References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-237-2012

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

Wespes

¹ Emmons

¹ Edwards

D. P.

¹ Hannigan

¹ Hurtmans

² Saunois

¹ Coheur

P.-F.

² Clerbaux

² ³ Coffey

M. T.

¹ Batchelor

R. L.

¹ Lindenmaier

⁴ Strong

⁴ Weinheimer

A. J.

¹ Nowak

J. B.

⁵ ⁶ Ryerson

T. B.

⁵ Crounse

J. D.

⁷ Wennberg

P. O.

⁷

National Center for Atmospheric Research, Boulder, CO, USA

Chimie Quantique et Photophysique, Université Libre de Bruxelles, Brussels, Belgium

UPMC Univ. Paris 6; Université Versailles St.-Quentin, CNRS/INSU, LATMOS-IPSL, Paris, France

Department of Physics, University of Toronto, Toronto, ON, Canada

NOAA, Earth System Research Laboratory, Boulder, CO, USA

Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, USA

California Institute of Technology, Pasadena, CA, USA

04 01 2012

12 1 237 259

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In this paper, we analyze tropospheric O3 together with HNO3 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 O3 and HNO3 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 O3 with HNO3 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 O3 and HNO3 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 O3 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 O3 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.

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