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<article language="en">
	<journal>
		<journal_title>Atmospheric Chemistry and Physics</journal_title>
		<journal_url>www.atmos-chem-phys.net</journal_url>
		<issn>1680-7316</issn>
		<eissn>1680-7324</eissn>
		<volume_number>9</volume_number>
		<issue_number>7</issue_number>
		<publication_year>2009</publication_year>
	</journal>
	<doi>10.5194/acp-9-2517-2009</doi>
	<article_url>http://www.atmos-chem-phys.net/9/2517/2009/</article_url>
	<abstract_html>http://www.atmos-chem-phys.net/9/2517/2009/acp-9-2517-2009.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys.net/9/2517/2009/acp-9-2517-2009.pdf</fulltext_pdf>
	<start_page>2517</start_page>
	<end_page>2532</end_page>
	<publication_date>2009-04-07</publication_date>
	<article_title content_type="html">Parameterization of cloud droplet formation for global and regional models: including adsorption activation from insoluble CCN</article_title>
	<authors>
		<author numeration="1" affiliations="1">
			<name>P. Kumar</name>
		</author>
		<author numeration="2" affiliations="2">
			<name>I. N. Sokolik</name>
		</author>
		<author numeration="3" affiliations="1,2">
			<name>A. Nenes</name>
			<email>nenes@eas.gatech.edu</email>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA</affiliation>
		<affiliation numeration="2" content_type="html">School of Earth and Atmospheric Sciences, Georgia Institute of Technology Atlanta, GA, 30332, USA</affiliation>
	</affiliations>
	<abstract content_type="html">Dust and black carbon aerosol have long been known to exert potentially
important and diverse impacts on cloud droplet formation. Most studies to
date focus on the soluble fraction of these particles, and overlook
interactions of the insoluble fraction with water vapor (even if known to be
hydrophilic). To address this gap, we developed a new parameterization
that considers cloud droplet formation within an ascending air
parcel containing insoluble (but wettable) particles externally mixed with
aerosol containing an appreciable soluble fraction. Activation of particles
with a soluble fraction is described through well-established Köhler
theory, while the activation of hydrophilic insoluble particles is treated
by &quot;adsorption-activation&quot; theory. In the latter, water vapor is adsorbed
onto insoluble particles, the activity of which is described by a multilayer
Frenkel-Halsey-Hill (FHH) adsorption isotherm modified to account for
particle curvature. We further develop FHH activation theory to &lt;i&gt;i&lt;/i&gt;) find
combinations of the adsorption parameters &lt;i&gt;A&lt;/i&gt;&lt;sub&gt;FHH&lt;/sub&gt;, &lt;i&gt;B&lt;/i&gt;&lt;sub&gt;FHH&lt;/sub&gt; which yield
atmospherically-relevant behavior, and, &lt;i&gt;ii&lt;/i&gt;) express activation properties
(critical supersaturation) that follow a simple power law with respect to
dry particle diameter.
&lt;br&gt;&lt;br&gt;
The new parameterization is tested by
comparing the parameterized cloud droplet number concentration against
predictions with a detailed numerical cloud model, considering a wide range
of particle populations, cloud updraft conditions, water vapor condensation
coefficient and FHH adsorption isotherm characteristics. The agreement
between parameterization and parcel model is excellent, with an average
error of 10% and &lt;i&gt;R&lt;/i&gt;&lt;sup&gt;2&lt;/sup&gt;~0.98. A preliminary sensitivity study
suggests that the sublinear response of droplet number to Köhler
particle concentration is not as strong for FHH particles.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Abdul-Razzak, H. and Ghan, S. J.: A parameterization of aerosol activation: 2. Multiple aerosol types, J. Geophys. Res., 105(D6), 6837–6844, 2000. </reference>
		<reference numeration="2" content_type="text"> Abdul-Razzak, H., Ghan, S. J., and Rivera-Carpio, C.: A parameterization of aerosol activation: 1. Single aerosol type, J. Geophys. Res., 103(D6), 6123–6131, 1998. </reference>
		<reference numeration="3" content_type="text"> Albrecht, B. A.: Aerosols, cloud microphysics, and fractional cloudiness, Science, 245, 1227–1230, 1989. </reference>
		<reference numeration="4" content_type="text"> Asa-Awuku, A. and Nenes, A.: The effect of solute dissolution kinetics on cloud droplet formation: Extended Köhler theory, J. Geophys. Res., 112, D22201, doi:10.1029/2005JD006934, 2007. </reference>
		<reference numeration="5" content_type="text"> Barahona, D. and Nenes, A.: Parameterization of cloud droplet formation in large-scale models: Including effects of entrainment, J. Geophys. Res., 112, D16206, doi:10.1029/2007JD008473, 2007. </reference>
