Atmospheric Chemistry and Physics
www.atmos-chem-phys.net
1680-7316
1680-7324
6
9
2006
10.5194/acp-6-2513-2006
http://www.atmos-chem-phys.net/6/2513/2006/
http://www.atmos-chem-phys.net/6/2513/2006/acp-6-2513-2006.html
http://www.atmos-chem-phys.net/6/2513/2006/acp-6-2513-2006.pdf
2513
2524
2006-06-30
Closure between measured and modeled cloud condensation nuclei (CCN) using size-resolved aerosol compositions in downtown Toronto
K. Broekhuizen
kbroekhuizen@mail.colgate.edu
R.Y.-W. Chang
W. R. Leaitch
S.-M. Li
J. P. D. Abbatt
Department of Chemistry, University of Toronto, 80 St. George St., Toronto, ON M5S 3H6, Canada
Meteorological Service of Canada, 4905 Dufferin St., Toronto, ON M3H 5T4, Canada
Department of Chemistry, Colgate University, 13 Oak Dr., Hamilton, NY 13346, USA
Measurements of cloud condensation nuclei (CCN) were made in downtown
Toronto during August and September, 2003. CCN measurements were performed
at 0.58% supersaturation using a thermal-gradient diffusion chamber,
whereas the aerosol size distribution and composition were simultaneously
measured with a TSI SMPS and APS system and an Aerodyne Aerosol Mass
Spectrometer (AMS), respectively. Aerosol composition data shows that the
particles were predominately organic in nature, in particular for those with
a vacuum aerodynamic diameter of <0.25 µm. In this study, the largest
contribution to CCN concentrations came from this size range, suggesting
that the CCN are also organic-rich. Using the size and composition
information, detailed CCN closure analyses were performed. In the first
analysis, the particles were assumed to be internally mixed, the organic
fraction was assumed to be insoluble, and the inorganic fraction was assumed
to be ammonium sulfate. The AMS time-of-flight data were used for Köhler
theory predictions for each particle size and composition to obtain the dry
diameter required for activation. By so doing, this closure analysis yielded
an average value of CCN<sub>predicted</sub>/CCN<sub>observed</sub>=1.12±0.05.
However, several sample days showed distinct bimodal distributions, and a
closure analysis was performed after decoupling the two particle modes. This
analysis yielded an average value of CCN<sub>predicted</sub>/CCN<sub>observed</sub>=1.03±0.05.
A sensitivity analysis was also performed to determine the
aerosol/CCN closure if the organic solubility, droplet surface tension, or
chamber supersaturation were varied.
Abbatt, J. P. D., Broekhuizen, K., and Kumar, P. P.: Cloud condensation nucleus activity of internally mixed ammonium sulfate/organic acid aerosol particles, Atmos. Environ., 39, 4767–4778, 2005.
Albrecht, B.: Aerosols, cloud microphysics and fractional cloudiness, Science, 245, 1227–1230, 1989.
Alfarra, M. R., Coe, H., Allan, J. D., et al.: Characterization of urban and rural organic particulate in the Lower Fraser Valley using two Aerodyne Aerosol Mass Spectrometers, Atmos. Environ., 38, 5745–5758, 2004.
Allan, J. D., Alfarra, M. R., Bower, K. N., et al.: Quantitative sampling using an Aerodyne aerosol mass spectrometer – 2. Measurements of fine particulate chemical composition in two U.K. cities, J. Geophys. Res.-Atmos., 108, 4091, doi:10.1029/2002JD002359, 2003.
Bigg, E. K.: Discrepancy between observation and prediction of concentrations of cloud condensation nuclei, Atmos. Res., 20, 82–86, 1986.
Bilde, M. and Svenningsson, B.: CCN activation of slightly soluble organics: Importance of small amounts of inorganic salt and particle phase, Tellus, Ser. B, 56, 128–134, 2004.
Broekhuizen, K., Kumar, P. P., and Abbatt, J. P. D.: Partially soluble organics as cloud condensation nuclei: Role of trace soluble and surface active species, Geophys. Res. Lett., 31, L01107, doi:10.1029/2003GL018203, 2004a.
