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Published January 4, 2012 | Published
Journal Article Open

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

Abstract

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.

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.

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