Atmospheric Chemistry and Physics
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2010
10.5194/acp-10-647-2010
http://www.atmos-chem-phys.net/10/647/2010/
http://www.atmos-chem-phys.net/10/647/2010/acp-10-647-2010.html
http://www.atmos-chem-phys.net/10/647/2010/acp-10-647-2010.pdf
647
668
2010-01-22
Contributions from transport, solid fuel burning and cooking to primary organic aerosols in two UK cities
J. D. Allan
james.allan@manchester.ac.uk
P. I. Williams
W. T. Morgan
C. L. Martin
M. J. Flynn
J. Lee
E. Nemitz
G. J. Phillips
M. W. Gallagher
H. Coe
National Centre for Atmospheric Science, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK
School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK
National Centre for Atmospheric Science, The University of York, Heslington, York, YO10 5DD, UK
Centre for Ecology and Hydrology, Bush Estate, Penicuik, Midlothian, EH26 0QB, UK
Organic matter frequently represents the single largest fraction of fine
particulates in urban environments and yet the exact contributions from
different sources and processes remain uncertain, owing in part to its
substantial chemical complexity. Positive Matrix Factorisation (PMF) has
recently proved to be a powerful tool for the purposes of source attribution
and profiling when applied to ambient organic aerosol data from the Aerodyne
Aerosol Mass Spectrometer (AMS). Here we present PMF analysis applied to AMS
data from UK cities for the first time. Three datasets are analysed, with
the focus on objectivity and consistency. The data were collected in London
during the Regent's Park and Tower Environmental Experiment (REPARTEE)
intensives and Manchester. These occurred during the autumn and wintertime,
such that the primary fraction would be prominent. Ambiguities associated
with rotationality within sets of potential solutions are explored and the
most appropriate solution sets selected based on comparisons with external
data. In addition to secondary organic aerosols, three candidate sources of
primary organic aerosol (POA) were identified according to mass spectral and
diurnal profiles; traffic emissions, cooking and solid fuel burning (for
space heating). Traffic represented, on average, 40% of POA during
colder conditions and exhibited a hydrocarbon-like mass spectrum similar to
those previously reported. Cooking aerosols represented 34% of POA and
through laboratory work, their profile was matched with that sampled from
the heating of seed oils, rather than previously-published spectra derived
from charbroiling. This suggests that in these locations, oil from frying
may have contributed more to the particulate than the meat itself. Solid
fuel aerosols represented 26% of POA during cold weather conditions but
were not discernable during the first REPARTEE campaign, when conditions
were warmer than the other campaigns. This factor showed features associated
with biomass burning and occurred mainly at night. Grid-scale emission
factors of the combustion aerosols suitable for use in chemical transport
models were derived relative to CO and NO<sub>x</sub>. The traffic aerosols were
found to be 20.5 μg m<sup>−3</sup> ppm<sup>−1</sup> relative to CO for Manchester
and 31.6 μg m<sup>−3</sup> ppm<sup>−1</sup> relative to NO<sub>x</sub> for London. Solid
fuel emissions were derived as 24.7 μg m<sup>−3</sup> ppm<sup>−1</sup> relative to
CO for Manchester. These correspond to mass emission ratios of 0.018, 0.026
(as NO) and 0.021 respectively and are of a similar order to previously
published estimates, derived from other regions or using other approaches.
Aiken, A. C., DeCarlo, P. F., and Jimenez, J. L.: Elemental analysis of organic species with electron ionization high-resolution mass spectrometry, Anal. Chem., 79, 8350–8358, 2007.
Aiken, A. C., Decarlo, P. F., Kroll, J. H., Worsnop, D. R., Huffman, J. A., Docherty, K. S., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D., Sun, Y., Zhang, Q., Trimborn, A., Northway, M., Ziemann, P. J., Canagaratna, M. R., Onasch, T. B., Alfarra, M. R., Prevot, A. S. H., Dommen, J., Duplissy, J., Metzger, A., Baltensperger, U., and Jimenez, J. L.: O/c and om/oc ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry, Environ. Sci. Technol., 42, 44780–4485, 2008.
Alfarra, M. R.: Insights into atmospheric organic aerosols using an aerosol mass spectrometer, PhD~Thesis, Department of Chemical Engineering, UMIST, Manchester, UK, 2004.