Broekhuizen, K., Thornberry, T., Kumar, P. P., and Abbatt, J. P. D.: Formation of cloud condensation nuclei by oxidative processing: Unsaturated fatty acids, J. Geophys. Res.-Atmos., 109, D24206, doi:10.1029/2004JD005298, 2004b.
Cantrell, W., Shaw, G., Cass, G. R., Chowdhury, Z., Hughes, L. S., Prather, K. A., Guazzotti, S. A., and Coffee, K. R.: Closure between aerosol particles and cloud condensation nuclei at Kaashidhoo Climate Observatory, J. Geophys. Res., 106, 28 711–28 718, 2001.
Chuang, P. Y., Collins, D. R., Pawlowska, H., Snider, J. R., Jonsson, H. H., Brenguier, J.-L., Flagan, R. C., and Seinfeld, J. H.: CCN measurements during ACE-2 and their relationship to cloud microphysical properties, Tellus, Ser. B, 52, 843–867, 2000.
Chung, C. E. and Ramanathan, V.: Aerosol loading over the Indian Ocean and its possible impact on regional climate, Indian J. Mar. Sci., 33, 40–55, 2004.
Corrigan, C. E. and Novakov, T.: Cloud condensation nucleus activity of organic compounds: a laboratory study, Atmos. Environ., 33, 2661–2668, 1999.
Covert, D. S., Gras, J. L., Wiedensohler, A., and Stratmann, F.: Comparison of directly measured CCN with CCN modeled from the number-size distribution in the marine boundary layer during ACE 1 at Cape Grim, Tasmania, J. Geophys. Res., 103, 16 597–16 608, 1998.
Cruz, C. N. and Pandis, S. N.: A study of the ability of pure secondary organic aerosol to act as cloud condensation nuclei, Atmos. Environ., 31, 2205–2214, 1997.
Durkee, P. A., Noone, K. J., Bluth, R. T., et al.: The impact of ship-produced aerosols on the microstructure and albedo of warm marine stratocumulus clouds: A test of MAST hypotheses 1i and 1ii, J. Atmos. Sci., 57, 2554–2569, 2000.
Dusek, U., Covert, D. S., Wiedensohler, A., Neususs, C., Weise, D., and Cantrell, W.: Cloud condensation nuclei spectra derived from size distributions and hygroscopic properties of the aerosol in coastal south-west Portugal during ACE-2, Tellus, Ser. B, 55, 35–53, 2003.
Facchini, M. C., Mircea, M., Fuzzi, S., and Charlson, R. J.: Cloud albedo enhancement by surface-active organic solutes in growing droplets, Nature, 401, 257–259, 1999.
Gerber, H. E., Hoppel, W. A., and Wojciechowski, T. A.: Experimental verification of the theoretical relationship between size and critical supersaturation of salt nuclei, J. Atmos. Sci., 34, 1836–1841, 1977.
Giebl, H., Berner, A., Reischl, G., Puxbaum, H., Kasper-Giebl, A., and Hitzenberger, R.: CCN activation of oxalic acid and malonic acid test aerosols with the University of Vienna cloud condensation nuclei counter, J. Aerosol Sci., 33, 1623–1634, 2002.
Givati, A. and Rosenfeld, D.: Quantifying precipitation suppression due to air pollution, J. Appl. Meteorol., 43, 1038–1056, 2004.
Hegg, D. A., Radke, L. F., and Hobbs, P. V.: Measurements of Aitken nuclei and cloud condensation nuclei in the marine atmosphere and their relation to the DMS-cloud-climate hypothesis, J. Geophys. Res., 96, 18 727–18 733, 1991.
Hegg, D. A., Ferek, R. J., and Hobbs, P. V.: Cloud condensation nuclei over the Arctic Ocean in early spring, J. Appl. Meteorol., 34, 2076–2082, 1995.
Hitzenberger, R., Berner, A., Giebl, H., Kromp, R., Larson, S. M., Rouc, A., Koch, A., Marischka, S., and Puxbaum, H.: Contribution of carbonaceous material to cloud condensation nuclei concentrations in European background (Mt. Sonnblick) and urban (Vienna) aerosols, Atmos. Environ., 33, 2647–2659, 1999.
