References

ACP

Atmospheric Chemistry and Physics

ACP

Atmos. Chem. Phys.

1680-7324

Copernicus Publications

Göttingen, Germany

10.5194/acp-13-6227-2013

An examination of parameterizations for the CCN number concentration based on in situ measurements of aerosol activation properties in the North China Plain

Deng

Z. Z.

https://orcid.org/0000-0002-0955-6350

¹ ² Zhao

C. S.

² Ma

² Ran

¹ Zhou

G. Q.

https://orcid.org/0000-0001-6016-4363

³ Lu

D. R.

¹ Zhou

X. J.

² ⁴

Key Laboratory of Middle Atmosphere and Global Environment Observation, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China

Department of Atmospheric and Oceanic Sciences, School of Physics, Peking University, Beijing, China

Shanghai Typhoon Institute, China Meteorological Administration, Shanghai, China

Centre for Atmosphere Watch and Services, Chinese Academy of Meteorological Sciences, China Meteorological Administration, Beijing, China

01 07 2013

13 13 6227 6237

2013

This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/

This article is available from https://acp.copernicus.org/articles/13/6227/2013/acp-13-6227-2013.html

The full text article is available as a PDF file from https://acp.copernicus.org/articles/13/6227/2013/acp-13-6227-2013.pdf

Precise quantification of the cloud condensation nuclei (CCN) number concentration is crucial for understanding aerosol indirect effects and characterizing these effects in models. An evaluation of various methods for CCN parameterization was carried out in this paper based on in situ measurements of aerosol activation properties within HaChi (Haze in China) project. Comparisons were made by closure studies between methods using CCN spectra, bulk activation ratios, cut-off diameters and size-resolved activation ratios. The estimation of CCN number concentrations by the method using aerosol size-resolved activation ratios, either averaged over a day or with diurnal variation, was found to be most satisfying and straightforward. This could be well expected since size-resolved activation ratios include information regarding the effects of size-resolved chemical compositions and mixing states on aerosol activation properties. The method using the averages of critical diameters, which were inferred from measured CCN number concentrations and particle number size distributions, also provided a good prediction of the CCN number concentration. Based on comparisons of all these methods in this paper, it was recommended that the CCN number concentration be predicted using particle number size distributions with inferred critical diameters or size-resolved activation ratios.

References 1

Albrecht, B. A.: Aerosols, Cloud Microphysics, and Fractional Cloudiness, Science, 245, 1227–1230, <a href="http://dx.doi.org/10.1126/science.245.4923.1227">https://doi.org/10.1126/science.245.4923.1227</a>, 1989.

Bigg, E. K., and Leek, C.: Cloud-active particles over the central Arctic Ocean, J. Geophys. Res., 106, 32155–32166, <a href="http://dx.doi.org/10.1029/1999jd901152">https://doi.org/10.1029/1999jd901152</a>, 2001.

Bougiatioti, A., Fountoukis, C., Kalivitis, N., Pandis, S. N., Nenes, A., and Mihalopoulos, N.: Cloud condensation nuclei measurements in the marine boundary layer of the Eastern Mediterranean: CCN closure and droplet growth kinetics, Atmos. Chem. Phys., 9, 7053–7066, <a href="http://dx.doi.org/10.5194/acp-9-7053-2009">https://doi.org/10.5194/acp-9-7053-2009</a>, 2009.

Breed, D., Bruintjes, R., Jensen, T., Salazar, V., and Piketh, S.: Aerosol and cloud droplet measurements in the United Arab Emirates, 11th Conference on Cloud Physics, 2002.

Delene, D. J. and Deshler, T.: Vertical profiles of cloud condensation nuclei above Wyoming, J. Geophys. Res., 106, 12579–12588, <a href="http://dx.doi.org/10.1029/2000jd900800">https://doi.org/10.1029/2000jd900800</a>, 2001.

Deng, Z., Zhao, C., Zhang, Q., Huang, M., and Ma, X.: Statistical analysis of microphysical properties and the parameterization of effective radius of warm clouds in Beijing area, Atmos. Res., 93, 888–896, 2009.