Alfarra, M. R., Coe, H., Allan, J. D., Bower, K. N., Boudries, H., Canagaratna, M. R., Jimenez, J. L., Jayne, J. T., Garforth, A., Li, S., and Worsnop, D. R.: Characterization of urban and rural organic particulate in the lower fraser valley using two aerodyne aerosol mass spectrometers, Atmos. Environ., 38, 5745–5758, 2004.
Alfarra, M. R., Prevot, A. S. H., Szidat, S., Sandradewi, J., Weimer, S., Lanz, V. A., Schreiber, D., Mohr, M., and Baltensperger, U.: Identification of the mass spectral signature of organic aerosols from wood burning emissions, Environ. Sci. Technol., 41, 5770–5777, doi:10.1021/Es062289b, 2007.
Allan, J. D., Alfarra, M. R., Bower, K. N., Williams, P. I., Gallagher, M. W., Jimenez, J. L., McDonald, A. G., Nemitz, E., Canagaratna, M. R., Jayne, J. T., Coe, H., and Worsnop, D. R.: Quantitative sampling using an aerodyne aerosol mass spectrometer – 2 Measurements of fine particulate chemical composition in two UK Cities, J. Geophys. Res.-Atmos., 108, 4091, doi:10.1029/2002JD002359, 2003a.
Allan, J. D., Jimenez, J. L., Williams, P. I., Alfarra, M. R., Bower, K. N., Jayne, J. T., Coe, H., and Worsnop, D. R.: Quantitative sampling using an aerodyne aerosol mass spectrometer – 1 Techniques of data interpretation and error analysis, J. Geophys. Res.-Atmos., 108, 4090, doi:10.1029/2002JD002358, 2003b.
Allan, J. D.: An aerosol mass spectrometer: Instrument development, data analysis techniques and quantitative atmospheric particulate measurements, PhD~Thesis, Department of Physics, UMIST, Manchester, 2004.
Allan, J. D., Coe, H., Bower, K. N., Alfarra, M. R., Delia, A. E., Jimenez, J. L., Middlebrook, A. M., Drewnick, F., Onasch, T. B., Canagaratna, M. R., Jayne, J. T., and Worsnop, D. R.: A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data, J. Aerosol. Sci., 35, 909–922, 2004.
Ams spectral database (unit mass resolution): http://cires.colorado.edu/jimenez-group/AMSsd/, last access: July~2009, 2009.
Bond, T. C., Streets, D. G., Yarber, K. F., Nelson, S. M., Woo, J. H., and Klimont, Z.: A technology-based global inventory of black and organic carbon emissions from combustion, J. Geophys. Res.-Atmos., 109, D14203, doi:10.1029/2003jd003697, 2004.
Bond, T. C., Habib, G., and Bergstrom, R. W.: Limitations in the enhancement of visible light absorption due to mixing state, J. Geophys. Res.-Atmos., 111, D20211, doi:10.1029/2006jd007315, 2006.
Canagaratna, M. R., Jayne, J. T., Ghertner, D. A., Herndon, S., Shi, Q., Jimenez, J. L., Silva, P. J., Williams, P., Lanni, T., Drewnick, F., Demerjian, K. L., Kolb, C. E., and Worsnop, D. R.: Chase studies of particulate emissions from in-use new york city vehicles, Aerosol Sci. Tech., 38, 555–573, 2004.
Canagaratna, M. R., Jayne, J. T., Jimenez, J. L., Allan, J. D., Alfarra, M. R., Zhang, Q., Onasch, T. B., Drewnick, F., Coe, H., Middlebrook, A., Delia, A., Williams, L. R., Trimborn, A. M., Northway, M. J., DeCarlo, P. F., Kolb, C. E., Davidovits, P., and Worsnop, D. R.: Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer, Mass Spectrom. Rev., 26, 185–222, 2007.
Capes, G., Johnson, B., McFiggans, G., Williams, P. I., Haywood, J., and Coe, H.: Aging of biomass burning aerosols over west africa: Aircraft measurements of chemical composition, microphysical properties, and emission ratios, J. Geophys. Res.-Atmos., 113, D00c15, doi:10.1029/2008jd009845, 2008.
Colvile, R. N., Hutchinson, E. J., Mindell, J. S., and Warren, R. F.: The transport sector as a source of air pollution, Atmos. Environ., 35, 1537–1565, 2001.
Corris, B.: Atmospheric aerosol: The link between compostion and physical behaviour, PhD~Thesis, School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Manchester, 2008.
