1School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences, Harvard University, Cambridge, Massachusetts, USA
2Department of Earth and Planetary Science, Graduate school of Science, University of Tokyo, Tokyo, Japan
3Cooperative Institute for Research in the Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado, USA
4Joint Institute for the Study of Atmosphere and Ocean, 3737 Brooklyn Ave NE, Seattle, Washington, USA
*now at: Atmospheric and Oceanic Sciences, Princeton University, Princeton, New Jersey, USA
**now at: Department of Earth Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, Massachusetts, USA
***now at: University of New South Wales, Sydney, New South Wales, Australia
****now at: Royal Netherlands Meteorological Institute, De Bilt, The Netherlands
Received: 22 Jun 2011 – Published in Atmos. Chem. Phys. Discuss.: 06 Jul 2011
Abstract. We use a global chemical transport model (GEOS-Chem CTM) to interpret observations of black carbon (BC) and organic aerosol (OA) from the NASA ARCTAS aircraft campaign over the North American Arctic in April 2008, as well as longer-term records in surface air and in snow (2007–2009). BC emission inventories for North America, Europe, and Asia in the model are tested by comparison with surface air observations over these source regions. Russian open fires were the dominant source of OA in the Arctic troposphere during ARCTAS but we find that BC was of prevailingly anthropogenic (fossil fuel and biofuel) origin, particularly in surface air. This source attribution is confirmed by correlation of BC and OA with acetonitrile and sulfate in the model and in the observations. Asian emissions are the main anthropogenic source of BC in the free troposphere but European, Russian and North American sources are also important in surface air. Russian anthropogenic emissions appear to dominate the source of BC in Arctic surface air in winter. Model simulations for 2007–2009 (to account for interannual variability of fires) show much higher BC snow content in the Eurasian than the North American Arctic, consistent with the limited observations. We find that anthropogenic sources contribute 90% of BC deposited to Arctic snow in January-March and 60% in April–May 2007–2009. The mean decrease in Arctic snow albedo from BC deposition is estimated to be 0.6% in spring, resulting in a regional surface radiative forcing consistent with previous estimates.
Revised: 28 Nov 2011 – Accepted: 29 Nov 2011 – Published: 13 Dec 2011
Citation: Wang, Q., Jacob, D. J., Fisher, J. A., Mao, J., Leibensperger, E. M., Carouge, C. C., Le Sager, P., Kondo, Y., Jimenez, J. L., Cubison, M. J., and Doherty, S. J.: Sources of carbonaceous aerosols and deposited black carbon in the Arctic in winter-spring: implications for radiative forcing, Atmos. Chem. Phys., 11, 12453-12473, doi:10.5194/acp-11-12453-2011, 2011.