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15805
15851
2007-11-13
Cloud condensation nuclei activity at Jeju Island, Korea in spring 2005
M. Kuwata
kuwata@atmos.rcast.u-tokyo.ac.jp
Y. Kondo
Y. Miyazaki
Y. Komazaki
J. H. Kim
S. S. Yum
H. Tanimoto
H. Matsueda
Research Center for Advanced Science and Technology, University of Tokyo, Tokyo, Japan
Department of Atmospheric Science, Yonsei University, Seoul, Korea
Atmospheric Environmental Div., National Inst. for Environmental Studies, Tsukuba, Japan
Geochemical Research Department, Meteorological Research Institute, Tsukuba, Japan
We measured the number concentrations of cloud condensation nuclei (CCN) and
the size distributions of CCN/CN (CN: condensation nuclei) ratios at
supersaturations (<i>SS</i>s) of 0.097, 0.27, 0.58, and 0.97% at Jeju-Island,
Korea during March-April 2005. Measurements of aerosol inorganic ions,
water-soluble organic carbon (WSOC), organic carbon (OC), and elemental
carbon (EC) in PM<sub>2.5</sub> were simultaneously made. The CCN/CN ratios increased
with increasing particle diameter, and the diameter at CCN/CN=0.5 was
defined as <i>D</i><sub>50</sub>. <i>D</i><sub>50</sub> represents the activation dry diameter of
atmospheric particles. The average <i>D</i><sub>50</sub> at <i>SS</i>=0.097% and 0.97% was
136 nm and 31 nm, respectively. The temporal variation of <i>D</i><sub>50</sub> at <i>SS</i>=0.097%
was correlated with the mass fraction of water-soluble components
(inorganic ions + WSOC), indicating that the temporal variation of CCN
activity was mainly controlled by changes in the water-soluble components
fraction. The critical dry diameter (<i>D</i><sub>crit</sub>), which is the threshold dry
diameter for CCN activation, was calculated from the observed aerosol
chemical compositions by Köhler theory for comparison with <i>D</i><sub>50</sub>. The
<i>D</i><sub>50</sub> at <i>SS</i>=0.097% was correlated (<i>r</i><sup>2</sup>=0.48) with calculated
<i>D</i><sub>crit</sub>, although <i>D</i><sub>crit</sub> were larger than <i>D</i><sub>50</sub> by 20–29% on
average. The systematic difference between <i>D</i><sub>50</sub> and <i>D</i><sub>crit</sub> could be
caused by the size dependence of the aerosol chemical compositions or
surface tension lowering caused by the mixing of water-soluble organic
compounds. This difference corresponds to a 27±14% uncertainty in
the CCN number concentration estimated from the observed particle number
size distribution.
Akimoto, H: Global air quality and pollution, Science, 302, 1716–1719, 2003.
Arnold, F: Atmospheric aerosol and cloud condensation nuclei formation: A possible influence of cosmic rays?, Space Sci. Rev., 125, 169–186, 2006.
Bae, M.-S., Schauer, J. J., DeMinter, J. T., Turner, J. R., Smith D., and Cary, R. A.: Validation of a semi-continuous instrument for elemental carbon and organic carbon using a thermal-optical method, Atmos. Environ., 38, 2885–2893, 2004.
Buzorius, G., McNaughton, C. S., Clarke, A. D., Covert, D. S., Blomquist, B., Nielsen, K., and Brechtel, F. J.: Secondary aerosol formation in continental outflow conditions during ACE-Asia, J. Geophys. Res., 109, D24203, doi:10.1029/2004JD004749, 2004.
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(D22), 28 711–28 718, 2001.
Carmichael, G. R., Hong, M., Ueda, H., Chen, L., Murano, K., Park, J. K., Lee, H., Kim, Y., Kang, C., and Shim, S.: Aerosol composition at Cheju Island, Korea, J. Geophys. Res., 102(D5), 6047–6062, 1997.
Cavalli, F., Facchini, M. C., Decesari, S., et al.: Advances in characterization of size-resolved organic matter in marine aerosol over the North Atlantic, J. Geophys. Res., 109, D24215, doi:10.1029/2004JD005137, 2004.
Chameides, W. L., Luo, C., Saylor, R., Streets, D. G., Huang, Y., Bergin, M., and Giorgi, F.: Correlation between model-calculated anthropogenic aerosols and satellite-derived cloud optical depths: Indication of indirect effect?, J. Geophys. Res., 107(D10), 4085, doi:10.1029/2000JD000208, 2002.
