Atmos. Chem. Phys. Discuss., 10, 24781-24820, 2010
www.atmos-chem-phys-discuss.net/10/24781/2010/
doi:10.5194/acpd-10-24781-2010
© Author(s) 2010. This work is distributed
under the Creative Commons Attribution 3.0 License.
Review Status
This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
The effect of meteorological and chemical factors on the agreement between observations and predictions of fine aerosol composition in Southwestern Ontario during BAQS-Met
M. Z. Markovic1, K. L. Hayden2, J. G. Murphy1, P. A. Makar2, R. A. Ellis1, R. Y.-W. Chang1, J. G. Slowik1, C. Mihele2, and J. Brook2
1Department of Chemistry, University of Toronto, Toronto, Ontario, Canada
2Air Quality Research Division, Environment Canada, Toronto, Ontario, Canada

Abstract. The Border Air Quality and Meteorology Study (BAQS-Met) was an intensive, collaborative field campaign during the summer of 2007 that investigated the effects of transboundary pollution, local pollution, and local meteorology on regional air quality in Southwestern Ontario. This analysis focuses on the measurements of the inorganic constituents of particulate matter with diameter of less than 1 μm (PM1), with a specific emphasis on nitrate. We evaluate the ability of AURAMS, the Environment Canada's chemical transport model, to represent regional air pollution in SW Ontario by comparing modelled aerosol inorganic chemical composition with measurements from Aerosol Mass Spectrometers (AMS) onboard the National Research Council (NRC) of Canada Twin Otter aircraft and at a ground site in Harrow, ON. The agreement between modelled and measured pNO3 at the ground site (observed mean (M_obs) = 0.50 μg m−3; modelled mean (M_mod) = 0.58 μg m−3; root mean square error (RSME) = 1.27 μg m−3) was better than aloft (M_obs = 0.32 μg m−3; M_mod = 0.09 μg m−3; RSME = 0.48 μg m−3). Possible reasons for discrepancies include errors in (i) emission inventories, (ii) atmospheric chemistry, (iii) predicted meteorological parameters, or (iv) gas/particle thermodynamics in the model framework. Using the inorganic thermodynamics model, ISORROPIA, in an offline mode, we find that the assumption of thermodynamic equilibrium is consistent with observations of gas and particle composition at Harrow. We develop a framework to assess the sensitivity of PM1 nitrate to meteorological and chemical parameters and find that errors in both the predictions of relative humidity and free ammonia (FA ≡ NH3(g) + NH4+ − SO42−) are responsible for the poor agreement between modelled and measured values.

Citation: Markovic, M. Z., Hayden, K. L., Murphy, J. G., Makar, P. A., Ellis, R. A., Chang, R. Y.-W., Slowik, J. G., Mihele, C., and Brook, J.: The effect of meteorological and chemical factors on the agreement between observations and predictions of fine aerosol composition in Southwestern Ontario during BAQS-Met, Atmos. Chem. Phys. Discuss., 10, 24781-24820, doi:10.5194/acpd-10-24781-2010, 2010.
 
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