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<article language="en">
	<journal>
		<journal_title>Atmospheric Chemistry and Physics Discussions</journal_title>
		<journal_url>www.atmos-chem-phys-discuss.net</journal_url>
		<issn>1680-7367</issn>
		<eissn>1680-7375</eissn>
		<volume_number>9</volume_number>
		<issue_number>5</issue_number>
		<publication_year>2009</publication_year>
	</journal>
	<doi>10.5194/acpd-9-20347-2009</doi>
	<article_url>http://www.atmos-chem-phys-discuss.net/9/20347/2009/</article_url>
	<abstract_html>http://www.atmos-chem-phys-discuss.net/9/20347/2009/acpd-9-20347-2009.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys-discuss.net/9/20347/2009/acpd-9-20347-2009.pdf</fulltext_pdf>
	<start_page>20347</start_page>
	<end_page>20369</end_page>
	<publication_date>2009-09-29</publication_date>
	<article_title content_type="html">Composition of cirrus-forming aerosols at the tropical tropopause</article_title>
	<authors>
		<author numeration="1" affiliations="1,2">
			<name>K. D. Froyd</name>
		</author>
		<author numeration="2" affiliations="1">
			<name>D. M. Murphy</name>
		</author>
		<author numeration="3" affiliations="3">
			<name>P. Lawson</name>
		</author>
		<author numeration="4" affiliations="4">
			<name>D. Baumgardner</name>
		</author>
		<author numeration="5" affiliations="5">
			<name>R. L. Herman</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">NOAA Earth System Research Laboratory, Chemical Sciences Division, Boulder, CO, USA</affiliation>
		<affiliation numeration="2" content_type="html">Cooperative Institute for Research in Environmental Science, University of Colorado, Boulder, CO, USA</affiliation>
		<affiliation numeration="3" content_type="html">SPEC Incorporated, Boulder, CO, USA</affiliation>
		<affiliation numeration="4" content_type="html">Universidad Nacional Autonoma de Mexico, Ciudad Universitaria, Mexico City, Mexico</affiliation>
		<affiliation numeration="5" content_type="html">Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, USA</affiliation>
	</affiliations>
	<abstract content_type="html">The composition of residual particles from evaporated cirrus ice
crystals near the tropical tropopause as well as unfrozen aerosols
were measured with a single particle mass spectrometer. Subvisible
cirrus residuals were predominantly composed of internal mixtures of
neutralized sulfate with organic material and were chemically
indistinguishable from unfrozen sulfate-organic aerosols. Ice
residuals were also similar in size to unfrozen aerosol. Heterogeneous
ice nuclei such as mineral dust were not enhanced in these subvisible
cirrus residuals. Biomass burning particles were depleted in the
residuals. Cloud probe measurements showing low cirrus ice crystal
number concentrations were inconsistent with conventional homogeneous
freezing. Recent laboratory studies provide heterogeneous nucleation
scenarios that may explain tropopause level subvisible cirrus
formation.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Abbatt,~J P D., Benz,~S., Cziczo,~D J., Kanji,~Z., Lohmann,~U., and Mohler,~O.: Solid ammonium sulfate aerosols as ice nuclei: A~pathway for cirrus cloud formation, Science, 313, 1770–1773, 2006. </reference>
		<reference numeration="2" content_type="text"> Alcala,~C M. and Dessler,~A E.: Observations of deep convection in the tropics using the Tropical Rainfall Measuring Mission (TRMM) precipitation radar, J. Geophys. Res.-Atmos., 107, 4792, doi:10.1029/2002JD002457, 2002. </reference>