Crosier, J., Allan, J. D., Coe, H., Bower, K. N., Formenti, P., and Williams, P. I.: Chemical composition of summertime aerosol in the po valley (italy), northern adriatic and black sea, Q. J. Roy. Meteor. Soc., 133, 61–75, doi:10.1002/qj.88, 2007.
Cross, E. S., Slowik, J. G., Davidovits, P., Allan, J. D., Worsnop, D. R., Jayne, J. T., Lewis, D. K., Canagaratna, M., and Onasch, T. B.: Laboratory and ambient particle density determinations using light scattering in conjunction with aerosol mass spectrometry, Aerosol Sci. Tech., 41, 343–359, 2007.
Dall'Osto, M., Harrison, R. M., Coe, H., and Williams, P.: Real-time secondary aerosol formation during a fog event in London, Atmos. Chem. Phys., 9, 2459–2469, 2009.
Dall'Osto, M., Harrison, R. M., Coe, H., Williams, P. I., and Allan, J. D.: Real time chemical characterization of local and regional nitrate aerosols, Atmos. Chem. Phys., 9, 3709–3720, 2009.
de Gouw, J. A., Middlebrook, A. M., Warneke, C., Goldan, P. D., Kuster, W. C., Roberts, J. M., Fehsenfeld, F. C., Worsnop, D. R., Canagaratna, M. R., Pszenny, A. A. P., Keene, W. C., Marchewka, M., Bertman, S. B., and Bates, T. S.: Budget of organic carbon in a polluted atmosphere: Results from the new england air quality study in 2002, J. Geophys. Res.-Atmos., 110, D16305, doi:10.1029/2004JD005623, 2005.
DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T., Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop, D. R., and Jimenez, J. L.: Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer, Anal. Chem., 78, 8281–8289, 2006.
Department for environment food and rural affairs (defra): The air quality strategy for england, scotland, wales and northern Ireland, http://www.defra.gov.uk/environment/airquality/strategy/pdf/air-qualitystrategy-vol1.pdf, last access: August~2009, \mboxvolume~1, cm~7169~nia~61/06-07, 2007.
Dinar, E., Mentel, T. F., and Rudich, Y.: The density of humic acids and humic like substances (HULIS) from fresh and aged wood burning and pollution aerosol particles, Atmos. Chem. Phys., 6, 5213–5224, 2006.
Dockery, D. W., Pope, C. A., Xu, X. P., Spengler, J. D., Ware, J. H., Fay, M. E., Ferris, B. G., and Speizer, F. E.: An association between air-pollution and mortality in 6~United States cities, New Engl. J. Med., 329, 1753–1759, 1993.
Drewnick, F., Hings, S. S., DeCarlo, P., Jayne, J. T., Gonin, M., Fuhrer, K., Weimer, S., Jimenez, J. L., Demerjian, K. L., Borrmann, S., and Worsnop, D. R.: A new time-of-flight aerosol mass spectrometer (tof-ams)-instrument description and first field deployment, Aerosol Sci. Tech., 39, 637–658, 2005.
Drewnick, F., Hings, S. S., Alfarra, M. R., Prevot, A. S. H., and Borrmann, S.: Aerosol quantification with the aerodyne aerosol mass spectrometer: Detection limits and ionizer background effects, Atmos. Meas. Tech., 2, 33–46, 2009.
Eatough, D. J., Grover, B. D., Woolwine, W. R., Eatough, N. L., Long, R., and Farber, R.: Source apportionment of 1 h semi-continuous data during the 2005 study of organic aerosols in riverside (soar) using positive matrix factorization, Atmos. Environ., 42, 2706–2719, doi:10.1016/j.atmosenv.2007.07.038, 2008.
European Union: Directive 2008/50/ec of the european parliament and of the council of 21~May~2008 on ambient air quality and cleaner air for europe, Official Journal of the European Union, L152, 2008.
Fehsenfeld, F., Calvert, J., Fall, R., Goldan, P., Guenther, A. B., Hewitt, C. N., Lamb, B., Liu, S., Trainer, M., Westberg, H., and Zimmerman, P.: Emissions of volatile organic compounds from vegetation and the implications for atmospheric chemistry, Global Biogeochem. Cy., 6, 389–430, 1992.
Fenger, J.: Urban air quality, Atmos. Environ., 33, 4877–4900, 1999.
