References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-8-1855-2008

Hygroscopic growth and activation of HULIS particles: experimental data and a new iterative parameterization scheme for complex aerosol particles

Ziese

¹ Wex

¹ Nilsson

² Salma

³ Ocskay

³ Hennig

¹ Massling

¹ Stratmann

Leibniz-Institute for Tropospheric Research, Permoser Strasse 15, 04318 Leipzig, Germany

Lund University, Department of Nuclear Physic, P.O. Box 118, 221 00 Lund, Sweden

Eötvös University, Institute of Chemistry, P.O. Box 32, 1518 Budapest, Hungary

28 03 2008

8 6 1855 1866

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The hygroscopic growth and activation of two HULIS (HUmic LIke Substance) and one Aerosol-Water-Extract sample, prepared from urban-type aerosol, were investigated. All samples were extracted from filters, redissolved in water and atomized for the investigations presented here. The hygroscopic growth measurements were done using LACIS (Leipzig Aerosol Cloud Interaction Simulator) together with a HH-TDMA (High Humidity Tandem Differential Mobility Analyzer). Hygroscopic growth was determined for relative humidities (RHs) up to 99.75%. The critical diameters for activation were measured for supersaturations between 0.2 and 1%. All three samples showed a similar hygroscopic growth behavior, and the two HULIS samples also were similar in their activation behavior, while the Aerosol-Water-Extract turned out to be more CCN active than the HULIS samples. The experimental data was used to derive parameterizations for the hygroscopic growth and activation of HULIS particles. The concept of ρion (Wex et al., 2007a) and the Szyszkowski-equation (Szyszkowski, 1908; Facchini, 1999) were used for parameterizing the Raoult and the Kelvin (surface tension) terms of the Köhler equation, respectively. This concept proved to be very successful for the HULIS samples in the saturation range from RHs larger than 98% up to activation. It was also shown to work well with data on HULIS taken from literature. Here, different atmospheric life-times and/or different sources for the different samples showed up in different coefficients for the parameterization. However, the parameterization did not work out well for the Aerosol-Water-Extract.

References 1

Albrecht, B.: Aerosol, cloud microphysics, and fractional cloudiness, Science, 245, 1227–1230, 1989.

Asa-Awuku, A., Nenes, A., Sullivan, A., Hennigan, C., and Weber, R.: Investigation of molar volume and surfactant characteristics of water-soluble organic compounds in biomass burning aerosol, Atmos. Chem. Phys., 8, 799–812, 2008.

Bilde, M. and Svenningsson, B.: CCN activation of slightly soluble organics: The importance of small amounts of inorganic salts and particle phase, Tellus, 56(B), 128–134, 2004.

Broekhuizen, K., Kumar, P., and Abbatt, J.: Partly soluble organics as cloud condensation nuclei: Role of trace soluble and surface active species, Geophys. Res. Lett., 31, L01107, doi:10.1029/2003GL018203, 2004.

Dinar, E., Mentel, T., 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, 2006a.

Dinar, E., Taranuik, I., Graber, E., Katsman, S., Moise, T., Anttila, T., Mentel, T., and Rudich, Y.: Cloud Condensation Nuclei properties of model and atmospheric HULIS, Atmos. Chem. Phys., 6, 2465–2482, 2006b.

Dinar, E., Taraniuk, I., Graber, E., Anttila, T., Mentel, T., and Rudich, Y.: Hygroscopic growth of atmospheric and model humic-like substances, J. Geophys. Res., 112, D05211, doi:10.1029/2006JD007442, 2007.

Dinar, E., Riziq, A. A., Spindler, C., Erlick, C., Kiss, G., and Rudich, Y.: The comples refractive index of atmospheric and model humic-like substances (HULIS) retrieved by a cavity ring down aerosol spectrometer (CRD-AS), Faraday Discuss., 137, 279–295, doi:10.1039/b703111d, 2008.

Facchini, M., Mircea, M., Fuzzi, S., and Charlson, R.: Cloud albedo enhancement by surface-active organic solutes in growing droplets, Nature, 401, 257–259, 1999.

Graber, E. and Rudich, Y.: Atmospheric HULIS: How humic-like are they? A comprehensive and critical review, Atmos. Chem. Phys., 6, 729–753, 2006.

Gysel, M., Weingartner, E., Nyeki, S., Paulsen, D., Baltensperger, U., Galambos, I., and Kiss, G.: Hygroscopic properties of water-soluble matter and humic-like organics in atmospheric fine aerosol, Atmos. Chem. Phys., 4, 35–50, 2004.

Hennig, T., Massling, A., Brechtel, F., and Wiedensohler, A.: A tandem DMA for highly temperature-stabilized hygroscopic particle growth measurements between 90% ans 98% relative humidity, J. Aerosol Sci., 36, 1210–1223, 2005.

Henning, S., Rosenorn, T., D'Anna, B., Gola, A., Svenningsson, B., and Bilde, M.: Cloud droplet activation and surface tension of mixtures of slightly soluble organics and inorganic salt, Atmos. Chem. Phys., 5, 575–582, 2005.

Hoffer, A., Gelencser, A., Guyon, P., Kiss, G., Schnid, O., Frank, G., Artaxo, P., and Andreae, M.: Optical properties of humic-like substances (HULIS) in biomass-burning aerosols, Atmos. Chem. Phys., 6, 3563–3570, 2006.

Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G, and Wilson, J.: Organic aerosol and global climate modelling: A review, Atmos. Chem. Phys., 5, 1053-1123, 2005.

