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Long-Range Transport of Sulfate to Canada GEOS-Chem Users Meeting

Long-Range Transport of Sulfate to Canada GEOS-Chem Users Meeting. Aaron van Donkelaar Dalhousie University April, 2007. NEI99. Streets. BRAVO. SO 2 emission inventories out of date Inventories used by GEOS-Chem. Global Inventories GEIA (1985) EDGAR (2000). Regional Inventories

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Long-Range Transport of Sulfate to Canada GEOS-Chem Users Meeting

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  1. Long-Range Transport of Sulfate to CanadaGEOS-Chem Users Meeting Aaron van Donkelaar Dalhousie University April, 2007

  2. NEI99 Streets BRAVO SO2 emission inventories out of date Inventories used by GEOS-Chem • Global Inventories • GEIA (1985) • EDGAR (2000) • Regional Inventories • Bravo (Mexico, 1999) • Streets (East Asia, 2000) • NEI99 (USA, 1999)

  3. Generation of Scale Factors Scale factors are used to approximate emission changes from the base year of the inventories. Regulated: limit pollutant emission (i.e. SOx, NOx, CO) • USA, Canada, Europe, Japan, etc. • Generate emission reports • EPA Acid Rain Program • The Canada-Wide Acid Rain Strategy • European Monitoring and Evaluation Program (EMEP) Unregulated: no emission controls • Asia, Africa, etc. • Must infer emissions changes from secondary sources, such as CDIAC CO2 emissions. • NOx: total CO2 • CO: liquid CO2 • SOx: solid CO2

  4. SOx Emissions Scalar (2000-2002)

  5. INTEX-B Intercontinental Chemical Transport Experiment - Phase B April/May 2006 Study influx of Asian pollution to North America Canadian Instrumentation: Cessna 207 Aircraft (Leaitch) 33 Flights AMS, O3, CO Lidar (Duck) Whistler Peak Measurements (MacDonald) AMS, O3, CO, Filter Pack

  6. GEOS-Chem successfully represents Cessna SO4= over Whistler Aerosol size limit not present in GEOS-Chem Scale AMS SO4= by average MOUDI impactor size factor (~1.4) No scaling applied to organics or nitrate Mean GEOS-Chem SO4= bias of +0.17 ug/m3 G-C (dotted) Cessna (solid) Sulfate Organics Nitrate From Rupakheti et al., 2005

  7. GEOS-Chem biased compared to DC-8 SO4= • Different sampling times and size cutoffs • Filter Pack • long sample • ~4 um cutoff • GC mean bias of +0.57 [ug/m3] • Mist Chamber • 1 min. sample • ~1 um cutoff • GC mean bias of +0.75 [ug/m3] • Filter Pack vs. Mist Chamber • 32% increase in mean model bias • role of size cutoff?

  8. SO2 measurements are well-captured above 900 mb GEOS-Chem SO2 [ppt] Pressure [mb] DC-8 • Averaged between 700 and 900 mb, filtered as Hudman et al., in press • GEOS-Chem mean bias of ~+4 ppt SO2 [ppt]

  9. GEOS-Chem SO2 columns low relative to OMI SO2 [DU] GEOS-Chem OMI SO2 [DU]

  10. Sulfate is a large component of AOD As noted by Heald et al., 2006, GEOS-Chem total AOD over pacific is low during spring AOD bias may represent underestimate in SO2 emissions or effects related to assumed size distribution MODIS AOD GEOS-Chem % AOD from SO4= GEOS-Chem MODIS GEOS-Chem AOD

  11. Influence of Asian sulfate on Canada Significant portion of SO4= over western Canada is of southeast Asian origin Eastern pollution largely north American sources Sulfur typically transported as SO4= SO4= 600 mb SO4= [ug/m3] Altitude [km] % Asian SO4= Altitude [km]

  12. Questions This research has been produced by the collaborative efforts of: Randall Martin Dalhousie University / Harvard-Smithsonian Center for Astrophysics Thomas Walker Dalhousie University Richard Leaitch, Anne Marie Macdonald, and Peter Liu Environment Canada Nickolay Krotkov Goddard Earth Sciences and Technology Center Jack Dibb University of New Hampshire Greg Huey Georgia Institute of Technology This work was supported by the National Sciences and Engineering Research Council of Canada Special Research Opportunity program.

  13. References • Brock, C., A., P. K. Hudson, E. R. Lovejoy, A. Sullivan, J. B. Nowak, L. G. Huey, O. R. Cooper, D. J. Cziczo, J. de Gouw, F. C. Fehsenfeld, J. S. Holloway, G. Hübler, B. G. Lafleur, D. M. Murphy, J. A. Neuman, D. K. Nicks, D. A. Orsini, D. D. Parish, T. B. Ryerson, D. J. Tanner, C. Varneke, R. J. Weber, and J. C. Wilson, Particle characteristics following cloud-modified transport from Asia to North America. Journal of Geophysical Research, 109, D23S26, doi: 10.1029/2003JD004198, 2004. • Heald, C. L., D. J. Jacob, R. J. Park, B. Alexander, T. D. Fairlie, R. M. Yantosca, and D. A. Chu, Transpacific transport of Asian anthropogenic aerosols and its impact on surface air quality in the United States. Journal of Geophysical Research, 111, D14310, doi:10.1029/2005JD006847, 2006. • Hudman, R. C., D. J. Jacob, S. Turquety, E. M. Leibensperger, L. T. Murray, S. Wu, A. B. Gilliland, M. Avery, T. H. Bertram, W. Brune, R. C. Cohen, J. E. Dibb, F. M. Flocke, A. Fried, J. Holloway, J. A. Neumann, R. Orville, A. Perring, X. Ren, G. W. Sachse, H. B. Singh, A. Swanson, P. J. Wooldridge, Surface and lightning sources of nitrogen oxides over the United States: magnitudes, chemical evolution, and outflow. Journal of Geophysical Research, in press. • Rupakheti, M., R. W. Leaitch, U. Lohmann, K. Hayden, P. Brickell, G. Lu, S.-M. Li, D. Toom-Sauntry, J. W. Bottenheim, J. R. Brook, R. Vet, J. T. Jayne, and D. R. Worsnop, An intensive study of the size and composition of submicron atmospheric aerosols at a rural site in Ontario, Canada. Aerosol Science and Technology, 39, 722-736, 2005.

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