Hudson, J. G.: Cloud condensation nuclei near marine cumulus, J. Geophys. Res., 98, 2693–2702, 1993.
Hudson, J. G. and Frisbie, P. R.: Surface cloud condensation nuclei and condensation nuclei measurements at Reno, Nevada, Atmos. Environ., Part A, 25, 2285–2299, 1991.
Jayne, J. T., Leard, D. C., Zhang, Z. F., Davidovits, P., Smith, K. A., Kolb, C. E., and Worsnop, D. R.: Development of an aerosol mass spectrometer for size and chemical composition analysis of submicron particles, Aerosol Sci. Tech., 33, 49–70, 2000.
Jimenez J. L., Jayne, J. T., Shi, Q., et al.: Ambient aerosol sampling using the aerodyne aerosol mass spectrometer, J. Geophys. Res.-Atmos., 108, 8425, doi:10.1029/2001JD001213, 2003.
Katz, U. and Kocmond, W. C.: An investigation of the size-supersaturation relationship of soluble condensation nuclei, J. Atmos. Sci., 30, 160–165, 1973.
Kumar, P. P., Broekhuizen, K., and Abbatt, J. P. D.: Organic acids as cloud condensation nuclei: Laboratory studies of highly soluble and insoluble species, Atmos. Chem. Phys., 3, 509–520, 2003.
Laaksonen, A., Korhonen, P., Kulmala, M., and Charlson, R. J.: Modification of the Köhler equation to include soluble trace gases and slightly soluble substances, J. Atmos. Sci., 55, 853–862, 1998.
Liu, P. S. K., Leaitch, W. R., Banic, C. M., Li, S.-M., Ngo, D., and Megaw, W. J.: Aerosol observations at Chebogue Point during the 1993 North Atlantic Regional Experiment: Relationships among cloud condensation nuclei, size distribution, and chemistry, J. Geophys. Res., 101, 28 971–28 990, 1996.
Martin, G. M., Johnson, D. W., and Spice, A.: The measurement and parameterization of effective radius of droplets in warm stratocumulus clouds, J. Atmos. Sci., 51, 1823–1842, 1994.
Mircea, M. , Facchini, M. C., Decesari, S., Cavalli, F., Emblico, L., Fuzzi, S., Vestin, A., Rissler, J., Swietlicki, E., Frank, G., Andreae, M. O., Maenhaut, W., Rudich, Y., and Artaxo, P.: Importance of the organic aerosol fraction for modeling aerosol hygroscopic growth and activation: a case study in the Amazon Basin, Atmos. Chem. Phys., 5, 3111–3126, 2005.
Murphy, D. M., Thomson, D. S., and Mahoney, M. J.: In-situ measurements of organics, meteoritic material, mercury and other elements in aerosols at 5 and 19 kilometers, Science, 282, 1664–1669, 1998.
Quinn, P. K., Covert, D. S., Bates, T. S., Kapustin, V. N., Ramsey-Bell, D. C., and McInnes, L. M.: Dimethylsulfide/cloud condensation nuclei/climate system: relevant size-resolved measurements of the chemical and physical properties of atmospheric aerosol particles, J. Geophys. Res., 98, 10 411–10 427, 1993.
Raymond, T. M. and Pandis S. N.: Cloud activation of single-component organic aerosol particles, J. Geophys. Res., 107, 4787, doi:10.1029/2002JD002159, 2002.
Raymond, T. M. and Pandis, S. N.: Formation of cloud droplets by multicomponent organic particles, J. Geophys. Res., 108, 4469, doi:10.1029/2003JD003503, 2003.
Rissler, J. , Swietlicki, E., Zhou, J., Roberts, G., Andreae, M. O., Gatti, L. V. and Artaxo, P.: Physical properties of the sub-micrometer aerosol over the Amazon rain forest during the wet-to-dry season transition – comparison of modeled and measured CCN concentrations, Atmos. Chem. Phys., 4, 2119–2143, 2004.
