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	<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>7</volume_number>
		<issue_number>5</issue_number>
		<publication_year>2007</publication_year>
	</journal>
	<doi>10.5194/acp-7-1407-2007</doi>
	<article_url>http://www.atmos-chem-phys.net/7/1407/2007/</article_url>
	<abstract_html>http://www.atmos-chem-phys.net/7/1407/2007/acp-7-1407-2007.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys.net/7/1407/2007/acp-7-1407-2007.pdf</fulltext_pdf>
	<start_page>1407</start_page>
	<end_page>1413</end_page>
	<publication_date>2007-02-28</publication_date>
	<article_title content_type="html">Is aerosol formation in cirrus clouds possible?</article_title>
	<authors>
		<author numeration="1" affiliations="1,2">
			<name>J. Kazil</name>
			<email>jan.kazil@noaa.gov</email>
		</author>
		<author numeration="2" affiliations="1">
			<name>E. R. Lovejoy</name>
		</author>
		<author numeration="3" affiliations="3">
			<name>E. J. Jensen</name>
		</author>
		<author numeration="4" affiliations="4">
			<name>D. R. Hanson</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">NOAA Earth System Research Laboratory, Boulder, CO, USA</affiliation>
		<affiliation numeration="2" content_type="html">NRC Research Associateship Programs, Washington, D.C., USA</affiliation>
		<affiliation numeration="3" content_type="html">NASA Ames Research Center, Moffett Field, CA, USA</affiliation>
		<affiliation numeration="4" content_type="html">Augsburg College, Minneapolis, MN, USA</affiliation>
	</affiliations>
	<abstract content_type="html">The recent observation of ultrafine aerosol particles in cirrus clouds has
raised the question whether aerosol formation within cirrus clouds is possible,
and if so, what mechanisms are involved.
We have developed an aerosol parcel model of neutral and charged
H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;/H&lt;sub&gt;2&lt;/sub&gt;O aerosol processes, including nucleation from the gas
phase and loss onto cirrus ice particles.
Laboratory thermodynamic data for sulfuric acid uptake and loss by small neutral
and charged clusters are used, allowing for a reliable description of both
neutral and charged nucleation down to the very low temperatures occurring in
the upper troposphere and lower stratosphere.
The model implements a first order scheme for resolving the aerosol size
distribution within its geometric size sections, which efficiently suppresses
numerical diffusion.
We operate the model offline on trajectories generated with a detailed 1D cirrus
model which describes ice crystal nucleation, deposition growth, vertical
advection of ice crystals and water vapor, and ice crystal sedimentation.
In this paper we explore the possibility of aerosol formation within
non-convective cirrus clouds and draw conclusions for aerosol formation in anvil
cirrus.
We find that sulfate aerosol formation within cirrus clouds can proceed even at
high ice surface area concentrations, and depends strongly on the size of the
cirrus ice crystals and on the surface area concentration of preexisting aerosol
particles.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Arnold, F., Schneider, J., Gollinger, K., Schlager, H., Schulte, P., Hagen, D E., Whitefield, P D., and Velthoven, P v.: Observation of upper tropospheric sulfur dioxide- and acetone-pollution: Potential implications for hydroxyl radical and aerosol formation, Geophys. Res. Lett., 24(1), 57&amp;ndash;60, \doi10.1029/96GL03693, 1997. </reference>
		<reference numeration="2" content_type="text"> Brock, C A., Hamill, P., Wilson, J C., Jonsson, H H., and Chan, K R.: Particle formation in the upper tropical troposphere: a source of nuclei for the stratospheric aerosol, Science, 270, 1650&amp;ndash;1653, 1995. </reference>
		<reference numeration="3" content_type="text"> Carslaw, K S., Clegg, S L., and Brimblecombe, P.: A thermodynamic model of the system HCl-HNO&lt;sub&gt;3&lt;/sub&gt;-H2SO&lt;sub&gt;4&lt;/sub&gt;-H&lt;sub&gt;2&lt;/sub&gt;O, including solubilities of HBr, from &amp;lt;200 K to 328 K, J. Phys. Chem., 99, 11 557&amp;ndash;11 574, 1995. </reference>
