Urban Toronto fine particulate matter (PM2.5) was physically and chemically characterized by online aerosol laser ablation mass spectrometry (LAMS) between January 2002 and February 2003. The mass spectra from the analysis of individual aerosol particles were classified according to chemical composition by a neural network approach called adaptive resonance theory (ART-2a). Temporal trends of the hourly analysis rate of over 120 different particles types were constructed and subjected to positive matrix factorization (PMF). This receptor modeling technique enabled the identification of nine distinct emission sources responsible for these particle types: biogenic, mixed crustal, organic nitrate, construction dust, Toronto soil/road salt, secondary salt, wood burning, intercontinental dust, and an unknown source of aluminum fluoride dust. Episodic events occurred with the wood burning, intercontinental dust, and unknown dust sources. This is the first paper reporting the application of PMF to single-particle spectral data.

Abstract. Tropospheric NO 2 vertical column densities have been retrieved and compared for the first time in Toronto, Canada, using three methods of differing spatial scales. Remotely sensed NO 2 vertical column densities, retrieved from multi-axis differential optical absorption spectroscopy and satellite remote sensing, were evaluated by comparison with in situ vertical column densities estimated using a pair of chemiluminescence monitors situated 0.01 and 0.5 km a.g.l. (above ground level). The chemiluminescence measurements were corrected for the influence of NO z , which reduced the NO 2 concentrations at 0.01 and 0.5 km by an average of 8 ± 1 % and 12 ± 1 %, respectively. The average absolute decrease in the chemiluminescence NO 2 measurement as a result of this correction was less than 1 ppb. The monthly averaged ratio of the NO 2 concentration at 0.5 to 0.01 km varied seasonally, and exhibited a negative linear dependence on the monthly average temperature, with Pearson's R = 0.83. During the coldest month, February, this ratio was 0.52 ± 0.04, while during the warmest month, July, this ratio was 0.34 ± 0.04, illustrating that NO 2 is not well mixed within 0.5 km above ground level. Good correlation was observed between the remotely sensed and in situ NO 2 vertical column densities (Pearson's R value ranging from 0.72 to 0.81), but the in situ vertical column densities were 52 to 58 % greater than the remotely sensed columns. These results indicate that NO 2 horizontal heterogeneity strongly impacted the magnitude of the remotely sensed columns. The in situ columns reflected an urban environment with major traffic sources, while the remotely sensed NO 2 vertical column densities were representative of the region, which included spatial heterogeneity introduced by residential neighbourhoods and Lake Ontario. Despite the difference in absolute values, the reasonable correlation between the vertical column densities determined by three distinct methods increased confidence in the validity of the values provided by each measurement technique.

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