Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

被引:109
作者
Slowik, J. G. [1 ]
Stroud, C. [2 ]
Bottenheim, J. W. [2 ]
Brickell, P. C. [2 ]
Chang, R. Y. -W. [1 ]
Liggio, J. [2 ]
Makar, P. A. [2 ]
Martin, R. V. [3 ,4 ]
Moran, M. D. [2 ]
Shantz, N. C. [1 ,2 ]
Sjostedt, S. J. [1 ]
van Donkelaar, A. [3 ]
Vlasenko, A. [1 ,2 ]
Wiebe, H. A. [2 ]
Xia, A. G. [2 ]
Zhang, J. [2 ]
Leaitch, W. R. [2 ]
Abbatt, J. P. D. [1 ]
机构
[1] Univ Toronto, Dept Chem, Toronto, ON M5S 1A1, Canada
[2] Environm Canada, Sci & Technol Branch, Toronto, ON, Canada
[3] Dalhousie Univ, Dept Phys & Atmospher Sci, Halifax, NS, Canada
[4] Harvard Smithsonian Ctr Astrophys, Atom & Mol Phys Div, Cambridge, MA 02138 USA
关键词
POSITIVE MATRIX FACTORIZATION; CLOUD CONDENSATION NUCLEI; MULTISCALE GEM MODEL; MASS-SPECTROMETER; MEXICO-CITY; HIGH-RESOLUTION; ALPHA-PINENE; PHOTOCHEMICAL OXIDATION; SOURCE APPORTIONMENT; LIGHT-SCATTERING;
D O I
10.5194/acp-10-2825-2010
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Measurements of aerosol composition, volatile organic compounds, and CO are used to determine biogenic secondary organic aerosol (SOA) concentrations at a rural site 70 km north of Toronto. These biogenic SOA levels are many times higher than past observations and occur during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct optical scattering and higher cloud condensation nuclei numbers.
引用
收藏
页码:2825 / 2845
页数:21
相关论文
共 107 条
[91]   Boreal forests, aerosols and the impacts on clouds and climate [J].
Spracklen, Dominick V. ;
Bonn, Boris ;
Carslaw, Kenneth S. .
PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES, 2008, 366 (1885) :4613-4626
[92]   OH-reactivity of volatile organic compounds at urban and rural sites across Canada: Evaluation of air quality model predictions using speciated VOC measurements [J].
Stroud, C. A. ;
Morneau, G. ;
Makar, P. A. ;
Moran, M. D. ;
Gong, W. ;
Pabla, B. ;
Zhang, J. ;
Bouchet, V. S. ;
Fox, David ;
Venkatesh, S. ;
Wang, D. ;
Dann, T. .
ATMOSPHERIC ENVIRONMENT, 2008, 42 (33) :7746-7756
[93]   Radiocarbon (14C)-deduced biogenic and anthropogenic contributions to organic carbon (OC) of urban aerosols from Zurich, Switzerland [J].
Szidat, S ;
Jenk, TM ;
Gäggeler, HW ;
Synal, HA ;
Fisseha, R ;
Baltensperger, U ;
Kalberer, M ;
Samburova, V ;
Reimann, S ;
Kasper-Giebl, A ;
Hajdas, I .
ATMOSPHERIC ENVIRONMENT, 2004, 38 (24) :4035-4044
[94]   Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area [J].
Tsimpidi, A. P. ;
Karydis, V. A. ;
Zavala, M. ;
Lei, W. ;
Molina, L. ;
Ulbrich, I. M. ;
Jimenez, J. L. ;
Pandis, S. N. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (02) :525-546
[95]   High natural aerosol loading over boreal forests [J].
Tunved, P ;
Hansson, HC ;
Kerminen, VM ;
Ström, J ;
Dal Maso, M ;
Lihavainen, H ;
Viisanen, Y ;
Aalto, PP ;
Komppula, M ;
Kulmala, M .
SCIENCE, 2006, 312 (5771) :261-263
[96]  
Ulbrich I., 2009, AMS Spectral Database
[97]   Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data [J].
Ulbrich, I. M. ;
Canagaratna, M. R. ;
Zhang, Q. ;
Worsnop, D. R. ;
Jimenez, J. L. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (09) :2891-2918
[98]   Measurements of VOCs by proton transfer reaction mass spectrometry at a rural Ontario site: Sources and correlation to aerosol composition [J].
Vlasenko, A. ;
Slowik, J. G. ;
Bottenheim, J. W. ;
Brickell, P. C. ;
Chang, R. Y. -W. ;
Macdonald, A. M. ;
Shantz, N. C. ;
Sjostedt, S. J. ;
Wiebe, H. A. ;
Leaitch, W. R. ;
Abbatt, J. P. D. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2009, 114
[99]   Secondary organic aerosol formation from anthropogenic air pollution: Rapid and higher than expected [J].
Volkamer, Rainer ;
Jimenez, Jose L. ;
San Martini, Federico ;
Dzepina, Katja ;
Zhang, Qi ;
Salcedo, Dara ;
Molina, Luisa T. ;
Worsnop, Douglas R. ;
Molina, Mario J. .
GEOPHYSICAL RESEARCH LETTERS, 2006, 33 (17)
[100]   A study of secondary organic aerosol formation in the anthropogenic-influenced southeastern United States [J].
Weber, Rodney J. ;
Sullivan, Amy P. ;
Peltier, Richard E. ;
Russell, Armistead ;
Yan, Bo ;
Zheng, Mei ;
de Gouw, Joost ;
Warneke, Carsten ;
Brock, Charles ;
Holloway, John S. ;
Atlas, Elliot L. ;
Edgerton, Eric .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2007, 112 (D13)