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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>9</volume_number>
		<issue_number>2</issue_number>
		<publication_year>2009</publication_year>
	</journal>
	<doi>10.5194/acp-9-721-2009</doi>
	<article_url>http://www.atmos-chem-phys.net/9/721/2009/</article_url>
	<abstract_html>http://www.atmos-chem-phys.net/9/721/2009/acp-9-721-2009.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys.net/9/721/2009/acp-9-721-2009.pdf</fulltext_pdf>
	<start_page>721</start_page>
	<end_page>732</end_page>
	<publication_date>2009-01-28</publication_date>
	<article_title content_type="html">Analysis of the hygroscopic and volatile properties of ammonium sulphate seeded and unseeded SOA particles</article_title>
	<authors>
		<author numeration="1" affiliations="1,5">
			<name>N. K. Meyer</name>
		</author>
		<author numeration="2" affiliations="2">
			<name>J. Duplissy</name>
		</author>
		<author numeration="3" affiliations="2">
			<name>M. Gysel</name>
		</author>
		<author numeration="4" affiliations="2">
			<name>A. Metzger</name>
		</author>
		<author numeration="5" affiliations="2">
			<name>J. Dommen</name>
		</author>
		<author numeration="6" affiliations="2">
			<name>E. Weingartner</name>
		</author>
		<author numeration="7" affiliations="2">
			<name>M. R. Alfarra</name>
		</author>
		<author numeration="8" affiliations="2">
			<name>A. S. H. Prevot</name>
		</author>
		<author numeration="9" affiliations="1">
			<name>C. Fletcher</name>
		</author>
		<author numeration="10" affiliations="3">
			<name>N. Good</name>
		</author>
		<author numeration="11" affiliations="3">
			<name>G. McFiggans</name>
		</author>
		<author numeration="12" affiliations="4">
			<name>Å. M. Jonsson</name>
		</author>
		<author numeration="13" affiliations="4">
			<name>M. Hallquist</name>
		</author>
		<author numeration="14" affiliations="2">
			<name>U. Baltensperger</name>
		</author>
		<author numeration="15" affiliations="1">
			<name>Z. D. Ristovski</name>
			<email>z.ristovski@qut.edu.au</email>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">International Laboratory for Air Quality and Health, Queensland University of Technology, Brisbane QLD 4000, Australia</affiliation>
		<affiliation numeration="2" content_type="html">Laboratory of Atmospheric Chemistry, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland</affiliation>
		<affiliation numeration="3" content_type="html">Centre for Atmospheric Sciences, School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, M60 1QD, UK</affiliation>
		<affiliation numeration="4" content_type="html">Department of Chemistry, Atmospheric Science, University of Gothenburg, 412 96 Gothenburg, Sweden</affiliation>
		<affiliation numeration="5" content_type="html">now at: IAST, FHNW University of Applied Sciences, Windisch 5210, Switzerland</affiliation>
	</affiliations>
	<abstract content_type="html">The volatile and hygroscopic properties of ammonium sulphate seeded and
unseeded secondary organic aerosol (SOA) derived from the photo-oxidation
of atmospherically relevant concentrations of α-pinene were studied.
The seed particles were electrospray generated ammonium sulphate
((NH4)&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;) having diameters of approximately 33 nm with a
quasi-mono-disperse size distribution (geometric standard deviation &amp;sigma;&lt;sub&gt;g&lt;/sub&gt;=1.3).