Clegg, S. L., Rard, J. A., and Pitzer, K. S.: Thermodynamic properties of 0-6 mol Kg-1 aqueous sulfuric acid from 273.15 K to 328.15 K, J. Chem. Soc. Faraday Trans., 90, 1875–1894, 1994.
Clegg, S. L., Milioto, S., and Palmer, D. A.: Osmotic and activity coefficients of aqueous (NH$_4)_2$SO<sub>4</sub> as a function of temperature, and (NH$_4)_2$SO<sub>4</sub> – H<sub>2</sub>SO<sub>4</sub> mixtures at 298.15 K and 323.15 K, J. Chem. Eng. Data, 41, 455–467, 1996.
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(D13), 16 597–16 608, 1998.
Decesari, S., Facchini, M. C., Fuzzi, S., McFiggans, G. B., Coe, H., and Bower, K. N.: The water-soluble organic component of size-segregated aerosol, cloud water and wet depositions from Jeju Island during ACE-Asia, Atmos. Environ., 39, 211–222, 2005.
Dinar, E., Taraniuk, I., Graber, E. R., Katsman, S., Moise, T., Anttila, T., Mentel, T. F., and Rudich, Y.: Cloud Condensation Nuclei properties of model and atmospheric HULIS, Atmos. Chem. Phys., 6, 2465–2481, 2006a.
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, 2006b.
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, 2006.
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.
Grabber, E. R. and Rudich, Y: Atmospheric HULIS: How humic-like are they? A comprehensive and critical review, Atmos. Phys. Chem., 6, 729–753, 2006.
Hoffer, A., Gelencsèr, A., Guyon, P., Kiss., G., Schmid, O., Frank, G. P., Artaxo, P., and Andrea, M. O.: Optical properties of humic-like substances (HULIS) in biomass-burning aerosols, Atmos. Chem. Phys., 6, 3563–3570, 2006, http://www.atmos-chem-phys.net/6/3563/2006/http://www.atmos-chem-phys.net/6/3563/2006/.
Hudson, J. G. and Yum, S. S.: Cloud condensation nuclei spectra and polluted and clean clouds over the Indian Ocean, J. Geophys. Res., 107(D19), 8022, doi:10.1029/2001JD000829, 2002.
Kawamoto, K., Hayasaka, T., Uno, I., and Ohara, T.: A correlative study on the relationship between modeled anthropogenic aerosol concentration and satellite-observed cloud properties over east Asia, J. Geophys. Res., 111, D19201, doi:10.1029/2005JD006919, 2006.
Kawamura, K., Umemoto, N., Mochida, M., Bertram, T., Howell, S., and Huebert, B. J.: Water-soluble dicarboxylic acids in the tropospheric aerosols collected over east Asia and western North Pacific by ACE-Asia C-130 aircraft, J. Geophys. Res., 108(D23), 8639, doi:10.1029/2002JD003256, 2003.
Kim, J., Yoon, S.-C., Jefferson, A., Kim, S.-W.: Aerosol hygroscopic properties during Asian dust pollution, and biomass burning episodes at Gosan, Korea in April 2001, Atmos. Environ., 40, 1550–1560, 2006.
Kiss, G, Tombàcz. E., and Hanson, H.-C.: Surface tension effects of Humic-like substances in the aqueous extract of tropospheric fine aerosol, J. Atmos. Chem., 50, 279–294, 2005.
Knutson, E. O. and Whitby, K. T.: Aerosol classification by electric mobility: Apparatus, theory, and applications, J. Aerosol. Sci., 6, 443–451, 1975.
Kondo, Y., Komazaki, Y., Miyazaki, Y., et al.: Temporal variations of elemental carbon in Tokyo, J. Geophys. Res., 111, D12205, doi:10.1029/2005JD006257, 2006.
Kondo, Y., Miyazaki, Y., Takegawa, N., Miyakawa, T., Weber, R. J., Jimenez, J. L., Zhang, Q., and Worsnop, D. R.: Oxygenated and water-soluble organic aerosols in Tokyo, J. Geophys. Res., 112, D01203, doi:10.1029/2006JD007056, 2007.
Kreidenweis, S. M., Koehler, K., DeMott, P. J., Prenni, A. J., Carrico, C., and Ervens, B.: Water activity and activation diameters from hygroscopicity data – Part I: Theory and application to inorganic salts, Atmos. Chem. Phys., 5, 1357–1370, 2005
Kuwata, M., Kondo, Y., Mochida, M., Takegawa, N., and Kawamura, K.: Dependence of CCN activity of less volatile particles on the amount of coating observed in Tokyo, J. Geophys. Res., 112, D11207, doi:10.1029/2006JD007758, 2007.