		<reference numeration="4" content_type="text"> Clarke, A D., Varner, J L., Eisele, F., Mauldin, R L., Tanner, D., and Litchy, M.: Particle production in the remote marine tropospere: Cloud outflow and subsidence during ACE 1, J. Geophys. Res., 103, 16 397&amp;ndash;16 409, 1998. </reference>
		<reference numeration="5" content_type="text"> Eichkorn, S., Wilhelm, S., Aufmhoff, H., Wohlfrom, K H., and Arnold, F.: Cosmic ray-induced aerosol-formation: First observational evidence from aircraft-based ion mass spectrometer measurements in the upper troposphere, Geophys. Res. Lett., 29(14), \doi10.1029/2002GL015044, 2002. </reference>
		<reference numeration="6" content_type="text"> Fischer, H., de Reus, M., Traub, M., Williams, J., Lelieveld, J., de Gouw, J., Warneke, C., Schlager, H., Minikin, A., Scheele, R., and Siegmund, P.: Deep convective injection of boundary layer air into the lowermost stratosphere at midlatitudes, Atmos. Chem. Phys., 3, 739&amp;ndash;745, 2003. </reference>
		<reference numeration="7" content_type="text"> Froyd, K D. and Lovejoy, E R.: Experimental Thermodynamics of Cluster Ions Composed of H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; and H&lt;sub&gt;2&lt;/sub&gt;O. 1. Positive Ions, J. Phys. Chem. A, 107, 9800&amp;ndash;9811, 2003a. </reference>
		<reference numeration="8" content_type="text"> Froyd, K D. and Lovejoy, E R.: Experimental Thermodynamics of Cluster Ions Composed of H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; and H&lt;sub&gt;2&lt;/sub&gt;O. 2. Measurements and ab Initio Structures of Negative Ions, J. Phys. Chem. A, 107, 9812&amp;ndash;9824, 2003b. </reference>
		<reference numeration="9" content_type="text"> Fuchs, N A.: The Mechanics of Aerosols, Macmillan, 1964. </reference>
		<reference numeration="10" content_type="text"> Hagen, D E., Podzimek, J., and Trueblood, M B.: Upper-tropospheric aerosol sampled during project FIRE IFO II., J. Atmos. Sci., 52, 4196&amp;ndash;4209, 1995. </reference>
		<reference numeration="11" content_type="text"> Hanke, M., Umann, B., Uecker, J., Arnold, F., and Bunz, H.: Atmospheric measurements of gas-phase HNO&lt;sub&gt;3&lt;/sub&gt; and SO&lt;sub&gt;2&lt;/sub&gt; using chemical ionization mass spectrometry during the MINATROC field campaign 2000 on Monte Cimone, Atmos. Chem. Phys., 3, 417&amp;ndash;436, 2003. </reference>
		<reference numeration="12" content_type="text"> Hanson, D R.: Mass accommodation of H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; and CH&lt;sub&gt;3&lt;/sub&gt;SO&lt;sub&gt;3&lt;/sub&gt;H on water-sulfuric acid solutions from 6% to 97% RH, J. Phys. Chem. A, 109, 6919&amp;ndash;6927, \doi10.1021/jp0510443, 2005. </reference>
		<reference numeration="13" content_type="text"> Hanson, D R. and Lovejoy, E R.: Measurement of the thermodynamics of the hydrated dimer and trimer of sulfuric acid, J. Phys. Chem. A, 110, 9525&amp;ndash;9528, \doi10.1021/jp062844w, 2006. </reference>
		<reference numeration="14" content_type="text"> Jacobson, M Z.: Fundamentals of atmospheric modeling, Cambridge University Press, 1999. </reference>
		<reference numeration="15" content_type="text"> Jaeglé, L., Jacob, D J., Brune, W H., Faloona, I., Tan, D., Heikes, B G., Kondo, Y., Sachse, G W., Anderson, B., Gregory, G L., Singh, H B., Pueschel, R., Ferry, G., Blake, D R., and Shetter, R E.: Photochemistry of HO&lt;sub&gt;x&lt;/sub&gt; in the upper troposphere at northern midlatitudes, J. Geophys. Res., 105, 3877&amp;ndash;3892, \doi10.1029/1999JD901016, 2000. </reference>
		<reference numeration="16" content_type="text"> Jensen, E. and Pfister, L.: Transport and freeze-drying in the tropical tropopause layer, J. Geophys. Res., 109, D02207, \doi10.1029/2003JD004022, 2004. </reference>
		<reference numeration="17" content_type="text"> Kazil, J., Lovejoy, E R., Barth, M C., and O&apos;Brien, K.: Aerosol nucleation over oceans and the role of galactic cosmic rays, Atmos. Chem. Phys., 6, 4905&amp;ndash;4924, 2006. </reference>