The volatile and hygroscopic properties of both seeded and
unseeded SOA were simultaneously measured with a VH-TDMA (volatility –
hygroscopicity tandem differential mobility analyzer). VH-TDMA
measurements of unseeded SOA show a decrease in the hygroscopic growth (HGF)
factor for increased volatilisation temperatures such that the more volatile
compounds appear to be more hygroscopic. This is opposite to the expected
preferential evaporation of more volatile but less hygroscopic material, but
could also be due to enhanced oligomerisation occurring at the higher
temperature in the thermodenuder. In addition, HGF measurements of seeded
SOA were measured as a function of time at two relative humidities, below
(RH 75%) and above (RH 85%) the deliquescence relative humidity (DRH)
of the pure ammonium sulphate seeds. As these measurements were conducted
during the onset phase of photo-oxidation, during particle growth, they
enabled us to find the dependence of the HGF as a function of the volume
fraction of the SOA coating. HGF&apos;s measured at RH of 85% showed a
continuous decrease as the SOA coating thickness increased. The measured
growth factors show good agreements with ZSR predictions indicating that, at
these RH values, there are only minor solute-solute interactions. At 75%
RH, as the SOA fraction increased, a rapid increase in the HGF was observed
indicating that an increasing fraction of the (NH&lt;sub&gt;4&lt;/sub&gt;)&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; is
subject to a phase transition, going into solution, with an increasing
volume fraction of SOA. To our knowledge this is the first time that SOA
derived from photo-oxidised α-pinene has been shown to affect the
equilibrium water content of inorganic aerosols below their DRH. For SOA
volume fractions above ~0.3 the measured growth factor followed
roughly parallel to the ZSR prediction based on fully dissolved
(NH&lt;sub&gt;4&lt;/sub&gt;)&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; although with a small difference that was just
larger than the error estimate. Both incomplete dissolution and negative
solute-solute interactions could be responsible for the lower HGF observed
compared to the ZSR predictions.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Alfarra, M. R., Paulsen, D., Gysel, M., Garforth, A. A., Dommen, J., Prevot, A. S. H., Worsnop, D. R., Baltensperger, U., and Coe, H.: A mass spectrometric study of secondary organic aerosols formed from the photooxidation of anthropogenic and biogenic precursors in a reaction chamber., Atmos. Chem. Phys., 6, 5279–5293, 2006. </reference>
		<reference numeration="2" content_type="text"> Andrews, E. and Larson, S. M.: Effect of surfactant layers on the size changes of aerosol particles as a function of relative humidity, Environ. Sci. Technol., 27, 857–865, 1993. </reference>
		<reference numeration="3" content_type="text"> Canagaratna, M. R., Jayne, J. T., Jimenez, J. L., Allan, J. D., Alfarra, M. R., Zhang, Q., Onasch, T. B., Drewnick, F., Coe, H., Middlebrook, A., Delia, A., Williams, L. R., Trimborn, A. M., Northway, M. J., Kolb, C. E., Davidovits, P., and Worsnop, D. R.: Chemical and microphysical characterization of ambient aerosols with the aerosol mass spectrometer, Mass. Spectrom. Rev., 26, 185–222, 2007. </reference>
		<reference numeration="4" content_type="text"> Choi, M. Y. and Chan, C. K.: The effects of organic species on the hygroscopic behaviors of inorganic aerosols, Environ. Sci. Technol., 36, 2422–2428, 2002. </reference>
		<reference numeration="5" content_type="text"> Chow, J. C., Watson, J. G., Fujita, E. M., Lu, Z. Q., Lawson, D. R., and Ashbaugh, L. L.: Temporal and spatial variations of PM(2.5) and PM(10) aerosol in the Southern California Air-Quality Study, Atmos. Environ., 28, 2061–2080, 1994. </reference>
