References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-7489-2010

Hygroscopicity distribution concept for measurement data analysis and modeling of aerosol particle mixing state with regard to hygroscopic growth and CCN activation

¹ Rose

¹ Cheng

Y. F.

² Gunthe

S. S.

¹ Massling

² Stock

² Wiedensohler

² Andreae

M. O.

¹ Pöschl

Max Planck Institute for Chemistry, 55020 Mainz, Germany

Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany

12 08 2010

10 15 7489 7503

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.

This article is available from http://www.atmos-chem-phys.net/10/7489/2010/acp-10-7489-2010.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/7489/2010/acp-10-7489-2010.pdf

This paper presents a general concept and mathematical framework of particle hygroscopicity distribution for the analysis and modeling of aerosol hygroscopic growth and cloud condensation nucleus (CCN) activity. The cumulative distribution function of particle hygroscopicity, H(κ, Dd) is defined as the number fraction of particles with a given dry diameter, Dd, and with an effective hygroscopicity parameter smaller than the parameter κ. From hygroscopicity tandem differential mobility analyzer (HTDMA) and size-resolved CCN measurement data, H(κ, Dd) can be derived by solving the κ-Köhler model equation. Alternatively, H(κ, Dd) can be predicted from measurement or model data resolving the chemical composition of single particles. A range of model scenarios are used to explain and illustrate the concept, and exemplary practical applications are shown with HTDMA and CCN measurement data from polluted megacity and pristine rainforest air. Lognormal distribution functions are found to be suitable for approximately describing the hygroscopicity distributions of the investigated atmospheric aerosol samples. For detailed characterization of aerosol hygroscopicity distributions, including externally mixed particles of low hygroscopicity such as freshly emitted soot, we suggest that size-resolved CCN measurements with a wide range and high resolution of water vapor supersaturation and dry particle diameter should be combined with comprehensive HTDMA measurements and size-resolved or single-particle measurements of aerosol chemical composition, including refractory components. In field and laboratory experiments, hygroscopicity distribution data from HTDMA and CCN measurements can complement mixing state information from optical, chemical and volatility-based techniques. Moreover, we propose and intend to use hygroscopicity distribution functions in model studies investigating the influence of aerosol mixing state on the formation of cloud droplets.

References 1

Aitchison,~J. and Brown,~J A C.: The lognormal distribution function, Cambridge Univ. Press, Cambridge, UK, 1957.

Andreae,~M O. and Rosenfeld,~D.: Aerosol-cloud-precipitation interactions. Part 1. The nature and sources of cloud-active aerosols, Earth-Sci. Rev., 89, 13–41, 2008.

Buzorius,~G., Zelenyuk,~A., Brechtel,~F., and Imre,~D.: Simultaneous determination of individual ambient particle size, hygroscopicity and composition, Geophys. Res. Lett., 29(20), 1974, \doi10.1029/2001gl014221, 2002.

Cheng,~Y F., Berghof,~M., Garland,~R M., Wiedensohler,~A., Wehner,~B., Müller,~T., Su,~H., Zhang,~Y H., Achtert,~P., Nowak,~A., Pöschl,~U., Zhu,~T., Hu,~M., and Zeng,~L M.: Influence of soot mixing state on aerosol light absorption and single scattering albedo during air mass aging at a~polluted regional site in northeastern china,~J. Geophys. Res., 114, D00G10, \doi10.1029/2008jd010883, 2009.

Clegg, S. L., Kleeman, M. J., Griffin, R. J., and Seinfeld, J. H.: Effects of uncertainties in the thermodynamic properties of aerosol components in an air quality model – Part 1: Treatment of inorganic electrolytes and organic compounds in the condensed phase, Atmos. Chem. Phys., 8, 1057–1085, doi:10.5194/acp-8-1057-2008, 2008.

Deirmendjian,~D.: Electromagnetic scattering on spherical polydisersions, Elsevier, New York, 1967.

Dusek,~U., Frank,~G P., Hildebrandt,~L., Curtius,~J., Schneider,~J., Walter,~S., Chand,~D., Drewnick,~F., Hings,~S., Jung,~D., Borrmann,~S., and Andreae,~M O.: Size matters more than chemistry for cloud-nucleating ability of aerosol particles, Science, 312, 1375–1378, \doi10.1126/science.1125261, 2006.

Frank, G. P., Dusek, U., and Andreae, M. O.: Technical note: A method for measuring size-resolved CCN in the atmosphere, Atmos. Chem. Phys. Discuss., 6, 4879–4895, doi:10.5194/acpd-6-4879-2006, 2006.