		<reference numeration="3" content_type="text"> Archuleta, C. M., DeMott, P. J., and Kreidenweis, S. M.: Ice nucleation by surrogates for atmospheric mineral dust and mineral dust/sulfate particles at cirrus temperatures, Atmos. Chem. Phys., 5, 2617–2634, 2005. </reference>
		<reference numeration="4" content_type="text"> Baumgardner,~D., Jonsson,~H., Dawson,~W., O&apos;Connor,~D., and Newton,~R.: The cloud, aerosol and precipitation spectrometer: a~new instrument for cloud investigations, Atmos. Res., 59, 251–264, 2001. </reference>
		<reference numeration="5" content_type="text"> Comstock,~J M., Ackerman,~T P., and Mace,~G G.: Ground-based lidar and radar remote sensing of tropical cirrus clouds at Nauru Island: Cloud statistics and radiative impacts, J. Geophys. Res.-Atmos., 107, 4714, doi:10.1029/2002JD002203, 2002. </reference>
		<reference numeration="6" content_type="text"> Cziczo,~D J., DeMott,~P J., Brooks,~S D., Prenni,~A J., Thomson,~D S., Baumgardner,~D., Wilson,~J C., Kreidenweis,~S M., and Murphy,~D M.: Observations of organic species and atmospheric ice formation, Geophys. Res. Lett., 31, L12116, doi:10.1029/2004GL019822, 2004a. </reference>
		<reference numeration="7" content_type="text"> Cziczo,~D J., Murphy,~D M., Hudson,~P K., and Thomson,~D S.: Single particle measurements of the chemical composition of cirrus ice residue during CRYSTAL-FACE, J. Geophys. Res.-Atmos., 109, D04201, doi:10.1029/2003JD004032, 2004b. </reference>
		<reference numeration="8" content_type="text"> Cziczo,~D J., Froyd,~K D., Gallavardin,~S J., Mohler,~O., and Murphy,~D M.: Deactivation of ice nuclei due to atmospherically relevant surface coatings, Environ. Res. Lett., submitted, 2009. </reference>
		<reference numeration="9" content_type="text"> Dessler,~A E. and Yang,~P.: The distribution of tropical thin cirrus clouds inferred from terra MODIS data, J. Climate, 16, 1241–1247, 2003. </reference>
		<reference numeration="10" content_type="text"> Dessler,~A E., Palm,~S P., Hart,~W D., and Spinhirne,~J D.: Tropopause-level thin cirrus coverage revealed by ICESat$/$Geoscience Laser Altimeter System, J. Geophys. Res.-Atmos., 111, D08203, doi:10.1029/2005JD006586, 2006. </reference>
		<reference numeration="11" content_type="text"> Fortin,~T J., Shilling,~J E., and Tolbert,~M A.: Infrared spectroscopic study of the low-temperature phase behavior of ammonium sulfate, J. Geophys. Res.-Atmos., 107, 4088, doi:10.1029/2001JD000677, 2002. </reference>
		<reference numeration="12" content_type="text"> Froyd, K. D., Murphy, D. M., Sanford, T. J., Thomson, D. S., Wilson, J. C., Pfister, L., and Lait, L.: Aerosol composition of the tropical upper troposphere, Atmos. Chem. Phys., 9, 4363–4385, 2009. </reference>
		<reference numeration="13" content_type="text"> Fueglistaler,~S., Dessler,~A E., Dunkerton,~T J., Folkins,~I., Fu,~Q., and Mote,~P W.: Tropical tropopause layer, Rev. Geophys., 47, RG1004, doi:10.1029/2008RG000267, 2009. </reference>
		<reference numeration="14" content_type="text"> Gallavardin,~S J., Froyd,~K D., Lohmann,~U., Moehler,~O., Murphy,~D M., and Cziczo,~D J.: Single particle laser mass spectrometry applied to differential ice nucleation experiments at the AIDA chamber, Aerosol Sci. Tech., 42, 773–791, 2008. </reference>