		<reference numeration="6" content_type="text"> Chuang, P. Y.: Measurement of the time scale of hygroscopic growth for atmospheric aerosols, J. Geophys. Res. D, Atmosphere, 108, 4282, doi:10.1029/2002JD002757, 2003. </reference>
		<reference numeration="7" content_type="text"> Clegg, S. L. and Seinfeld, J. H.: Thermodynamic models of aqueous solutions containing inorganic electrolytes and dicarboxylic acids at 298.15 K. 2. Systems including dissociation function equilibria, J. Phys. Chem, 110, 5718–5734, 2006. </reference>
		<reference numeration="8" content_type="text"> Cocker III, D. R., Clegg, S. L., Flagan, R. C., and Seinfeld, J. H.: The effect of water on gas-particle partitioning of secondary organic aerosol. Part I: [alpha]-pinene/ozone system, Atmos. Environ., 35, 6049–6072, 2001. </reference>
		<reference numeration="9" content_type="text"> Cruz, C. N. and Pandis, S. N.: The effect of organic coatings on the cloud condensation nuclei activation of inorganic atmospheric aerosol, J. Geophys. Res., 103, 13111–13123, 1998. </reference>
		<reference numeration="10" content_type="text"> Cruz, C. N. and Pandis, S. N.: Deliquescence and hygroscopic growth of mixed inorganic-organic atmospheric aerosol, Environ. Sci. Technol., 34, 4313–4319, 2000. </reference>
		<reference numeration="11" content_type="text"> Dick, W. D., Saxena, P., and McMurry, P. H.: Estimation of water uptake by organic compounds in submicron aerosols measured during the southeastern aerosol and visibility study, J. Geophys. Res, 105, 1471–1479, 2000. </reference>
		<reference numeration="12" content_type="text"> Duce, R. A., Mohnen, V. A., Zimmerman, P. R., Grosjean, D., Cautreels, W., Chatfield, R., Jaenicke, R., Ogren, J. A., Pellizzari, E. D., and Wallace, G. T.: Organic material in the global troposphere, Geophys. Rev., 21, 921–952, 1983. </reference>
		<reference numeration="13" content_type="text"> Duplissy, J., Gysel, M., Alfarra, M. R., Dommen, J., Metzger, A., Prevot, A. S. H., Weingartner, E., Laaksonen, A., Raatikainen, T., Good, N., Turner, S. F., McFiggans, G., and Baltensperger, U.: The cloud forming potential of secondary organic aerosol under near atmospheric conditions, Geophys, Res. Lett., 35, L03818, doi:10.1029/2007GL031075, 2008. </reference>
		<reference numeration="14" content_type="text"> Edney, E. O., Kleindienst, T. E., Jaoui, M., Lewandowski, M., Offenberg, J. H., Wang, W., and Claeys, M.: Formation of 2-methyl tetrols and 2-methylglyceric acid in secondary organic aerosol from laboratory irradiated isoprene/NO&lt;sub&gt;x&lt;/sub&gt;/SO2/air mixtures and their detection in ambient PM$_2.5$ samples collected in the eastern United States, Atmos. Environ., 39, 5281–5289, 2005. </reference>
		<reference numeration="15" content_type="text"> Erdakos, G. B., Chang, E. I., Pankow, J. F., and Seinfeld, J. H.: Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water – Part 3: Organic compounds, water, and ionic constituents by consideration of short-, mid-, and long-range effects using X-UNIFAC.3, Atmos. Environ., 40, 6437–6452, 2006. </reference>
		<reference numeration="16" content_type="text"> Fletcher, C. A., Johnson, G. R., Ristovski, Z. D., and Harvey, M.: Hygroscopic and volatile properties of marine aerosol, observed at Cape Grim during the P2P campaign, Environ. Chem., 4, 162–171, 2007. </reference>
		<reference numeration="17" content_type="text"> Gysel, M., Weingartner, E., and Baltensperger, U.: Hygroscopicity of aerosol particles at low temperatures. 2. Theoretical and experimental hygroscopic properties of laboratory generated aerosols, Environ. Sci. Technol., 36, 63–68, 2002. </reference>