Fuller, K. A., Malm, W. C., and Kreidenweis, S. M.: Effects of mixing on extinction by carbonaceous particles, J. Geophys. Res.-Atmos., 104, 15941–15954, 1999.
Grieshop, A. P., Donahue, N. M., and Robinson, A. L.: Is the gas-particle partitioning in alpha-pinene secondary organic aerosol reversible?, Geophys. Res. Lett., 34, L14810, doi:10.1029/2007gl029987, 2007.
Hamilton, J. F., Webb, P. J., Lewis, A. C., Hopkins, J. R., Smith, S., and Davy, P.: Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS, Atmos. Chem. Phys., 4, 1279–1290, 2004.
Harrison, R M., Nemitz, E., Dall'Osto, M., et al.: Atmospheric Chemistry and Physics in the Atmosphere of a Developed Megacity (London): An Overview of the REPARTEE Experiment and its Conclusions, in preparation, 2010.
Helfter, C., Famulari, D., Phillips, G. J., Barlow, J. F., Grimmond, S., Wood, C., and Nemitz, E.: Long-term flux measurements of CO<sub>2</sub> above central london, Atmos. Chem. Phys. Discuss., in preparation, 2010.
Huffman, J. A., Docherty, K. S., Aiken, A. C., Cubison, M. J., Ulbrich, I. M., DeCarlo, P. F., Sueper, D., Jayne, J. T., Worsnop, D. R., Ziemann, P. J., and Jimenez, J. L.: Chemically-resolved aerosol volatility measurements from two megacity field studies, Atmos. Chem. Phys., 9, 7161–7182, 2009.
Huffman, J. A., Docherty, K. S., Mohr, C., Cubison, M. J., Ulbrich, I. M., Ziemann, P. J., Onasch, T. B., and Jimenez, J. L.: Chemically-resolved volatility measurements of organic aerosol from different sources, Environ. Sci. Technol., 43, 5351–5357, doi:10.1021/es803539d, 2009b.
Ibald-Mulli, A., Wichmann, H. E., Kreyling, W., and Peters, A.: Epidemiological evidence on health effects of ultrafine particles, J. Aerosol. Med., 15, 189–201, 2002.
Jacobson, M. C., Hansson, H. C., Noone, K. J., and Charlson, R. J.: Organic atmospheric aerosols: Review and state of the science, Rev. Geophys., 38, 267–294, 2000.
Jaeckels, J. M., Bae, M. S., and Schauer, J. J.: Positive matrix factorization (pmf) analysis of molecular marker measurements to quantify the sources of organic aerosols, Environ. Sci. Technol., 41, 5763–5769, doi:10.1021/Es062536b, 2007.
Jayne, J. T., Leard, D. C., Zhang, X. F., Davidovits, P., Smith, K. A., Kolb, C. E., and Worsnop, D. R.: Development of an aerosol mass spectrometer for size and composition analysis of submicron particles, Aerosol Sci. Tech., 33, 49–70, 2000.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of organic aerosols in the atmosphere, Science, 326, 1525–1529, doi:10.1126/science.1180353, 2009.
Jordan, T. B., Seen, A. J., and Jacobsen, G. E.: Levoglucosan as an atmospheric tracer for woodsmoke, Atmos. Environ., 40, 5316–5321, doi:10.1016/j.atmosenv.2006.03.023, 2006.
Katrib, Y., Martin, S. T., Hung, H.-M., Rudich, Y., Zhang, H., Slowik, J. G., Davidovits, P., Jayne, J. T., and Worsnop, D. R.: Products and mechanisms of ozone reactions with oleic acid for aerosol particles having core-shell morphologies, J. Phys. Chem A, 108, 6686–6695, 2004.
Khalil, M. A. K. and Rasmussen, R. A.: Tracers of wood smoke, Atmos. Environ., 37, 1211–1222, doi:10.1016/S1352-2310(02)01014-2, 2003.
Kleeman, M. J., Robert, M. A., Riddle, S. G., Fine, P. M., Hays, M. D., Schauer, J. J., and Hannigan, M. P.: Size distribution of trace organic species emitted from biomass combustion and meat charbroiling, Atmos. Environ., 42, 3059–3075, 2008.
Kreyling, W. G., Semmler-Behnke, M., and Moller, W.: Ultrafine particle-lung interactions: Does size matter?, J. Aerosol. Med., 19, 74–83, 2006.