		<reference numeration="15" content_type="text"> Garrett,~T J., Heymsfield,~A J., McGill,~M J., Ridley,~B A., Baumgardner,~D G., Bui,~T P., and Webster,~C R.: Convective generation of cirrus near the tropopause, J. Geophys. Res.-Atmos., 109, D21203, doi:10.1029/2004JD004952, 2004. </reference>
		<reference numeration="16" content_type="text"> Hartmann,~D L., Holton,~J R., and Fu,~Q.: The heat balance of the tropical tropopause, cirrus, and stratospheric dehydration, Geophys. Res. Lett., 28, 1969–1972, 2001. </reference>
		<reference numeration="17" content_type="text"> Hudson,~P K., Murphy,~D M., Cziczo,~D J., Thomson,~D S., de Gouw,~J A., Warneke,~C., Holloway,~J., Jost,~J R., and Hubler,~G.: Biomass-burning particle measurements: Characteristic composition and chemical processing, J. Geophys. Res.-Atmos., 109, D23S27, doi:10.1029/2003JD004398, 2004. </reference>
		<reference numeration="18" content_type="text"> Jensen,~E., and Pfister,~L.: Transport and freeze-drying in the tropical tropopause layer, J. Geophys. Res.-Atmos., 109, D02207, doi:10.1029/2003JD004022, 2004. </reference>
		<reference numeration="19" content_type="text"> Jensen,~E J., Toon,~O B., Pfister,~L., and Selkirk,~H B.: Dehydration of the upper troposphere and lower stratosphere by subvisible cirrus clouds near the tropical tropopause, Geophys. Res. Lett., 23, 825–828, 1996. </reference>
		<reference numeration="20" content_type="text"> Jensen,~E J., Toon,~O B., Vay,~S A., Ovarlez,~J., May,~R., Bui,~T P., Twohy,~C H., Gandrud,~B W., Pueschel,~R F., and Schumann,~U.: Prevalence of ice-supersaturated regions in the upper troposphere: Implications for optically thin ice cloud formation, J. Geophys. Res.-Atmos., 106, 17253–17266, 2001. </reference>
		<reference numeration="21" content_type="text"> Jensen, E. J., Smith, J. B., Pfister, L., Pittman, J. V., Weinstock, E. M., Sayres, D. S., Herman, R. L., Troy, R. F., Rosenlof, K., Thompson, T. L., Fridlind, A. M., Hudson, P. K., Cziczo, D. J., Heymsfield, A. J., Schmitt, C., and Wilson, J. C.: Ice supersaturations exceeding 100% at the cold tropical tropopause: implications for cirrus formation and dehydration, Atmos. Chem. Phys., 5, 851–862, 2005. </reference>
		<reference numeration="22" content_type="text"> Jensen, E. J., Pfister, L., Bui, T. V., Lawson, P., Baker, B., Mo, Q., Baumgardner, D., Weinstock, E. M., Smith, J. B., Moyer, E. J., Hanisco, T. F., Sayres, D. S., Clair, J. M. St., Alexander, M. J., Toon, O. B., and Smith, J. A.: Formation of large (&amp;#x2243;100 μm) ice crystals near the tropical tropopause, Atmos. Chem. Phys., 8, 1621–1633, 2008. </reference>
		<reference numeration="23" content_type="text"> Jensen, E. J., Lawson, P., Baker, B., Pilson, B., Mo, Q., Heymsfield, A. J., Bansemer, A., Bui, T. P., McGill, M., Hlavka, D., Heymsfield, G., Platnick, S., Arnold, G. T., and Tanelli, S.: On the importance of small ice crystals in tropical anvil cirrus, Atmos. Chem. Phys., 9, 5519–5537, 2009a. </reference>
		<reference numeration="24" content_type="text"> Jensen,~E J., Pfister,~L., Bui,~T.-P., Lawson,~P., and Baumgardner,~D.: Ice nucleation and cloud microphysical properties in tropical tropopause layer cirrus, Atmos. Chem. Phys., submitted, 2009b. </reference>
		<reference numeration="25" content_type="text"> Kärcher, B.: Properties of subvisible cirrus clouds formed by homogeneous freezing, Atmos. Chem. Phys., 2, 161–170, 2002. </reference>