Deng, Z. Z., Zhao, C. S., Ma, N., Liu, P. F., Ran, L., Xu, W. Y., Chen, J., Liang, Z., Liang, S., Huang, M. Y., Ma, X. C., Zhang, Q., Quan, J. N., Yan, P., Henning, S., Mildenberger, K., Sommerhage, E., Schäfer, M., Stratmann, F., and Wiedensohler, A.: Size-resolved and bulk activation properties of aerosols in the North China Plain, Atmos. Chem. Phys., 11, 3835–3846, <a href="http://dx.doi.org/10.5194/acp-11-3835-2011">https://doi.org/10.5194/acp-11-3835-2011</a>, 2011.

Detwiler, A., Langerud, D., and Depue, T.: Investigation of the Variability of Cloud Condensation Nuclei Concentrations at the Surface in Western North Dakota, J. Appl. Meteorol. Clim., 49, 136–145, 2010.

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, <a href="http://dx.doi.org/10.1126/science.1125261">https://doi.org/10.1126/science.1125261</a>, 2006.

Ervens, B., Cubison, M. J., Andrews, E., Feingold, G., Ogren, J. A., Jimenez, J. L., Quinn, P. K., Bates, T. S., Wang, J., Zhang, Q., Coe, H., Flynn, M., and Allan, J. D.: CCN predictions using simplified assumptions of organic aerosol composition and mixing state: a synthesis from six different locations, Atmos. Chem. Phys., 10, 4795–4807, <a href="http://dx.doi.org/10.5194/acp-10-4795-2010">https://doi.org/10.5194/acp-10-4795-2010</a>, 2010.

Fitzgerald, J. W.: Dependence of the supersaturation spectrum of CCN on aerosol size distribution and composition, J. Atmos. Sci., 30, 628–634, 1973.

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, <a href="http://dx.doi.org/10.5194/acpd-6-4879-2006">https://doi.org/10.5194/acpd-6-4879-2006</a>, 2006..

Gunthe, S. S., Rose, D., Su, H., Garland, R. M., Achtert, P., Nowak, A., Wiedensohler, A., Kuwata, M., Takegawa, N., Kondo, Y., Hu, M., Shao, M., Zhu, T., Andreae, M. O., and Pöschl, U.: Cloud condensation nuclei (CCN) from fresh and aged air pollution in the megacity region of Beijing, Atmos. Chem. Phys., 11, 11023–11039, <a href="http://dx.doi.org/10.5194/acp-11-11023-2011">https://doi.org/10.5194/acp-11-11023-2011</a>, 2011.

Hagen, D. E. and Alofs, D. J.: Linear Inversion Method to Obtain Aerosol Size Distributions from Measurements with a Differential Mobility Analyzer, Aerosol Sci. Tech., 2, 465–475, 1983.

Hobbs, P. V., Stith, J. L., and Radke, L. F.: Cloud-Active Nuclei from Coal-Fired Electric Power Plants and Their Interactions with Clouds, J. Appl. Meteorol., 19, 439–451, <a href="http://dx.doi.org/10.1175/1520-0450(1980)019<0439:canfcf>2.0.CO;2">https://doi.org/10.1175/1520-0450(1980)019<0439:canfcf>2.0.CO;2</a>, 1980.

Hudson, J. G. and Yum, S. S.: Cloud condensation nuclei spectra and polluted and clean clouds over the Indian Ocean, J. Geophys. Res., 107, 8022, <a href="http://dx.doi.org/10.1029/2001jd000829">https://doi.org/10.1029/2001jd000829</a>, 2002.

Hudson, J. G., Garrett, T. J., Hobbs, P. V., Strader, S. R., Xie, Y., and Yum, S. S.: Cloud Condensation Nuclei and Ship Tracks, J. Atmos. Sci., 57, 2696-2706, <a href="http://dx.doi.org/10.1175/1520-0469(2000)057<2696:CCNAST>2.0.CO;2">https://doi.org/10.1175/1520-0469(2000)057<2696:CCNAST>2.0.CO;2</a>, 2000.

Ji, Q. and Shaw, G. E.: On supersaturation spectrum and size distributions of cloud condensation nuclei, Geophys. Res. Lett., 25, 1903–1906, <a href="http://dx.doi.org/10.1029/98gl01404">https://doi.org/10.1029/98gl01404</a>, 1998.

Junge, C. and McLaren, E.: Relationship of cloud nuclei spectra to aerosol size distribution and composition, J. Atmos. Sci., 28, 382–390, 1971.