Laaksonen, A., Hamed, A., Joutsensaari, J., Hiltunen, L., Cavalli, F., Junkermann, W., Asmi, A., Fuzzi, S., and Facchini, M. C.: Cloud condensation nucleus production from nucleation events at a highly polluted region, Geophys. Res. Lett., 32, L06812, doi:10.1029/2004GL022092, 2005.
Lee, J. Y., Kim, Y. P., Kang, C.-H., Ghim, Y. S., and Kaneyasu, N.: Temporal trend and long-range transport of particulate polycyclic aromatic hydrocarbons at Gosan in northeast Asia between 2001 and 2004, J. Geophys. Res., 111, D11303, doi:10.1029/2005JD006537, 2006.
Lohmann, U. and Feichter, J.: Global indirect aerosol effects: a review, Atmos. Chem. Phys., 5, 715–737, 2005, http://www.atmos-chem-phys.net/5/715/2005/http://www.atmos-chem-phys.net/5/715/2005/.
Markowski, G. R.: Improving Twomey's algorithm for inversion of aerosol measurement data, Aerosol. Sci . Technol., 7, 127–141, 1987.
McFiggans, G., Artaxo, P., Baltensperger, U., et al.: The effect of physical and chemical aerosol properties on warm cloud droplet activation, Atmos. Chem. Phys., 6, 2593–2649, 2006, http://www.atmos-chem-phys.net/6/2593/2006/http://www.atmos-chem-phys.net/6/2593/2006/.
Matsumoto, K., H. Tanaka, H., Nagao, I., and Ishizaka, Y.: Contribution of particulate sulfate and organic carbon to cloud condensation nuclei in the marine atmosphere, Geophys. Res. Lett., 24(6), 655–658, 1997.
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, doi:10.1029/2006JD007588, 2007.
Miyazaki, Y., Kondo, Y., Takegawa, N., Komazaki, Y., Fukuda, M., Kawamura, K., Mochida, M., Okuzawa, K., and Weber, R. J.: Time-resolved measurements of water-soluble organic carbon in Tokyo, J. Geophys. Res., 111, D23206, doi:10.1029/2006JD007125, 2006.
Miyazaki, Y., Kondo, Y., Kodama, D., Han, S., Koike, M., Komazaki, Y., Tanimoto, H., and Matsueda, H.: Chemical characteristics of water-soluble organic carbon in the Asian outflow, J. Geophys. Res., in press, 2007.
Mochida, M., Kawamura, K., Umemoto, N., Kobayashi, M., Matsunaga, S., Lim, H., Turpin, B. J., Bates, T. S., and Simoneit, B. R. T.: Spatial distributions of oxygenated organic compounds (dicarboxylic acids, fatty acids, and levoglucosan) in marine aerosols over the western Pacific and off the coast of East Asia: Continental outflow of organic aerosols during the ACE-Asia campaign, J. Geophys. Res., 108(D23), 8638, doi:10.1029/2002JD003249, 2003.
Mochida, M., Kuwata, M., Miyakawa, T., Takegawa, N., Kawamura, K., and Kondo, Y.: Relationship between hygroscopicity and cloud condensation nuclei activity for urban aerosols in Tokyo, J. Geophys. Res., 111, D23204, doi:10.1029/2005JD006980, 2006.
Mochida, M., Umemoto, N., Kawamura, K., Lim, H.-J., and Turpin, B. J.: Bimodal size distributions of various organic acids and fatty acids in the marine atmosphere: Influence of anthropogenic aerosols, Asian dusts, and sea spray off the coast of East Asia, J. Geophys. Res., 112, D15209, doi:10.1029/2006JD007773, 2007.
O'Dowd, C. D., Hameri, K., Makela, J. M., et al.: A dedicated study of New Particle Formation and Fate in the Coastal Environment (PARFORCE): Overview of objectives and achievements, J. Geophys. Res., 107(D19), 8108, doi:10.1029/2001JD000555, 2002.
Orsini, D. A., Ma, Y., Sullivan, A., Sierau, B., Baumann, K., and Weber, R. J.: Refinements to the particle–into-liquid sampler (PILS) for ground and airborne measurements of water soluble aerosol composition, Atmos. Environ., 37, 1243–1259, 2003.