Künzli, N., Kaiser, R., Medina, S., Studnicka, M., Chanel, O., Filliger, P., Herry, M., Horak, F., Puybonnieux-Texier, V., Quénel, P., Schneider, J., Seethaler, R., Vergnaud, J. C., and Sommer, H.: Public-health impact of outdoor and traffic-related air pollution: A european assessment, Lancet, 356, 795–801, 2000.
Lack, D. A., Cappa, C. D., Covert, D. S., Baynard, T., Massoli, P., Sierau, B., Bates, T. S., Quinn, P. K., Lovejoy, E. R., and Ravishankara, A. R.: Bias in filter-based aerosol light absorption measurements due to organic aerosol loading: Evidence from ambient measurements, Aerosol Sci. Tech., 42, 1033–1041, doi:10.1080/02786820802389277, 2008.
Lanz, V. A., Alfarra, M. R., Baltensperger, U., Buchmann, B., Hueglin, C., and Prévôt, A. S. H.: Source apportionment of submicron organic aerosols at an urban site by factor analytical modelling of aerosol mass spectra, Atmos. Chem. Phys., 7, 1503–1522, 2007.
Lanz, V. A., Alfarra, M. R., Baltensperger, U., Buchmann, B., Hueglin, C., Szidat, S., Wehrli, M. N., Wacker, L., Weimer, S., Caseiro, A., Puxbaum, H., and Prevot, A. S. H.: Source attribution of submicron organic aerosols during wintertime inversions by advanced factor analysis of aerosol mass spectra, Environ. Sci. Technol., 42, 214–220, doi:10.1021/Es0707207, 2008.
Longley, I. D., Gallagher, M. W., Dorsey, J. R., Flynn, M., Bower, K. N., and Allan, J. D.: Street canyon aerosol pollutant transport measurements, Sci. Total Environ., 334, 327–336, 2004.
Matthew, B. M., Middlebrook, A. M., and Onasch, T. B.: Collection efficiencies in an aerodyne aerosol mass spectrometer as a function of particle phase for laboratory generated aerosols, Aerosol Sci. Tech., 42, 884–898, 2008.
Mauderly, J. L. and Chow, J. C.: Health effects of organic aerosols, Inhal. Toxicol., 20, 257–288, doi:10.1080/08958370701866008, 2008.
Maudgalya, T., Genaidy, A., Weckman, G., Shell, R., Karwowski, W., and Wallace, S.: A critical appraisal of epidemiological studies investigating the effects of ultrafine particles on human health, Hum. Factor. Ergon. Man., 18, 358–373, doi:10.1002/Hfm.20115, 2008.
McFiggans, G., Alfarra, M. R., Allan, J., Bower, K., Coe, H., Cubison, M., Topping, D., Williams, P., Decesari, S., Facchini, C., and Fuzzi, S.: Simplification of the representation of the organic component of atmospheric particulates, Faraday Discuss., 130, 341–362, 2005.
Mohr, C., Huffman, J. A., Cubison, M. J., Aiken, A. C., Docherty, K. S., Kimmel, J. R., Ulbrich, I. M., Hannigan, M., and Jimenez, J. L.: Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations, Environ. Sci. Technol., 43, 2443–2449, doi:10.1021/es8011518, 2009.
Morino, Y., Kondo, Y., Takegawa, N., Miyazaki, Y., Kita, K., Komazaki, Y., Fukuda, M., Miyakawa, T., Moteki, N., and Worsnop, D. R.: Partitioning of HNO<sub>3</sub> and particulate nitrate over tokyo: Effect of vertical mixing, J. Geophys. Res.-Atmos., 111, D15215, doi:10.1029/2005jd006887, 2006.
National atmospheric emissions inventory (naei): http://www.naei.org.uk/, last access: 4~August, 2009.
Nemitz, E., Phillips, G. J., DiMarco, C. F., Allan, J. D., Barlow, J. F., Coe, H., Dall'Osto, M., Harrison, R. M., and Williams, P. I.: Controls of concentrations, gradients and fluxes of inorganic reactive gases and aerosol components above london, Atmos. Chem. Phys. Discuss., in preparation, 2010.
Paatero, P.: Least squares formulation of robust non-negative factor analysis, Chemometr. Intell. Lab., 37, 23–35, 1997.
Paatero, P.: The multilinear engine – a table-driven, least squares program for solving multilinear problems, including the n-way parallel factor analysis model, J. Comput. Graph. Stat., 8, 854–888, 1999.