Garland, R. M., Yang, H., Schmid, O., Rose, D., Nowak, A., Achtert, P., Wiedensohler, A., Takegawa, N., Kita, K., Miyazaki, Y., Kondo, Y., Hu, M., Shao, M., Zeng, L. M., Zhang, Y. H., Andreae, M. O., and Pöschl, U.: Aerosol optical properties in a rural environment near the mega-city Guangzhou, China: implications for regional air pollution, radiative forcing and remote sensing, Atmos. Chem. Phys., 8, 5161–5186, doi:10.5194/acp-8-5161-2008, 2008.

Garland,~R M., Schmid,~O., Nowak,~A., Achtert,~P., Wiedensohler,~A., Gunthe,~S S., Takegawa,~N., Kita,~K., Kondo,~Y., Hu,~M., Shao,~M., Zeng,~L M., Zhu,~T., Andreae,~M O., and Pöschl,~U.: Aerosol optical properties observed during campaign of air quality research in Beijing 2006 (CAREbeijing-2006): characteristic differences between the inflow and outflow of Beijing city air, J. Geophys. Res., 114, D00G04, \doi10.1029/2008jd010780, 2009.

Gunthe, S. S., King, S. M., Rose, D., Chen, Q., Roldin, P., Farmer, D. K., Jimenez, J. L., Artaxo, P., Andreae, M. O., Martin, S. T., and Pöschl, U.: Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity, Atmos. Chem. Phys., 9, 7551–7575, doi:10.5194/acp-9-7551-2009, 2009.

Kammermann, L., Gysel, M., Weingartner, E., Herich, H., Cziczo, D. J., Holst, T., Svenningsson, B., Arneth, A., and Baltensperger, U.: Subarctic atmospheric aerosol composition: 3. Measured and modeled properties of cloud condensation nuclei, J. Geophys. Res., 115, D04202, doi:10.1029/2009JD012447, 2010.

Kreidenweis, S. M., Petters, M. D., and Chuang, P. Y.: Cloud particle precursors, in: Clouds in the perturbed climate system – their relationship to energy balance, atmospheric dynamics, and precipitation, edited by: Heintzenberg, J. and Charlson, R. J., MIT Press, Cambridge, 291–317, 2009.

Krejci, R., Ström, J., de Reus, M., and Sahle, W.: Single particle analysis of the accumulation mode aerosol over the northeast Amazonian tropical rain forest, Surinam, South America, Atmos. Chem. Phys., 5, 3331–3344, doi:10.5194/acp-5-3331-2005, 2005.

Kuwata, M. and Kondo, Y.: Dependence of size-resolved CCN spectra on the mixing state of nonvolatile cores observed in Tokyo, J. Geophys. Res., 113, D19202, doi:10.1029/2007JD009761, 2008.

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

Massling,~A., Stock,~M., Wehner,~B., Wu,~Z J., Hu,~M., Brügemann,~E., Gnauk,~T., Herrmann,~H., and Wiedensohler,~A.: Size segregated water uptake of the urban submicrometer aerosol in Beijing, Atmos. Environ., 43, 1578–1589, 2009.

McDonald,~J E.: Erroneous cloud-physics applications of raoult law,~J. Meteorol., 10, 68–78, 1953.

McMurry,~P H., Litchy,~M., Huang,~P.-F., Cai,~X., Turpin,~B J., Dick,~W D., and Hanson,~A.: Elemental composition and morphology of individual particles separated by size and \mboxhygroscopicity with the tdma, Atmos. Environ., 30, 101–108, 1996.

Mikhailov, E., Vlasenko, S., Niessner, R., and Pöschl, U.: Interaction of aerosol particles composed of protein and saltswith water vapor: hygroscopic growth and microstructural rearrangement, Atmos. Chem. Phys., 4, 323–350, doi:10.5194/acp-4-323-2004, 2004.

Mikhailov, E., Vlasenko, S., Martin, S. T., Koop, T., and Pöschl, U.: Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations, Atmos. Chem. Phys., 9, 9491–9522, doi:10.5194/acp-9-9491-2009, 2009.

Moore,~R H., and Nenes,~A.: Scanning flow CCN analysis – A method for fast measurements of ccn spectra, Aerosol Sci. Technol., 43, 1192–1207, 2009.

Moore,~R H., Nenes,~A., and Medina,~J.: Scanning Mobility CCN Analysis – A method for fast measurements of size resolved CCN distributions and activation kinetics,~Aerosol Sci. Technol., 44 , 861–871, doi:10.1080/02786820903289780, 2010.

Murphy,~D M., Cziczo,~D J., Froyd,~K D., Hudson,~P K., Matthew,~B M., Middlebrook,~A M., Peltier,~R E., Sullivan,~A., Thomson,~D S., and Weber,~R J.: Single-particle mass spectrometry of tropospheric aerosol particles,~J. Geophys. Res., 111, D23S32, \doi10.1029/2006jd007340, 2006.