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, <a href="http://dx.doi.org/10.1029/2009jd012447">https://doi.org/10.1029/2009jd012447</a>, 2010.

Kerminen, V.-M., Paramonov, M., Anttila, T., Riipinen, I., Fountoukis, C., Korhonen, H., Asmi, E., Laakso, L., Lihavainen, H., Swietlicki, E., Svenningsson, B., Asmi, A., Pandis, S. N., Kulmala, M., and Petäjä, T.: Cloud condensation nuclei production associated with atmospheric nucleation: a synthesis based on existing literature and new results, Atmos. Chem. Phys., 12, 12037–12059, <a href="http://dx.doi.org/10.5194/acp-12-12037-2012">https://doi.org/10.5194/acp-12-12037-2012</a>, 2012.

Knutson, E. O. and Whitby, K. T.: Aerosol classification by electric mobility: apparatus, theory, and applications, J. Aerosol Sci., 6, 443–451, 1975.

Kuwata, M., Kondo, Y., Miyazaki, Y., Komazaki, Y., Kim, J. H., Yum, S. S., Tanimoto, H., and Matsueda, H.: Cloud condensation nuclei activity at Jeju Island, Korea in spring 2005, Atmos. Chem. Phys., 8, 2933–2948, <a href="http://dx.doi.org/10.5194/acp-8-2933-2008">https://doi.org/10.5194/acp-8-2933-2008</a>, 2008.

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

Lathem, T. L. and Nenes, A.: Water Vapor Depletion in the DMT Continuous-Flow CCN Chamber: Effects on Supersaturation and Droplet Growth, Aerosol Sci. Tech., 45, 604–615, <a href="http://dx.doi.org/10.1080/02786826.2010.551146">https://doi.org/10.1080/02786826.2010.551146</a>, 2011.

Liu, P. F., Zhao, C. S., Göbel, T., Hallbauer, E., Nowak, A., Ran, L., Xu, W. Y., Deng, Z. Z., Ma, N., Mildenberger, K., Henning, S., Stratmann, F., and Wiedensohler, A.: Hygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain, Atmos. Chem. Phys., 11, 3479–3494, <a href="http://dx.doi.org/10.5194/acp-11-3479-2011">https://doi.org/10.5194/acp-11-3479-2011</a>, 2011.

Low, R. D. H.: A generalized equation for the solution effect in droplet growth, J. Atmos. Sci., 26, 608–611, 1969.

Ma, N., Zhao, C. S., Nowak, A., Müller, T., Pfeifer, S., Cheng, Y. F., Deng, Z. Z., Liu, P. F., Xu, W. Y., Ran, L., Yan, P., Göbel, T., Hallbauer, E., Mildenberger, K., Henning, S., Yu, J., Chen, L. L., Zhou, X. J., Stratmann, F., and Wiedensohler, A.: Aerosol optical properties in the North China Plain during HaChi campaign: an in-situ optical closure study, Atmos. Chem. Phys., 11, 5959–5973, <a href="http://dx.doi.org/10.5194/acp-11-5959-2011">https://doi.org/10.5194/acp-11-5959-2011</a>, 2011.

Ma, N., Zhao, C. S., Müller, T., Cheng, Y. F., Liu, P. F., Deng, Z. Z., Xu, W. Y., Ran, L., Nekat, B., van Pinxteren, D., Gnauk, T., Müller, K., Herrmann, H., Yan, P., Zhou, X. J., and Wiedensohler, A.: A new method to determine the mixing state of light absorbing carbonaceous using the measured aerosol optical properties and number size distributions, Atmos. Chem. Phys., 12, 2381–2397, <a href="http://dx.doi.org/10.5194/acp-12-2381-2012">https://doi.org/10.5194/acp-12-2381-2012</a>, 2012.

Martins, J., Gonçalves, F., Morales, C., Fisch, G., Pinheiro, F., Leal Júnior, J., Oliveira, C., Silva, E., Oliveira, J., Costa, A., and Silva Dias, M.: Cloud condensation nuclei from biomass burning during the Amazonian dry-to-wet transition season, Meteorol. Atmos. Phys., 104, 83–93, 2009.