		<reference numeration="6" content_type="text"> Boucher, O. and Lohmann, U.: The sulfate-CCN-cloud albedo effect: A sensitivity study with 2 general circulation models, Tellus, Ser. B, 47, 281–300, 1995. </reference>
		<reference numeration="7" content_type="text"> Brunauer, S., Emmett, P. H., and Teller, E.: Adsorption of gases in multimolecular layers, J. Am. Chem. Soc., 60(2), 309–319, 1938. </reference>
		<reference numeration="8" content_type="text"> Clarke, A. D., Shinozuka, Y., Kapustin, V. N., Howell, S., Huebert, B., Doherty, S., Anderson, T., Covert, D., Anderson, J., Hua, X., Moore II, K. G., McNaughton, C., Carmichael, G., and Weber, R.: Size distributions and mixtures of dust and black carbon aerosol in Asian outflow: Physiochemistry and optical properties, J. Geophys. Res., 109, D15S09, doi:10.1029/2003JD004378, 2004. </reference>
		<reference numeration="9" content_type="text"> Cohard, J.-M., Pinty, J.-P., and Suhre, K.: On the parameterization of activation spectra from cloud condensation nuclei microphysical properties, J. Geophys. Res., 105(D9), 11753–11766, 2000. </reference>
		<reference numeration="10" content_type="text"> Conant, W. C., Van Reken, T. M., Rissman, T. A., Varutbangkul, V., Jonsson, H. H., Nenes, A., Jimenez, J. L., Delia, A. E., Bahreini, R., Roberts, G. C., Flagan, R. C., and Seinfeld, J. H.: Aerosol-cloud drop concentration closure in warm cumulus, J. Geophys. Res., 109, D13204, doi:10.1029/2003JD004324, 2004. </reference>
		<reference numeration="11" content_type="text"> D&apos;Almeida, G. A.: On the variability of desert aerosol radiative characteristics, J. Geophys. Res., 92, 3017–3027, 1987. </reference>
		<reference numeration="12" content_type="text"> Feingold, G. and Chuang, P.: Analysis of the Influence of Film-Forming compounds on Droplet Growth: Implications for Cloud Microphysical Processes and Climate, J. Atmos. Sci., 59, 2006–2018, 2002. </reference>
		<reference numeration="13" content_type="text"> Feingold, G. and Heymsfield, A. J.: Parameterization of condensational growth of droplets for use in general circulation models, J. Atmos. Sci, 49, 2325–2342, 1992. </reference>
		<reference numeration="14" content_type="text"> Fletcher, N. H.: Size effect in heterogeneous nucleation, J. Chem. Phys., 29, 572–576, 1958. </reference>
		<reference numeration="15" content_type="text"> Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D. W., Haywood, J., Lean, J., Lowe, D. C., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., and Van Dorland, R.: Changes in Atmospheric Constituents and in Radiative Forcing, in: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., and Miller, H. L., Cambridge University Press, Cambridge, UK and New York, NY, USA, 129–234, 2007. </reference>
		<reference numeration="16" content_type="text"> Fountoukis, C. and Nenes, A.: Continued development of a cloud droplet formation parameterization for global climate models, J. Geophys. Res., 110, D11212, doi:10.1029/2004JD005591, 2005. </reference>
		<reference numeration="17" content_type="text"> Fukuta, N. and Walter, L. A.: Kinetics of hydrometer growth from the vapor; spherical model, J. Atmos. Sci., 27, 1160–1172, 1970. </reference>
		<reference numeration="18" content_type="text"> Ghan, S., G. Guzman, and H. Abdul-Razzak: Competition between sea-salt and sulfate particles as cloud condensation nuclei, J. Atmos. Sci., 55, 3340–3347, 1998. </reference>
		<reference numeration="19" content_type="text"> Gultepe, I. and Isaac, G. A.: The relationship between cloud droplet and aerosol number concentrations for climate models, Int. J. Climatol., 16, 941–946, 1996. </reference>
		<reference numeration="20" content_type="text"> Henson, B. F.: An adsorption model of insoluble particle activation: Application to black carbon, J. Geophys. Res., 112, D24S16, doi:10.1029/2007JD008549, 2007. </reference>
		<reference numeration="21" content_type="text"> Hess, M., Koepke, P., and Schult, I.: Optical Properties of Aerosols and Clouds: The Software Package OPAC, B. Am. Meteor. Soc., 79, 831–844, 1998. </reference>
		<reference numeration="22" content_type="text"> Jeong, G.-R. and Sokolik, I. N.: Effect of mineral dust aerosols on photolysis rates in clean and polluted marine environments, J. Geophys. Res., 112, D21308, doi:10.1029/2007JD008442, 2007. </reference>
		<reference numeration="23" content_type="text"> Khvorostyanov, V. I. and Curry, J. A.: Refinements to the Köhler&apos;s theory of aerosol equilibrium radii, size spectra and droplet activation: Effects of humidity and insoluble fraction, J. Geophys. Res., 112, D05206, doi:10.1029/2006JD007672, 2007. </reference>