Niedermeier, D., Wex, H., Voigtländer, J., Stratmann, F., Brüggemann, E., Kiselev, A., Henk, H., and Heintzenberg, J.: LACIS-measurements and parameterization of sea-salt particle hygroscopic growth and activation, Atmos. Chem. Phys., 8, 579–590, doi:10.5194/acp-8-579-2008, 2008.

Orsini,~D A., Wiedensohler,~A., and Covert,~D S.: Volatility measurements of atmospheric aerosols in the mid and south pacific using a~volatility-tandem-differential-mobility-analyzer, J. Aerosol Sci., 27, S53–S54, 1996.

Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, doi:10.5194/acp-7-1961-2007, 2007.

Petters,~M D., Carrico,~C M., Kreidenweis,~S M., Prenni,~A J., DeMott,~P J., Collett Jr.,~J L., and Moosmüller,~H.: Cloud condensation nucleation activity of biomass burning aerosol, J. Geophys. Res., 114, D22205, \doi10.1029/2009jd012353, 2009a.

Petters, M. D., Wex, H., Carrico, C. M., Hallbauer, E., Massling, A., McMeeking, G. R., Poulain, L., Wu, Z., Kreidenweis, S. M., and Stratmann, F.: Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol – Part 2: Theoretical approaches, Atmos. Chem. Phys., 9, 3999–4009, doi:10.5194/acp-9-3999-2009, 2009b.

Pruppacher,~H R. and Klett,~J D.: Microphysics of clouds and precipitation, Kluwer Academic Publishers, Dordrecht, 1997.

Pöschl,~U., Rose,~D., and Andreae,~M O.: Climatologies of cloudrelated aerosols – part~2: Particle hygroscopicity and cloud condensation nuclei activity, in: Clouds in the perturbed climate system, edited by: Heintzenberg,~J. and Charlson,~R J., MIT Press, Cambridge, 2009.

Reutter, P., Su, H., Trentmann, J., Simmel, M., Rose, D., Gunthe, S. S., Wernli, H., Andreae, M. O., and Pöschl, U.: Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN), Atmos. Chem. Phys., 9, 7067–7080, doi:10.5194/acp-9-7067-2009, 2009.

Rissler, J., Vestin, A., Swietlicki, E., Fisch, G., Zhou, J., Artaxo, P., and Andreae, M. O.: Size distribution and hygroscopic properties of aerosol particles from dry-season biomass burning in Amazonia, Atmos. Chem. Phys., 6, 471–491, doi:10.5194/acp-6-471-2006, 2006.

Robinson,~R A. and Stokes,~R H.: Electrolyte solutions, revised, Butterworths Scientific Pub, London, 1959.

Rose, D., Gunthe, S. S., Mikhailov, E., Frank, G. P., Dusek, U., Andreae, M. O., and Pöschl, U.: Calibration and measurement uncertainties of a continuous-flow cloud condensation nuclei counter (DMT-CCNC): CCN activation of ammonium sulfate and sodium chloride aerosol particles in theory and experiment, Atmos. Chem. Phys., 8, 1153–1179, doi:10.5194/acp-8-1153-2008, 2008.

Rose, D., Nowak, A., Achtert, P., Wiedensohler, A., Hu, M., Shao, M., Zhang, Y., Andreae, M. O., and Pöschl, U.: Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity, Atmos. Chem. Phys., 10, 3365–3383, doi:10.5194/acp-10-3365-2010, 2010a.

Rose, D., Garland, R. M., Yang, H., Gunthe, S. S., Su, H., Berghof, M., Cheng, Y. F., Wehner, B., Wiedensohler, A., Takegawa, N., Kondo, Y., Hu, M., Zhang, Y., Andreae, M. O., and Pöchl, U.: Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 2: Size-resolved aerosol chemical composition, diurnal cycles, and mixing state of CCN-inactive soot particles, to be submitted, 2010b.

Rose, D.: Measurement and modeling of cloud condensation nuclei in continental air, Doctoral dissertation, Johannes-Gutenberg-University, Mainz, Germany, 2010c.

Schwarz,~J P., Gao,~R S., Fahey,~D W., Thomson,~D S., Watts,~L A., Wilson,~J C., Reeves,~J M., Darbeheshti,~M., Baumgardner,~D G., Kok,~G L., Chung,~S H., Schulz,~M., Hendricks,~J., Lauer,~A., Kärcher,~B., Slowik,~J G., Rosenlof,~K H., Thompson,~T L., Langford,~A O., Loewenstein,~M., and Aikin,~K C.: Single-particle measurements of midlatitude black carbon and light-scattering aerosols from the boundary layer to the lower stratosphere, J. Geophys. Res., 111, D16207, \doi10.1029/2006jd007076, 2006.