Medina, J., Nenes, A., Sotiropoulou, R.-E. P., Cottrell, L. D., Ziemba, L. D., Beckman, P. J., and Griffin, R. J.: Cloud condensation nuclei closure during the International Consortium for Atmospheric Research on Transport and Transformation 2004 campaign: Effects of size-resolved composition, J. Geophys. Res., 112, D10S31, <a href="http://dx.doi.org/10.1029/2006jd007588">https://doi.org/10.1029/2006jd007588</a>, 2007.

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, <a href="http://dx.doi.org/10.5194/acp-5-3111-2005">https://doi.org/10.5194/acp-5-3111-2005</a>, 2005.

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. Tech., 44, 861–871, 2010.

Petters, M. D., Prenni, A. J., Kreidenweis, S. M., and DeMott, P. J.: On Measuring the Critical Diameter of Cloud Condensation Nuclei Using Mobility Selected Aerosol, Aerosol Sci. Tech., 41, 907–913, 2007.

Pruppacher, H. R. and Klett, J. D.: Microphysics of clouds and precipitation, Kluwer Academic Publishers, Dordrecht, the Netherlands, 944 pp., 1997.

Ramanathan, V., Crutzen, P. J., Kiehl, J. T., and Rosenfeld, D.: Aerosols, Climate, and the Hydrological Cycle, Science, 294, 2119–2124, <a href="http://dx.doi.org/10.1126/science.1064034">https://doi.org/10.1126/science.1064034</a>, 2001.

Ran, L., Zhao, C. S., Xu, W. Y., Lu, X. Q., Han, M., Lin, W. L., Yan, P., Xu, X. B., Deng, Z. Z., Ma, N., Liu, P. F., Yu, J., Liang, W. D., and Chen, L. L.: VOC reactivity and its effect on ozone production during the HaChi summer campaign, Atmos. Chem. Phys., 11, 4657–4667, <a href="http://dx.doi.org/10.5194/acp-11-4657-2011">https://doi.org/10.5194/acp-11-4657-2011</a>, 2011.

Roberts, G. C. and Nenes, A.: A continuous-flow streamwise thermal-gradient CCN chamber for atmospheric measurements, Aerosol Sci. Tech., 39, 206–221, 2005.

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, <a href="http://dx.doi.org/10.1029/2001jd000583">https://doi.org/10.1029/2001jd000583</a>, 2002.

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, <a href="http://dx.doi.org/10.5194/acp-8-1153-2008">https://doi.org/10.5194/acp-8-1153-2008</a>, 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, <a href="http://dx.doi.org/10.5194/acp-10-3365-2010">https://doi.org/10.5194/acp-10-3365-2010</a>, 2010.

Ross, K. E., Piketh, S. J., Bruintjes, R. T., Burger, R. P., Swap, R. J., and Annegarn, H. J.: Spatial and seasonal variations in CCN distribution and the aerosol-CCN relationship over southern Africa, J. Geophys. Res., 108, 8481, <a href="http://dx.doi.org/10.1029/2002jd002384">https://doi.org/10.1029/2002jd002384</a>, 2003.

Snider, J. R. and Brenguier, J. L.: Cloud condensation nuclei and cloud droplet measurements during ACE-2, Tellus B, 52, 828–842, 2000.

Squires, P. and Twomey, S.: A Comparison of Cloud Nucleus Measurements over Central North America and the Caribbean Sea, J. Atmos. Sci., 23, 401–404, <a href="http://dx.doi.org/10.1175/1520-0469(1966)023<0401:acocnm>2.0.CO;2">https://doi.org/10.1175/1520-0469(1966)023<0401:acocnm>2.0.CO;2</a>, 1966.

Stroud, C. A., Nenes, A., Jimenez, J. L., DeCarlo, P. F., Huffman, J. A., Bruintjes, R., Nemitz, E., Delia, A. E., Toohey, D. W., Guenther, A. B., and Nandi, S.: Cloud Activating Properties of Aerosol Observed during CELTIC, J. Atmos. Sci., 64, 441–459, 2007.

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

Twohy, C. H. and Anderson, J. R.: Droplet nuclei in non-precipitating clouds: composition and size matter, Environ. Res. Lett., 3, 045002, <a href="http://dx.doi.org/10.1088/1748-9326/3/4/045002">https://doi.org/10.1088/1748-9326/3/4/045002</a>, 2008.

Twomey, S.: The nuclei of natural cloud formation part I: The chemical diffusion method and its application to atmospheric nuclei, Pure Appl. Geophys., 43, 227–242, 1959a.