		<reference numeration="18" content_type="text"> Kulmala, M., Dal Maso, M., Mäkelä, J M., Pirjola, L., Väkevä, M., Aalto, P., Miikkulainen, P., Hämeri, K., and O&apos;Dowd, C D.: On the formation, growth and composition of nucleation mode particles, Tellus B, 53, 479&amp;ndash;490, \doi10.1034/j.1600-0889.2001.530411.x, 2001. </reference>
		<reference numeration="19" content_type="text"> Kulmala, M., Reissell, A., Sipilä, M., Bonn, B., Ruuskanen, T M., Lehtinen, K E J., Kerminen, V.-M., and Ström, J.: Deep convective clouds as aerosol production engines: Role of insoluble organics, J. Geophys. Res., 111, 17 202, \doi10.1029/2005JD006963, 2006. </reference>
		<reference numeration="20" content_type="text"> Lee, S.-H., Reeves, J M., Wilson, J C., Hunton, D E., Viggiano, A A., Miller, T M., Ballenthin, J O., and Lait, L R.: Particle Formation by Ion Nucleation in the Upper Troposphere and Lower Stratosphere, Science, 301, 1886&amp;ndash;1889, 2003. </reference>
		<reference numeration="21" content_type="text"> Lee, S.-H., Wilson, J C., Baumgardner, D., Herman, R L., Weinstock, E M., LaFleur, B G., Kok, G., Anderson, B., Lawson, P., Baker, B., Strawa, A., Pittman, J V., Reeves, J M., and Bui, T P.: New particle formation observed in the tropical/subtropical cirrus clouds, J. Geophys. Res., 109, 20 209, \doi10.1029/2004JD005033, 2004. </reference>
		<reference numeration="22" content_type="text"> Liou, K.-N.: Influence of Cirrus Clouds on Weather and Climate Processes: A Global Perspective, Mon. Wea. Rev., 114, 1167&amp;ndash;1199, \doi10.1175/1520-0493, 1986. </reference>
		<reference numeration="23" content_type="text"> Lovejoy, E R., Hanson, D R., and Huey, L G.: Kinetics and products of the gas-phase reaction of SO&lt;sub&gt;3&lt;/sub&gt; with water, J. Phys. Chem., 100, 19 911&amp;ndash;19 916, \doi10.1021/jp962414d, 1996. </reference>
		<reference numeration="24" content_type="text"> Lovejoy, E R., Curtius, J., and Froyd, K D.: Atmospheric ion-induced nucleation of sulfuric acid and water, J. Geophys. Res., 109, D08204, \doi10.1029/2003JD004460, 2004. </reference>
		<reference numeration="25" content_type="text"> Minikin, A., Petzold, A., Ström, J., Krejci, R., Seifert, M., van Velthoven, P., Schlager, H., and Schumann, U.: Aircraft observations of the upper tropospheric fine particle aerosol in the Northern and Southern Hemispheres at midlatitudes, Geophys. Res. Lett., 30, 1503, \doi10.1029/2002GL016458, 2003. </reference>
		<reference numeration="26" content_type="text"> O&apos;Brien, K.: The theory of cosmic-ray and high-energy solar-particle transport in the atmosphere, in: The natural radiation environment VII, edited by: McLaughlin, J P., Simopoulos, E S., and Steinhäusler, F., Elsevier, seventh International Symposium on the Natural Radiation Environment, Rhodes, Greece, 20&amp;ndash;24 May 2002, 2005. </reference>
		<reference numeration="27" content_type="text"> Thornton, D C., Bandy, A R., Blomquist, B W., Davis, D D., and Talbot, R W.: Sulfur dioxide as a source of condensation nuclei in the upper troposphere of the Pacific Ocean, J. Geophys. Res., 101, 1883&amp;ndash;1890, 1996. </reference>
		<reference numeration="28" content_type="text"> Thornton, D C., Bandy, A R., Blomquist, B W., Driedger, A R., and Wade, T P.: Sulfur dioxide distribution over the Pacific Ocean 1991&amp;ndash;1996, J. Geophys. Res., 104, 5845&amp;ndash;5854, 1999. </reference>
		<reference numeration="29" content_type="text"> Wang, P.-H., Minnis, P., McCormick, M P., Kent, G S., and Skeens, K M.: A 6-year climatology of cloud occurrence frequency from Stratospheric Aerosol and Gas Experiment II observations (1985-1990), J. Geophys. Res., 101, 29 407&amp;ndash;29 430, \doi10.1029/96JD01780, 1996. </reference>
		<reference numeration="30" content_type="text"> Wylie, D P. and Menzel, W P.: Eight Years of High Cloud Statistics Using HIRS., J. Clim., 12, 170&amp;ndash;184, 1999. </reference>
	</references>
</article>