Paatero, P., Hopke, P. K., Song, X. H., and Ramadan, Z.: Understanding and controlling rotations in factor analytic models, Chemometr. Intell. Lab., 60, 253–264, 2002.
Paatero, P., Hopke, P. K., Hoppenstock, J., and Eberly, S. I.: Advanced factor analysis of spatial distributions of PM$_2.5$ in the eastern united states, Environ. Sci. Technol., 37, 2460–2476, doi:10.1021/Es0261978, 2003.
Petzold, A., Schloesser, H., Sheridan, P. J., Arnott, W. P., Ogren, J. A., and Virkkula, A.: Evaluation of multiangle absorption photometry for measuring aerosol light absorption, Aerosol Sci. Tech., 39, 40–51, doi:10.1080/027868290901945, 2005.
Phillips, G. J., Thomas, R., Famulari, D., Williams, P. I., Crosier, J., Allan, J. D., Coe, H., Gallagher, M., Flynn, M., and Nemitz, E.: Fluxes of submicron aerosol components above three UK cities, Atmos. Chem. Phys. Discuss., in preparation, 2010.
Pio, C. A., Legrand, M., Oliveira, T., Afonso, J., Santos, C., Caseiro, A., Fialho, P., Barata, F., Puxbaum, H., Sanchez-Ochoa, A., Kasper-Giebl, A., Gelencser, A., Preunkert, S., and Schock, M.: Climatology of aerosol composition (organic versus inorganic) at nonurban sites on a west-east transect across europe, J. Geophys. Res.-Atmos., 112, D23s02, doi:10.1029/2006jd008038, 2007.
Polson, D., Fowler, D., Nemitz, E., Skiba, U., McDonald, A., Famulari, D., DiMarco, C. F., Simmons, I., Weston, K., Purvis, R. M., Coe, H., Manning, A. J., and Webster, H.: Boundary-layer-budget measurements of greenhouse gas emissions at the country scale, Q. J. Roy. Meteor. Soc., in press, 2010.
Pope, C. A. and Dockery, D. W.: Health effects of fine particulate air pollution: Lines that connect, J. Air Waste Manage., 56, 709–742, 2006.
Robinson, A. L., Subramanian, R., Donahue, N. M., Bernardo-Bricker, A., and Rogge, W. F.: Source apportionment of molecular markers and organic aerosol, 3 Food cooking emissions, Environ. Sci. Technol., 40, 7820–7827, doi:10.1021/Es060781p, 2006.
Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage, A. M., Grieshop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N.: Rethinking organic aerosols: Semivolatile emissions and photochemical aging, Science, 315, 1259–1262, doi:10.1126/science.1133061, 2007.
Saxena, P. and Hildemann, L. M.: Water-soluble organics in atmospheric particles: A critical review of the literature and application of thermodynamics to identify candidate compounds, J. Atmos. Chem., 24, 57–109, 1996.
Schauer, J. J., Kleeman, M. J., Cass, G. R., and Simoneit, B. R. T.: Measurement of emissions from air pollution sources, 1 C1 through C29 organic compounds from meat charbroiling, Environ. Sci. Technol., 33, 1566-1577, 1999.
Schauer, J. J., Kleeman, M. J., Cass, G. R., and Simoneit, B. R. T.: Measurement of emissions from air pollution sources, 4 C-1–C-27 organic compounds from cooking with seed oils, Environ. Sci. Technol., 36, 567–575, doi:10.1021/es002053m, 2002.
Schneider, J., Hock, N., Weimer, S., and Borrmann, S.: Nucleation particles in diesel exhaust: Composition inferred from in situ mass spectrometric analysis, Environ. Sci. Technol., 39, 6153–6161, 2005.
Schneider, J., Weimer, S., Drewnick, F., Borrmann, S., Helas, G., Gwaze, P., Schmid, O., Andreae, M. O., and Kirchner, U.: Mass spectrometric analysis and aerodynamic properties of various types of combustion-related aerosol particles, Int. J. Mass Spectrom., 258, 37–49, doi:10.1016/j.ijms.2006.07.008, 2006.
Schneider, J., Kirchner, U., Borrmann, S., Vogt, R., and Scheer, V.: In situ measurements of particle number concentration, chemically resolved size distributions and black carbon content of traffic-related emissions on german motorways, rural roads and in city traffic, Atmos. Environ., 42, 4257–4268, 2008.