Seinfeld,~J H. and Pandis,~S N.: Atmospheric chemistry and physics, from air pollution to climate change, John Wiley, New York, 362~pp., 2006.

Snider, J., Wex, H., Rose, D., Kristensson, A., Stratmann, F., Hennig, T., Henning, S., Kiselev, A., Bilde, M., Burkhart, M., Dusek, U., Frank, G., Kiendler-Scharr, A., Mentel, Th., Petters, M., and Pöschl, U.: Intercomparison of cloud condensation nuclei and hygroscopic fraction measurements: Coated soot particles investigated during LACIS Experiment in November (LExNo), J. Geophys. Res., doi:10.1029/2009JD012618, in press, 2010.

Stolzenburg, M. and McMurry, P. H.: TDMAFIT user's manual, Tech. Rep. PTL Publication No. 653, University of Minnesota, Department of Mechanical Engineering, Particle Technology Laboratory, 1988.

Sullivan, R. C., Moore, M. J. K., Petters, M. D., Kreidenweis, S. M., Roberts, G. C., and Prather, K. A.: Effect of chemical mixing state on the hygroscopicity and cloud nucleation properties of calcium mineral dust particles, Atmos. Chem. Phys., 9, 3303–3316, doi:10.5194/acp-9-3303-2009, 2009.

Svenningsson, B., Rissler, J., Swietlicki, E., Mircea, M., Bilde, M., Facchini, M. C., Decesari, S., Fuzzi, S., Zhou, J., Mønster, J., and Rosenørn, T.: Hygroscopic growth and critical supersaturations for mixed aerosol particles of inorganic and organic compounds of atmospheric relevance, Atmos. Chem. Phys., 6, 1937–1952, doi:10.5194/acp-6-1937-2006, 2006.

Svenningsson, B. and Bilde, M.: Relaxed step functions for evaluation of CCN counter data on size-separated aerosol particles, Aerosol Sci., 39, 592–608, 2008.

Swietlicki, E., Hansson, H. C., Meri, K., Svenningsson, B., Massling, A., McFiggans, G., McMurry, P. H., Pet, T., Tunved, P., Gysel, M., Topping, D., Weingartner, E., Baltensperger, U., Rissler, J., Wiedensohler, A., and Kulmala, M.: Hygroscopic properties of submicrometer atmospheric aerosol particles measured with h-tdma instruments in various environments a review, Tellus B, 60, 432–469, 2008.

Vestin,~A., Rissler,~J., Swietlicki,~E., Frank,~G P., and Andreae,~M O.: Cloud-nucleating properties of the amazonian biomass burning aerosol: Cloud condensation nuclei measurements and modeling, J. Geophys. Res., 112, D14201, \doi10.1029/2006jd008104, 2007.

Wehner,~B., Berghof,~M., Cheng,~Y F., Achtert,~P., Birmili,~W., Nowak,~A., Wiedensohler,~A., Garland,~R M., Pöschl,~U., Hu,~M., and Zhu,~T.: Mixing state of nonvolatile aerosol particle fractions and comparison with light absorption in the polluted Beijing region,~J. Geophys. Res., 114, D00G17, \doi10.1029/2008jd010923, 2009.

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 super-saturations of an atmospheric hulis sample, Geophys. Res. Lett., 34, L02818, \doi10.1029/2006gl028260, 2007.

Wex, H., Petters, M. D., Carrico, C. M., Hallbauer, E., Massling, A., McMeeking, G. R., Poulain, L., Wu, Z., Kreidenweis, S. M., and Stratmann, F.: Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol: Part 1 – Evidence from measurements, Atmos. Chem. Phys., 9, 3987–3997, doi:10.5194/acp-9-3987-2009, 2009.

Wiedensohler,~A., Cheng,~Y F., Nowak,~A., Wehner,~B., Achtert,~P., Berghof,~M., Birmili,~W., Wu,~Z J., Hu,~M., Zhu,~T., Takegawa,~N., Kita,~K., Kondo,~Y., Lou,~S R., Hofzumahaus,~A., Holland,~F., Wahner,~A., Gunthe,~S S., Rose,~D., Su,~H., and Pöschl,~U.: Rapid aerosol particle growth and increase of cloud condensation nucleus activity by secondary aerosol formation and condensation: A~case study for regional air pollution in Northeastern China, J. Geophys. Res., 114, D00G08, \doi10.1029/2008jd010884, 2009.