References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-2991-2011

Photochemical processing of organic aerosol at nearby continental sites: contrast between urban plumes and regional aerosol

Slowik

J. G.

¹ ³ ⁵ Brook

⁴ Chang

R. Y.-W.

¹ ³ Evans

G. J.

² ³ Hayden

⁴ Jeong

C.-H.

⁴ Li

S.-M.

⁴ Liggio

⁴ Liu

P. S. K.

⁴ McGuire

² ³ Mihele

⁴ Sjostedt

¹ ³ ⁴ Vlasenko

¹ ³ ⁴ Abbatt

J. P. D.

¹ ²

Department of Chemistry, University of Toronto, Toronto, Canada

Department of Chemical Engineering and Applied Chemistry, University of Toronto, Toronto, Canada

Southern Ontario Centre for Atmospheric Aerosol Research, University of Toronto, Toronto, Canada

Science and Technology Branch, Environment Canada, Toronto, Canada

now at: Paul Scherrer Institut, 5232 Villigen PSI, Switzerland

31 03 2011

11 6 2991 3006

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/2991/2011/acp-11-2991-2011.pdf

As part of the BAQS-Met 2007 field campaign, Aerodyne time-of-flight aerosol mass spectrometers (ToF-AMS) were deployed at two sites in southwestern Ontario from 17 June to 11 July 2007. One instrument was located at Harrow, ON, a rural, agriculture-dominated area approximately 40 km southeast of the Detroit/Windsor/Windsor urban area and 5 km north of Lake Erie. The second instrument was located at Bear Creek, ON, a rural site approximately 70 km northeast of the Harrow site and 50 km east of Detroit/Windsor. Positive matrix factorization analysis of the combined organic mass spectral dataset yields factors related to secondary organic aerosol (SOA), direct emissions, and a factor tentatively attributed to the reactive uptake of isoprene and/or condensation of its early generation reaction products. This is the first application of PMF to simultaneous AMS measurements at different sites, an approach which allows for self-consistent, direct comparison of the datasets. Case studies are utilized to investigate processing of SOA from (1) fresh emissions from Detroit/Windsor and (2) regional aerosol during periods of inter-site flow. A strong correlation is observed between SOA/excess CO and photochemical age as represented by the NOx/NOy ratio for Detroit/Windsor outflow. Although this correlation is not evident for more aged air, measurements at the two sites during inter-site transport nevertheless show evidence of continued atmospheric processing by SOA production. However, the rate of SOA production decreases with airmass age from an initial value of ~10.1 μg m−3 ppmvCO−1 h−1 for the first ~10 h of plume processing to near-zero in an aged airmass (i.e. after several days). The initial SOA production rate is comparable to the observed rate in Mexico City over similar timescales.

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