Shiraiwa, M., Kondo, Y., Moteki, N., Takegawa, N., Miyazaki, Y., and Blake, D. R.: Evolution of mixing state of black carbon in polluted air from Tokyo, Geophys. Res. Lett., 34, L16803, doi:10.1029/2007gl029819, 2007.
Siegmann, K. and Sattler, K.: Aerosol from hot cooking oil, a possible health hazard, J. Aerosol. Sci., 27, S493–S494, 1996.
Simon, H., Allen, D. T., and Wittig, A. E.: Fine particulate matter emissions inventories: Comparison's of emissions estimates with observations from recent field programs, J. Air Waste Manage., 58, 320–343, doi:10.3155/1047-3289.58.2.320, 2008.
Simoneit, B. R. T.: Biomass burning – a review of organic tracers for smoke from incomplete combustion, Appl. Geochem., 17, 129–162, 2002.
Slowik, J. G., Cross, E. S., Han, J. H., Davidovits, P., Onasch, T. B., Jayne, J. T., Williams, L. R., Canagaratna, M. R., Worsnop, D. R., Chakrabarty, R. K., Moosmuller, H., Arnott, W. P., Schwarz, J. P., Gao, R. S., Fahey, D. W., Kok, G. L., and Petzold, A.: An inter-comparison of instruments measuring black carbon content of soot particles, Aerosol Sci. Technol., 41, 295–314, 2007.
Smoke control areas: http://www.uksmokecontrolareas.co.uk/, last access: 6~April, 2009.
Takegawa, N., Miyazaki, Y., Kondo, Y., Komazaki, Y., Miyakawa, T., Jimenez, J. L., Jayne, J. T., Worsnop, D. R., Allan, J. D., and Weber, R. J.: Characterization of an aerodyne aerosol mass spectrometer (ams): Intercomparison with other aerosol instruments, Aerosol Sci. Tech., 39, 760–770, 2005.
Turpin, B. J. and Lim, H. J.: Species contributions to pm2.5 mass concentrations: Revisiting common assumptions for estimating organic mass, Aerosol Sci. Tech., 35, 602–610, 2001.
Ulbrich, I. M., Canagaratna, M. R., Zhang, Q., Worsnop, D. R., and Jimenez, J. L.: Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data, Atmos. Chem. Phys., 9, 2891–2918, 2009.
US environmental protection agency technology transfer network clearinghouse for inventories and emissions factors (chief): http://www.epa.gov/ttn/chief/index.html, last access: 4~August, 2009.
Weimer, S., Alfarra, M. R., Schreiber, D., Mohr, M., Prevot, A. S. H., and Baltensperger, U.: Organic aerosol mass spectral signatures from wood-burning emissions: Influence of burning conditions and wood type, J. Geophys. Res.-Atmos., 113, D10304, doi:10.1029/2007jd009309, 2008.
Williams, B. J., Goldstein, A. H., Kreisberg, N. M., and Hering, S. V.: An in-situ instrument for speciated organic composition of atmospheric aerosols: Thermal desorption aerosol gc/ms-fid~(tag), Aerosol Sci. Tech., 40, 627–638, 2006.
Wroth, C. and Wiles, A.: Population and vital statistics by area of usual residence in the United Kingdom, 2007, Office for National Statistics, Newport, UK, series vs~no~34, ppi~no~30, 2009.
Yeung, L. L. and To, W. M.: Size distributions of the aerosols emitted from commercial cooking processes, Indoor Built Environ., 17, 220–229, doi:10.1177/1420326x08092043, 2008.
Zahardis, J. and Petrucci, G. A.: The oleic acid-ozone heterogeneous reaction system: products, kinetics, secondary chemistry, and atmospheric implications of a model system - a review, \mboxAtmos. Chem. Phys., 7, 1237–1274, 2007.
Zhang, Q., Alfarra, M. R., Worsnop, D. R., Allan, J. D., Coe, H., Canagaratna, M. R., and Jimenez, J. L.: Deconvolution and quantification of hydrocarbon-like and oxygenated organic aerosols based on aerosol mass spectrometry, Environ. Sci. Technol., 39, 4938–4952, 2005a.
Zhang, Q., Worsnop, D. R., Canagaratna, M. R., and Jimenez, J. L.: Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: insights into sources and processes of organic aerosols, Atmos. Chem. Phys., 5, 3289–3311, 2005.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J., Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys. Res. Lett., 34, L13801, doi:10.1029/2007GL029979, 2007.