Rissman, T. A., VanReken, T. M., Wang, J., Gasparini, R., Collins, D. R., Jonsson, H. H., Brechtel, F. J., Flagan, R. C., and Seinfeld, J. H.: Characterization of ambient aerosol from measurements of cloud condensation nuclei (CCN) during the 2003 Atmospheric Radiation Measurement (ARM) Aerosol Intensive Observational Period (IOP) at the Southern Great Plains (SGP) Site in Oklahoma, J. Geophys. Res.-Atmos., 111, D05S11, doi:10.1029/2004JD005695, 2006.
Roberts, G. C., Artaxo, P., Zhou, J., Swietlicki, E., and Andreae, M. O.: Sensitivity of CCN spectra on chemical and physical properties of aerosol: A case study from the Amazon Basin, J. Geophys. Res., 107, 8070, doi:10.1029/2001JD00583, 2002.
Rosenfeld, D.: TRMM observed first direct evidence of smoke from forest fires inhibiting rainfall, Geophys. Res. Lett., 26, 3105–3108, 1999.
Rosenfeld, D.: Suppression of rain and snow by urban and industrial air pollution, Science, 287, 1793–1796, 2000.
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.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, John Wiley & Sons, Inc., New York City, NY, pp 792, 1998.
Shulman, M. L., Jacobson, M. C., Carlson, R. J., Synovec, R. E., and Young, T. E.: Dissolution behavior and surface tension effects of organic compounds in nucleating cloud droplets, Geophys. Res. Lett., 23, 277–280, 1996.
Snider, J. R. and Brenguier, J.-L.: Cloud condensation nuclei and cloud droplet measurements during ACE-2, Tellus, Ser. B, 52, 828–842, 2000.
Snider, J. R., Guibert, S., Brenguier, J.-L., and Putaud, J.-P.: Aerosol activation in marine stratocumulus clouds: 2. Köhler and parcel theory closure studies, J. Geophys. Res., 108, 8629, doi:10.1029/2002JD002692, 2003.
Tan, P. V., Evans, G. J., Tsai, J., Owega, S., Fila, M., Malpica, O., and Brook, J. R.: On-line analysis of urban particulate matter focusing on elevated wintertime aerosol concentrations, Environ. Sci. Tech. 36, 3512–3518, 2002.
Twomey, S.: Influence of pollution on the short-wave albedo of clouds, J. Atmos. Sci., 34, 1149–1152, 1977.
VanReken, T. M., Rissman, T. A., Roberts, G. C., Varutbangkul, V., Jonsson, H. H., Flagan, R. C., and Seinfeld, J.H.: Toward aerosol/cloud condensation nuclei (CCN) closure during CRYSTAL-FACE, J. Geophys. Res., 108, 4633, doi:10.1029/2003JD003582, 2003.
VanReken, T. M., Ng, N. L., Flagan, R. C., and Seinfeld, J. H.: Cloud condensation nucleus activation properties of biogenic secondary organic aerosol, J. Geophys. Res.-Atmos., 110, D07206, doi:10.1029/2004JD005465, 2005.
Volckens, J., and Peters, T. M.: Counting and particle transmission efficiency of the aerodynamic particle sizer, J. Aerosol Sci., 36, 1400–1408, 2005.
Wood, R., Johnson, D., Osborne, S., et al.: Boundary layer and aerosol evolution during the 3rd Lagrangian experiment of ACE-2, Tellus Ser. B, 52, 401–422, 2000.
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. Tech., 39, 4938–4952, doi:10.1021/es048568l, 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, 2005b.
Zhang, X., Smith, K. A., Worsnop, D. R., Jimenez, J. L., Jayne, J. T., Kolb, C. E., Morris, J., and Davidovits, P.: Numerical characterization of particle beam collimation: Part II Integrated aerodynamic-lens-nozzle system, Aerosol Sci. Tech., 38, 619–638, 2004.
Zhou, J., Swietlicki, E., Berg, O. H., Aalto, P. P., Hämeri, K., Nilsson, E. D., and Leck, C.: Hygroscopic properties of aerosol particles over the central Arctic Ocean during summer, J. Geophys. Res., 106, 32 111–32 123, 2001.