Kiselev, A., Wex, H., Stratmann, F., Nadeev, A., and Karpushenko, D.: White-light optical particle spectrometer for in-situ measurements of condensational growth of aerosol particles, Appl. Optics, 44, 4693–4701, 2005.

Kiss, G., Tombacz, E., and Hansson, H.-C.: Surface tension effects of humic-like substances in the aqueous extract of tropospheric fine aerosol, J. Atmos. Chem., 50, 279–294, 2005.

Köhler, H.: The nucleus in and the growth of hygroscopic droplets, T. Faraday Soc., 32, 1152–1161, 1936.

Lance, S., Medina, J., Smith, J., and Nenes, A.: Mapping the operation of the DMT continuous Flow CCN counter, Aerosol Sci. Technol., 40, 242–254, 2006.

McFiggans, G., Artaxo, P., Baltensperger, U., Coe, H., Facchini, M. C., Feingold, G., Fuzzi, S., Gysel, M., Laaksonen, A., Lohmann, U., Mentel, T. F., Murphy, D. M., O'Dowd, C. D., Snider, J. R., and Weingartner, E.: The effect of physical and chemical aerosol properties on warm cloud droplet activation, Atmos. Chem. Phys., 6, 2593–2649, 2006.

Rader, D. and McMurry, P.: Application of the tandem differential mobility analyser to studies of droplet growth or evaporation, J. Aerosol Sci., 17, 771–787, 1986.

Salma, I., Ocskay, R., Varga, I., and Maenhaut, W.: Surface tension of atmospheric humic-like substances in connection with relaxation, dilution, and solution pH, J. Geophys. Res., 111, D23205, doi:10.1029/2005JD007015, 2006.

Salma, I., Ocskay, R., Chi, X., and Maenhaut, W.: Sampling artefacts, concentration and chemical composition of fine water-soluble organic carbon and humic-like substances in a continental urban atmospheric environment, Atmos. Environ., 41, 4106–4118, 2007.

Samburova, V., Zenobi, R., and Kalberer, M.: Characterisation of high molecular weight compounds in urban atmospheric particles, Atmos. Chem. Phys., 5, 2163–2170, 2005.

Sjogren, S., Gysel, M., Weingartner, E., Baltensperger, U., Cubison, M. J., Coe, H., Zardini, A. A., Marcolli, C., Krieger,U. K. and Peter, T.: Hygroscopic growth and water uptake kinetics of two-phase aerosol particles consisting of ammonium sulfate, adipic acid and humic acid mixtures, J. Aerosol Sci., 38, 157–171, 2007.

Sorjamaa, R., Svenningsson, B., Raatikainen, T., Henning, S., Bilde, M., and Laaksonen, A.: The role of surfactants in Köhler theory reconsidered, Atmos. Chem. Phys., 4, 2107–2117, 2004.

Stratmann, F., Kiselev, A., Wurzler, S., Wendisch, M., Heintzenberg, J., Charlson, R., Diehl, K., Wex, H., and Schmidt, S.: Laboratory studies and numerical simulations of cloud droplet formation under realistic supersaturation conditions, J. Atmos. Ocean. Tech., 21, 876–887, 2004.

Szyszkowski, B.: Experimentelle Studien über kapillare Eigenschaften der wässrigen Lösungen von Fettsäuren, Z. Phys. Chem., 64, 385–414, 1908.

Tang, I.: Chemical and size effects of hygroscopic aerosols in light scattering coefficients, J. Geophys. Res., 101, 19 245–19 250, 1996.

Tang, I. and Munkelwitz, H.: Water activities, densities, and refractive indices of aqueous sulfate and sodium nitrate droplets of atmospheric importance, J. Geophys. Res., 99, 18 801–18 808, 1994.

Taraniuk, I., Graber, E. R., Kostinski, A., and Rudich, Y.: Surfactant properties of atmospheric and model humic-like substances (HULIS), Geophys. Res. Lett., 34, L16807, doi:10.1029/2007GL029576, 2007.

Twomey, S.: Pollution and the planetary albedo, Atmos. Environ., 8, 1251–1256, 1974.

Varga, B., Kiss, G., Ganszky, I., Gelencser, A., and Krivacsy, Z.: Isolation of water-soluble organic matter from atmospheric aerosol, Talanta, 55, 561–572, 2001.

Wex, H., Kiselev, A., Stratmann, F., Zoboki, J., and Brechtel, F.: Measured and modeled equilibrium sizes of NaCl and (NH4)2SO4 particles at relative humidities up to 99.1%, J. Geophys. Res., 110, D21212, doi:10.1029/2004JD005507, 2005.

Wex, H., Kiselev, A., Ziese, M., and Stratmann, F.: Calibration of LACIS as a CCN detector and its use in measuring activation and hygroscopic growth of atmospheric aerosol particles, Atmos. Chem. Phys., 6, 4519–4527, 2006.

Wex, H., Hennig, T., Salma, I., Ocskay, R., Kiselev, A., Henning, S., Massling, A., Wiedensohler, A., and Stratmann, F.: hygroscopic growth and measured and modeled critical supersaturations of an atmospheric HULIS sample, Geophys. Res. Lett., 34, L02818, doi:10.1029/2006GL028260, 2007a.

Wex, H., Ziese, M., Kiselev, A., Henning, S., and Stratmann, F.: Deliquescence and hygroscopic growth of succinic acid particles measured with LACIS, Geophys. Res. Lett., L17810, doi:10.1029/2007GL030185, 2007b.