		<reference numeration="24" content_type="text"> Köhler, H.: The nucleus in and the growth of hygroscopic droplets, Trans. Faraday Soc., 32(2), 1152–1161, 1936. </reference>
		<reference numeration="25" content_type="text"> Langmuir, J.: The constitution and fundamental properties of solids and liquids. Part I. Solids, J. Am. Chem. Soc., 38, 2221–2295, 1916. </reference>
		<reference numeration="26" content_type="text"> Lowell, S., Shields, J. E., Thomas, M. A., and Thommes, M.: Characterization of Porous Solids and Powders: Surface Area, Pore Size and Density, Kluwer Academic Publishers, The Netherlands, 24–26, 2004. </reference>
		<reference numeration="27" content_type="text"> Meskhidze, N., Nenes, A., Conant, W. C., and Seinfeld, J. H.: Evaluation of a new cloud droplet activation parameterization with in situ data from CRYSTAL-FACE and CSTRIPE, J. Geophys. Res., 110, D16202, doi:10.1029/2004JD005703, 2005. </reference>
		<reference numeration="28" content_type="text"> Ming, Y., Ramaswamy, V., Donner, L. J., and Phillips, V. T. J.: A new parameterization of cloud droplet activation applicable to general circulation models, J. Atmos. Sci., 63, 1348–1356, 2006. </reference>
		<reference numeration="29" content_type="text"> Nenes, A., Ghan, S. J., Abdul-Razzak, H., Chuang, P. Y., and Seinfeld, J. H.: Kinetic limitations on cloud droplet formation and impact on cloud albedo, Tellus, Ser. B, 53, 133–149, 2001. </reference>
		<reference numeration="30" content_type="text"> Nenes, A. and Seinfeld, J. H.: Parameterization of cloud droplet formation in global climate models, J. Geophys. Res., 108(D14), 4415, doi:10.1029/2002JD002911, 2003. </reference>
		<reference numeration="31" content_type="text"> Nenes, A., Charlson, R. J., Facchini, M. C., Kulmala, M., Laaksonen, A., and Seinfeld, J. H.: Can chemical effects on cloud droplet number rival the first indirect effect?, Geophys. Res. Lett., 29(17), 1848, doi:10.1029/2002GL015295, 2002. </reference>
		<reference numeration="32" content_type="text"> Peng, Y., Lohmann, U., and Leaitch, W. R.: Importance of vertical velocity variations in the cloud droplet nucleation process of marine stratocumulus, J. Geophys. Res., 110, D21213, doi:10.1029/2004JD004922, 2005. </reference>
		<reference numeration="33" content_type="text"> Pontikis, C. A., Rigaud, A., and Hicks, E. M.: Entrainment and mixing as related to the microphysical properties of shallow warm cumulus clouds, J. Atmos. Sci., 44, 2150–2165, 1987. </reference>
		<reference numeration="34" content_type="text"> Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, John Wiley, New York, USA, 767–773, 1998. </reference>
		<reference numeration="35" content_type="text"> Seisel, S., Pashkova, A., Lian, Y., and Zellner, R.: Water uptake on mineral dust and soot: A fundamental view of hydrophilicity of atmospheric particles?, Faraday Discuss., 130, 437–451, 2005. </reference>
		<reference numeration="36" content_type="text"> Sorjamaa, R. and Laaksonen, A.: The effect of H&lt;sub&gt;2&lt;/sub&gt;O adsorption on cloud drop activation of insoluble particles: a theoretical framework, Atmos. Chem. Phys., 7, 6175–6180, 2007 </reference>
		<reference numeration="37" content_type="text"> Twohy, C. H., Kreidenweis, S. M., Eidhammer, T., Browell, E. V., Heymsfield, A. J., Bansemer, A. R., Anderson, B. E., Chen, G., Ismail, S., DeMott, P. J., and Van Den Heever, S. C.: Saharan dust particles nucleate droplets in eastern Atlantic clouds, Geophys. Res. Lett., 36, 1–6, 2009. </reference>
		<reference numeration="38" content_type="text"> 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, 1959. </reference>
		<reference numeration="39" content_type="text"> Twomey, S.: Pollution and the planetary albedo, Atmos. Environ., 8, 1251–1256, 1974. </reference>
		<reference numeration="40" content_type="text"> Wexler, A. S. and Ge, Z. Z.: Hydrophobic particles can activate at lower relative humidity than slightly hygroscopic ones: a Köhler theory incorporating surface fixed charge, J. Geophys. Res., 103(D6), 6083–6088, 1998. </reference>
		<reference numeration="41" content_type="text"> Whitby, K. T.: The physical characteristics of sulfur aerosols, Atmos. Environ., 12, 135–139, 1978. </reference>
		<reference numeration="42" content_type="text"> Wiegner, M., Gasteiger, J., Kandler, K., Weinzierl, B., Rasp, K., Esselborn, M., Freudenthaler, V., Heese, B., Toledano, C., Tesche, M., and Althausen, D.: Numerical simulations of optical properties of Saharan dust aerosols with emphasis on linear depolarization ratio, Tellus, 61B, 180–194, 2009. </reference>
	</references>
</article>