Pang Y., Turpin, B. J., and Gundel, L. A.: On the importance of organic oxygen for understanding organic aerosol particles, Aerosol. Sci . Technol., 40, 128–133, 2006.
Raymond, T. M. and Pandis, S. N.: Cloud activation of single-component organic aerosol particles, J. Geophys. Res., 107(D24), 4787, doi:10.1029/2002JD002159, 2002.
Reade, L., Jennings, S. G., and McSweeney, G.: Cloud condensation nuclei measurements at Mace Head, Ireland, over the period 1994–2002, Atmos. Res., 82, 610–621, 2006.
Richter, A., Burrows, J. P., Nüb, C., Grainer, C., and Niemeier, U.: Increase in tropospheric nitrogen dioxide over China observed from space, Nature, 437, 129–132, 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(D20), 8070, doi:10.1029/2001JD000583, 2002.
Roberts, G. C., and Nenes, A.: A continuous-flow streamwise thermal gradient CCN chamber for atmospheric measurements, Aerosol Sci . Tech., 39, 206–221, 2005.
Sawa, Y., Tanimoto, H., Yonemura, S., Matsueda, H., Wada, A., Taguchi, S., Hayasaka, T., Tsuruta, H., Tohjima, Y., and Mukai, H.: Widespread pollution events of carbon monoxide observed over the western North Pacific during the EAREX 2005 campaign, J. Geophys. Res., 112, D22S26, doi:10.1029/2006JD008055, 2007.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, John Wiley & Sons, Inc, New York, 2006.
Simoneit, B. R. T., Kobayashi, M., Mochida, M., Kawamura, K., Lee, M., Lim, H.-J., Turpin, B. J., and Komazaki, Y.: Composition and major sources of organic compounds of aerosol particulate matter sampled during the ACE-Asia campaign, J. Geophys. Res., 109, D19S10, doi:10.1029/2004JD004598, 2004.
Sotiropoulou, R. E. P., Tagaris, E., Pilinis, C., Anttila, T., and Kulmala, M.: Modeling new particle formation during air pollution episodes: Impacts on aerosol and cloud condensation nuclei, Aerosol Sci . Tech., 40, 557-572, 2006.
Streets, D. G., Tsai, N. Y., Akimoto, H., and Oka, K.: Sulfur dioxide emissions in Asia in t he period 1985–1997, Atmos. Environ., 34, 4413–4424, 2000.
Sullivan, A. P., Weber, R. J., Clements, A. L., Turner, J. R., Bae, M. S., and Schauer, J. J.: A method for on-line measurement of water-soluble organic carbon in ambient aerosol particles: Results from an urban site, Geophys. Res. Lett., 31, L13105, doi:10.1029/2004GL019681, 2004.
Takegawa, N., Miyazaki, Y., Kondo, Y., Komazaki, Y., T. Miyakawa, T., Jimenez, J. L., Jayne, J. T., Worsnop, D. R., Allan, J., and Weber, R. J.: Characterization of an Aerodyne Aerosol Mass Spectrometer (AMS): Intercomparison with other aerosol instruments, Aerosol Sci. Tech., 39, 760–770, 2005.
Topping, D., Coe, H., McFiggans, Burgess, G. R., Allan, J., Alfarra, M. R., Bower, K., Choularton, T. W., Decesari, S., and Facchini, M. C.: Aerosol chemical characteristics from sampling conducted on the Island of Jeju Korea during ACE Asia, Atmos. Environ., 38, 2111–2123, 2004.
Twomey, S.: Pollution and the planetary albedo, Atmos. Environ., 8, 1251–1256, 1974.
Van Reken, 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(D20), 4633, doi:10.1029/2003JD003582, 2003.
Yum, S. S., Hudson, J. G., Song, K. Y., and Choi, B.-C.: Springtime cloud condensation nuclei concentrations on the west coast of Korea, Geophys. Res. Lett., 32, L09814, doi:10.1029/2005GL022641, 2005.
Yum, S. S., Roberts, G., Kim, J. H., Song, K., and Kim, D.: Submicron aerosol size distributions and cloud condensation nuclei concentrations measured at Gosan, Korea during the ABC-EAREX 2005, J. Geophys. Res., 112, D22S32, doi:10.1029/2006JD008212, 2007.
Wiedensohler, A.: Technical Note. An Approximation of the bipolar charge distribution for particles in the submicron size range, J. Aerosol Sci., 19, 387–389, 1988.