Twomey, S.: The nuclei of natural cloud formation part II: The supersaturation in natural clouds and the variation of cloud droplet concentration, Pure Appl. Geophys., 43, 243-249, 1959b.

Twomey, S.: Pollution and the Planetary Albedo, Atmos. Environ., 8, 1251–1256, 1974.

Twomey, S. and Warner, J.: Comparison of Measurements of Cloud Droplets and Cloud Nuclei, J. Atmos. Sci., 24, 702-703, <a href="http://dx.doi.org/10.1175/1520-0469(1967)024<0702:COMOCD>2.0.CO;2">https://doi.org/10.1175/1520-0469(1967)024<0702:COMOCD>2.0.CO;2</a>, 1967.

Wang, J., Cubison, M. J., Aiken, A. C., Jimenez, J. L., and Collins, D. R.: The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols, Atmos. Chem. Phys., 10, 7267–7283, <a href="http://dx.doi.org/10.5194/acp-10-7267-2010">https://doi.org/10.5194/acp-10-7267-2010</a>, 2010.

Wex, H., McFiggans, G., Henning, S., and Stratmann, F.: Influence of the external mixing state of atmospheric aerosol on derived CCN number concentrations, Geophys. Res. Lett., 37, 10805, <a href="http://dx.doi.org/10.1029/2010GL043337">https://doi.org/10.1029/2010GL043337</a>, 2010.

Wiedensohler, A.: An approximation of the bipolar charge distribution for particles in the submicron size range, J. Aerosol Sci., 19, 387–389, 1988.

Wiedensohler, A., Birmili, W., Nowak, A., Sonntag, A., Weinhold, K., Merkel, M., Wehner, B., Tuch, T., Pfeifer, S., Fiebig, M., Fjäraa, A. M., Asmi, E., Sellegri, K., Depuy, R., Venzac, H., Villani, P., Laj, P., Aalto, P., Ogren, J. A., Swietlicki, E., Williams, P., Roldin, P., Quincey, P., Hüglin, C., Fierz-Schmidhauser, R., Gysel, M., Weingartner, E., Riccobono, F., Santos, S., Grüning, C., Faloon, K., Beddows, D., Harrison, R., Monahan, C., Jennings, S. G., O'Dowd, C. D., Marinoni, A., Horn, H. G., Keck, L., Jiang, J., Scheckman, J., McMurry, P. H., Deng, Z., Zhao, C. S., Moerman, M., Henzing, B., de Leeuw, G., Löschau, G., and Bastian, S.: Mobility particle size spectrometers: harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions, Atmos. Meas. Tech., 5, 657–685, <a href="http://dx.doi.org/10.5194/amt-5-657-2012">https://doi.org/10.5194/amt-5-657-2012</a>, 2012.

Xu, W. Y., Zhao, C. S., Ran, L., Deng, Z. Z., Liu, P. F., Ma, N., Lin, W. L., Xu, X. B., Yan, P., He, X., Yu, J., Liang, W. D., and Chen, L. L.: Characteristics of pollutants and their correlation to meteorological conditions at a suburban site in the North China Plain, Atmos. Chem. Phys., 11, 4353–4369, <a href="http://dx.doi.org/10.5194/acp-11-4353-2011">https://doi.org/10.5194/acp-11-4353-2011</a>, 2011.

Young, K. C. and Warren, A. J.: A reexamination of the derivation of the equilibrium supersaturation curve for soluble particles, J. Atmos. Sci., 49, 1138–1143, 1992.

Zhao, C., Tie, X., Brasseur, G., Noone, K. J., Nakajima, T., Zhang, Q., Zhang, R., Huang, M., Duan, Y., Li, G., and Ishizaka, Y.: Aircraft measurements of cloud droplet spectral dispersion and implications for indirect aerosol radiative forcing, Geophys. Res. Lett., 33, L16809, <a href="http://dx.doi.org/10.1029/2006gl026653">https://doi.org/10.1029/2006gl026653</a>, 2006a.

Zhao, C., Tie, X., and Lin, Y.: A possible positive feedback of reduction of precipitation and increase in aerosols over eastern central China, Geophys. Res. Lett., 33, L11814, <a href="http://dx.doi.org/10.1029/2006gl025959">https://doi.org/10.1029/2006gl025959</a>, 2006b.