		<reference numeration="26" content_type="text"> Karcher,~B.: Cirrus clouds in the tropical tropopause layer: Role of heterogeneous ice nuclei, Geophys. Res. Lett., 31, L12101, doi:10.1029/2004GL019774, 2004. </reference>
		<reference numeration="27" content_type="text"> Koop,~T., Luo,~B P., Tsias,~A., and Peter,~T.: Water activity as the determinant for homogeneous ice nucleation in aqueous solutions, Nature, 406, 611–614, 2000. </reference>
		<reference numeration="28" content_type="text"> Krämer, M., Schiller, C., Afchine, A., Bauer, R., Gensch, I., Mangold, A., Schlicht, S., Spelten, N., Sitnikov, N., Borrmann, S., de Reus, M., and Spichtinger, P.: Ice supersaturations and cirrus cloud crystal numbers, Atmos. Chem. Phys., 9, 3505–3522, 2009. </reference>
		<reference numeration="29" content_type="text"> Lawson,~R P., O&apos;Connor,~D., Zmarzly,~P., Weaver,~K., Baker,~B., Mo,~Q X., and Jonsson,~H.: The 2D-S (Stereo) probe: Design and preliminary tests of a~new airborne, high-speed, high-resolution particle Imaging probe, J. Atmos. Ocean. Tech., 23, 1462–1477, 2006. </reference>
		<reference numeration="30" content_type="text"> Lawson, R. P., Pilson, B., Baker, B., Mo, Q., Jensen, E., Pfister, L., and Bui, P.: Aircraft measurements of microphysical properties of subvisible cirrus in the tropical tropopause layer, Atmos. Chem. Phys., 8, 1609–1620, 2008. </reference>
		<reference numeration="31" content_type="text"> Liu,~C T.: Geographical and seasonal distribution of tropical tropopause thin clouds and their relation to deep convection and water vapor viewed from satellite measurements, J. Geophys. Res.-Atmos., 112, D09205, doi:10.1029/2006JD007479, 2007. </reference>
		<reference numeration="32" content_type="text"> Luo,~B P., Peter,~T., Fueglistaler,~S., Wernli,~H., Wirth,~M., Kiemle,~C., Flentje,~H., Yushkov,~V A., Khattatov,~V., Rudakov,~V., Thomas,~A., Borrmann,~S., Toci,~G., Mazzinghi,~P., Beuermann,~J., Schiller,~C., Cairo,~F., Di Donfrancesco,~G., Adriani,~A., Volk,~C M., Strom,~J., Noone,~K., Mitev,~V., MacKenzie,~R A., Carslaw,~K S., Trautmann,~T., Santacesaria,~V., and Stefanutti,~L.: Dehydration potential of ultrathin clouds at the tropical tropopause, Geophys. Res. Lett., 30, 1557, doi:10.1029/2002GL016737, 2003. </reference>
		<reference numeration="33" content_type="text"> Massie,~S., Gettelman,~A., Randel,~W., and Baumgardner,~D.: Distribution of tropical cirrus in relation to convection, J. Geophys. Res.-Atmos., 107, 4591, doi:10.1029/2001JD001293, 2002. </reference>
		<reference numeration="34" content_type="text"> May,~R D.: Open-path, near-infrared tunable diode laser spectrometer for atmospheric measurements of \chemH_2O, J. Geophys. Res.-Atmos., 103, 19161–19172, 1998. </reference>
		<reference numeration="35" content_type="text"> McFarquhar,~G M., Heymsfield,~A J., Spinhirne,~J., and Hart,~B.: Thin and subvisual tropopause tropical cirrus: Observations and radiative impacts, J. Atmos. Sci., 57, 1841–1853, 2000. </reference>
		<reference numeration="36" content_type="text"> Mohler,~O., Benz,~S., Saathoff,~H., Schnaiter,~M., Wagner,~R., Schneider,~J., Walter,~S., Ebert,~V., and Wagner,~S.: The effect of organic coating on the heterogeneous ice nucleation efficiency of mineral dust aerosols, Environ. Res. Lett., 3, 025007, doi:10.1088/1748-9326/3/2/025007, 2008. </reference>
