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Analysis of ozone and nitric acid in spring and summer Arctic pollution using aircraft, ground-based, satellite observations and MOZART-4 model: source attribution and partitioning

Wespes, C. and Emmons, L. and Edwards, D. P. and Hannigan, J. and Hurtmans, D. and Saunois, M. and Coheur, P. -F. and Clerbaux, C. and Coffey, M. T. and Batchelor, R. L. and Lindenmaier, R. and Strong, K. and Weinheimer, A. J. and Nowak, J. B. and Ryerson, T. B. and Crounse, J. D. and Wennberg, P. O. (2012) Analysis of ozone and nitric acid in spring and summer Arctic pollution using aircraft, ground-based, satellite observations and MOZART-4 model: source attribution and partitioning. Atmospheric Chemistry and Physics, 12 (1). pp. 237-259. ISSN 1680-7316. doi:10.5194/acp-12-237-2012.

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In this paper, we analyze tropospheric O_3 together with HNO_3 during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport) program, combining observations and model results. Aircraft observations from the NASA ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) and NOAA ARCPAC (Aerosol, Radiation and Cloud Processes affecting Arctic Climate) campaigns during spring and summer of 2008 are used together with the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) to assist in the interpretation of the observations in terms of the source attribution and transport of O_3 and HNO_3 into the Arctic (north of 60° N). The MOZART-4 simulations reproduce the aircraft observations generally well (within 15%), but some discrepancies in the model are identified and discussed. The observed correlation of O_3 with HNO_3 is exploited to evaluate the MOZART-4 model performance for different air mass types (fresh plumes, free troposphere and stratospheric-contaminated air masses). Based on model simulations of O_3 and HNO_3 tagged by source type and region, we find that the anthropogenic pollution from the Northern Hemisphere is the dominant source of O3 and HNO3 in the Arctic at pressures greater than 400 hPa, and that the stratospheric influence is the principal contribution at pressures less 400 hPa. During the summer, intense Russian fire emissions contribute some amount to the tropospheric columns of both gases over the American sector of the Arctic. North American fire emissions (California and Canada) also show an important impact on tropospheric ozone in the Arctic boundary layer. Additional analysis of tropospheric O_3 measurements from ground-based FTIR and from the IASI satellite sounder made at the Eureka (Canada) and Thule (Greenland) polar sites during POLARCAT has been performed using the tagged contributions. It demonstrates the capability of these instruments for observing pollution at northern high latitudes. Differences between contributions from the sources to the tropospheric columns as measured by FTIR and IASI are discussed in terms of vertical sensitivity associated with these instruments. The first analysis of O_3 tropospheric columns observed by the IASI satellite instrument over the Arctic is also provided. Despite its limited vertical sensitivity in the lowermost atmospheric layers, we demonstrate that IASI is capable of detecting low-altitude pollution transported into the Arctic with some limitations.

Item Type:Article
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URLURL TypeDescription
Weinheimer, A. J.0000-0001-6175-8286
Ryerson, T. B.0000-0003-2800-7581
Crounse, J. D.0000-0001-5443-729X
Wennberg, P. O.0000-0002-6126-3854
Additional Information:© 2012 Author(s). This work is distributed under the Creative Commons Attribution 3.0 License.. Received: 13 July 2011; Published in Atmos. Chem. Phys. Discuss.: 22 August 2011; Revised: 12 December 2011; Accepted: 14 December 2011; Published: 4 January 2012. The National Center for Atmospheric Research is supported by the National Science Foundation. The NCAR FTS observation program at Thule, GR is supported under contract by the National Aeronautics and Space Administration (NASA). This work is also supported by the NSF Office of Polar Programs (OPP). We wish to thank the Danish Meteorological Institute for support at the Thule site. The PEARL Bruker 125HR measurements at Eureka were made by the Canadian Network for the Detection of Atmospheric Change (CANDAC), led by James R. Drummond, and in part by the Canadian Arctic ACE Validation Campaigns, led by Kaley A. Walker. They were supported by the Atlantic Innovation Fund/Nova Scotia Research Innovation Trust, Canada Foundation for Innovation, Canadian Foundation for Climate and Atmospheric Sciences, Canadian Space Agency, Environment Canada, Government of Canada International Polar Year funding, Natural Sciences and Engineering Research Council, Northern Scientific Training Program, Ontario Innovation Trust, Polar Continental Shelf Program, and Ontario Research Fund. The authors wish to thank PEARL site manager Pierre F. Fogal, the CANDAC operators, and the staff at Environment Canada’s Eureka weather station for logistical and on-site support. IASI has been developed and built under the responsibility of the Centre National d’Etudes Spatiales (CNES, France). It is flown onboard the Metop satellites as part of the EUMETSAT Polar System. The IASI L1 data are received through the EUMETCast near real time data distribution service. P. F. Coheur is Research Associate (Chercheur Qualifié) with F.R.S.-FNRS. The research in Belgium was funded by the F.R.S.-FNRS (M.I.S. nF.4511.08), the Belgian State Federal Office for Scientific, Technical and Cultural Affairs and the European Space Agency (ESA-Prodex arrangements). Financial support by the ‘Actions de Recherche Concertées’ (Communauté Française de Belgique) is also acknowledged. The research in France is supported by CNES. This research has been supported by NASA’s Tropospheric Chemistry Program (ARCTAS) under grant NNX08AD22G, NNX08AD29G, and NNX07AL57G.
Funding AgencyGrant Number
Atlantic Innovation Fund/Nova Scotia Research Innovation TrustUNSPECIFIED
Canada Foundation for InnovationUNSPECIFIED
Canadian Foundation for Climate and Atmospheric SciencesUNSPECIFIED
Canadian Space Agency (CSA)UNSPECIFIED
Environment CanadaUNSPECIFIED
Government of Canada International Polar YearUNSPECIFIED
Natural Sciences and Engineering Research Council of Canada (NSERC)UNSPECIFIED
Northern Scientific Training ProgramUNSPECIFIED
Ontario Innovation TrustUNSPECIFIED
Polar Continental Shelf ProgramUNSPECIFIED
Ontario Research FundUNSPECIFIED
F.R.S.-FNRSM.I.S. nF.4511.08
Belgian State Federal Office for Scientific, Technical and Cultural AffairsUNSPECIFIED
European Space Agency (ESA-Prodex arrangements)UNSPECIFIED
Actions de Recherche Concertées (Communauté Française de Belgique)UNSPECIFIED
Centre National d'Études Spatiales (CNES)UNSPECIFIED
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Record Number:CaltechAUTHORS:20120305-121701322
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Official Citation:Wespes, C., Emmons, L., Edwards, D. P., Hannigan, J., Hurtmans, D., Saunois, M., Coheur, P.-F., Clerbaux, C., Coffey, M. T., Batchelor, R. L., Lindenmaier, R., Strong, K., Weinheimer, A. J., Nowak, J. B., Ryerson, T. B., Crounse, J. D., and Wennberg, P. O.: Analysis of ozone and nitric acid in spring and summer Arctic pollution using aircraft, ground-based, satellite observations and MOZART-4 model: source attribution and partitioning, Atmos. Chem. Phys., 12, 237-259, doi:10.5194/acp-12-237-2012, 2012.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:29577
Deposited By: Jason Perez
Deposited On:13 Mar 2012 18:10
Last Modified:09 Nov 2021 17:08

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