 (range 16–121 Tg a−1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a−1; range 13–20 Tg a−1, with one model at 37 Tg a−1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a−1 (range 28–209 Tg a−1), which is on average 85% of the total OA deposition.

Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern.

Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to −0.62 (−0.51) based on the comparison against OC (OA) urban data of all models at the surface, −0.15 (+0.51) when compared with remote measurements, and −0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.


Citation: Tsigaridis, K., Daskalakis, N., Kanakidou, M., Adams, P. J., Artaxo, P., Bahadur, R., Balkanski, Y., Bauer, S. E., Bellouin, N., Benedetti, A., Bergman, T., Berntsen, T. K., Beukes, J. P., Bian, H., Carslaw, K. S., Chin, M., Curci, G., Diehl, T., Easter, R. C., Ghan, S. J., Gong, S. L., Hodzic, A., Hoyle, C. R., Iversen, T., Jathar, S., Jimenez, J. L., Kaiser, J. W., Kirkevåg, A., Koch, D., Kokkola, H., Lee, Y. H., Lin, G., Liu, X., Luo, G., Ma, X., Mann, G. W., Mihalopoulos, N., Morcrette, J.-J., Müller, J.-F., Myhre, G., Myriokefalitakis, S., Ng, N. L., O'Donnell, D., Penner, J. E., Pozzoli, L., Pringle, K. J., Russell, L. M., Schulz, M., Sciare, J., Seland, Ø., Shindell, D. T., Sillman, S., Skeie, R. B., Spracklen, D., Stavrakou, T., Steenrod, S. D., Takemura, T., Tiitta, P., Tilmes, S., Tost, H., van Noije, T., van Zyl, P. G., von Salzen, K., Yu, F., Wang, Z., Wang, Z., Zaveri, R. A., Zhang, H., Zhang, K., Zhang, Q., and Zhang, X.: The AeroCom evaluation and intercomparison of organic aerosol in global models, Atmos. Chem. Phys., 14, 10845-10895, doi:10.5194/acp-14-10845-2014, 2014.
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