		<reference numeration="37" content_type="text"> Murphy,~D M., Cziczo,~D J., Hudson,~P K., Thomson,~D S., Wilson,~J C., Kojima,~T., and Buseck,~P R.: Particle generation and resuspension in aircraft inlets when flying in clouds, Aerosol Sci. Tech., 38, 400–408, 2004. </reference>
		<reference numeration="38" content_type="text"> Murphy,~D M. and Koop,~T.: Review of the vapour pressures of ice and supercooled water for atmospheric applications, Q. J. Roy. Meteor. Soc., 131, 1539–1565, 2005. </reference>
		<reference numeration="39" content_type="text"> 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.-Atmos., 111, D23S32, doi:10.1029/2006JD007340, 2006a. </reference>
		<reference numeration="40" content_type="text"> Murphy,~D M., Hudson,~P K., Thomson,~D S., Sheridan,~P J., and Wilson,~J C.: Observations of mercury-containing aerosols, Environ. Sci. Technol., 40, 3163–3167, 2006b. </reference>
		<reference numeration="41" content_type="text"> Murray, B. J.: Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets, Atmos. Chem. Phys., 8, 5423–5433, 2008. </reference>
		<reference numeration="42" content_type="text"> Murray,~B J., Wilson,~T W., Dobbie,~S., Cui,~Z., Möhler,~O., Schnaiter,~M., Wagner,~R., Benz,~S., Niemand,~M., Saathoff,~H., Ebert,~V., Wagner,~S., and Kärcher,~B.: Glassy aerosols modify tropical tropopause cirrus and humidity, in preparation, 2009. </reference>
		<reference numeration="43" content_type="text"> Park, S., Jiménez, R., Daube, B. C., Pfister, L., Conway, T. J., Gottlieb, E. W., Chow, V. Y., Curran, D. J., Matross, D. M., Bright, A., Atlas, E. L., Bui, T. P., Gao, R.-S., Twohy, C. H., and Wofsy, S. C.: The CO&lt;sub&gt;2&lt;/sub&gt; tracer clock for the Tropical Tropopause Layer, Atmos. Chem. Phys., 7, 3989–4000, 2007. </reference>
		<reference numeration="44" content_type="text"> Pfister,~L., Selkirk,~H B., Jensen,~E J., Schoeberl,~M R., Toon,~O B., Browell,~E V., Grant,~W B., Gary,~B., Mahoney,~M J., Bui,~T V., and Hintsa,~E.: Aircraft observations of thin cirrus clouds near the tropical tropopause, J. Geophys. Res.-Atmos., 106, 9765–9786, 2001. </reference>
		<reference numeration="45" content_type="text"> Pruppacher,~H R. and Klett,~J D.: Microphysics of clouds and precipitation, 2nd rev. ed., Atmospheric and oceanographic sciences library, vol 18, Kluwer Academic Publishers, Dordrecht, Boston, 954~pp., 1997. </reference>
		<reference numeration="46" content_type="text"> Schwartz,~C. and Mace,~G G.: Co-occurrence statistics of tropical tropopause layer cirrus with lower cloud layers as derived from CloudSat and Calipso data, in preparation, 2009. </reference>
		<reference numeration="47" content_type="text"> Thomson,~D S., Schein,~M E., and Murphy,~D M.: Particle analysis by laser mass spectrometry WB-57F instrument overview, Aerosol Sci. Tech., 33, 153–169, 2000. </reference>
		<reference numeration="48" content_type="text"> Troy,~R F.: Field studies of ice supersaturations in the tropical tropopause layer, Ph.D. Thesis, Geophysics and Space Physics, University of California at Los Angeles, 2007. </reference>
		<reference numeration="49" content_type="text"> Zobrist, B., Marcolli, C., Pedernera, D. A., and Koop, T.: Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 8, 5221–5244, 2008. </reference>
	</references>
</article>