		<reference numeration="18" content_type="text"> Gysel, M., Weingartner, E., Nyeki, S., Paulsen, D., Baltensperger, U., Galambos, I., and Kiss, G.: Hygroscopic properties of water-soluble matter and humic-like organics in atmospheric fine aerosol Atmos. Chem. Phys., 4, 35–50, 2004. </reference>
		<reference numeration="19" content_type="text"> Hansson, H. C., Rood, M. J., Koloutsou Vakakis, S., Hameri, K., Orsini, D., and Wiedensohler, A.: NaCl aerosol particle hygroscopicity dependence on mixing with organic compounds, J. Atmos. Chem., 31, 321–346, 1998. </reference>
		<reference numeration="20" content_type="text"> Hinz, K. P. and Spengler, B.: Instrumentation, data evaluation and quantification in on-line aerosol mass spectrometry, J. Mass Spectrometry, 42, 843–860, 2007. </reference>
		<reference numeration="21" content_type="text"> Jacobson, M. C., Hansson, H. C., Noone, K. J., and Charlson, R. J.: Organic atmospheric aerosols: Review and state of the science, Rev. Geophys, 38, 267–294, 2000. </reference>
		<reference numeration="22" content_type="text"> Johnson, G., Ristovski, Z., and Morawska, L.: Method for measuring the hygroscopic behaviour of lower volatility fractions in an internally mixed aerosol, J. Aerosol Sci., 35, 443–455, 2004. </reference>
		<reference numeration="23" content_type="text"> Johnson, G. R., Ristovski, Z. D., D&apos;Anna, B., and Morawska, L.: Hygroscopic behavior of partially volatilized coastal marine aerosols using the volatilization and humidification tandem differential mobility analyzer technique, J. Geophys. Res., 110, D20203, 2005. </reference>
		<reference numeration="24" content_type="text"> Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: A review, Atmos. Chem. Phys., 5, 1053–1123, 2005. </reference>
		<reference numeration="25" content_type="text"> Kerminen, V. M.: The effects of particle chemical character and atmospheric processes on particle hygroscopic properties, J. Aerosol Sci., 28, 121–132, 1997. </reference>
		<reference numeration="26" content_type="text"> Kiepe, J., Noll, O., and J., G.: Modified LIQUAC and modified LIFAC - a further development of electrolyte models for the reliable prediction of phase equilibria with strong electrolytes, Ind. Eng. Chem. Res., 45, 2361–2373, 2006. </reference>
		<reference numeration="27" content_type="text"> Krivacsy, Z., Gelencser, A., Kiss, G., Meszaros, G., Molnar, A., Hoffer, A., Meszaros, T., Sarvari, Z., Temesi, D., Varga, B., Baltensperger, U., Nyeki, S., and Weingartner, E.: Study on the chemical character of water soluble organic compounds in fine atmospheric aerosol at the Jungfraujoch, J Atmos Chem., 39, 235–259, 2001a. </reference>
		<reference numeration="28" content_type="text"> Krivacsy, Z., Hoffer, A., Sarvari, Z., Temesi, D., Baltensperger, U., Nyeki, S., Weingartner, E., Kleefeld, S., and Jennings, S. G.: Role of organic and black carbon in the chemical composition of atmospheric aerosol at European background sites, Atmos. Environ., 35, 6233–6244, 2001b. </reference>
		<reference numeration="29" content_type="text"> Lightstone, J. M., Onasch, T. B., Imre, D., and Oatis, S.: Deliquescence, efflorescence, and water activity in ammonium nitrate and mixed ammonium nitrate/succinic acid microparticles, J. Phys. Chem., 104, 9337–9346, 2000. </reference>
		<reference numeration="30" content_type="text"> Marcolli, C., Luo, B., and Peter, T.: Mixing of organic aerosol fractions: Liquids as thermodynamically stable phases, J. Phys. Chem. A, 108, 2216–2224, 2004. </reference>
		<reference numeration="31" content_type="text"> Marcolli, C. and Krieger, U. K.: Phase changes during hygroscopic cycles of mixed organic/inorganic model systems of tropospheric aerosols, J. Phys. Chem. A, 110, 1881–1893, 2006. </reference>
		<reference numeration="32" content_type="text"> McMurry, P. H. and Stolzenburg, M. R.: On the sensitivity of particle size to relative humidity for Los Angeles aerosols., Atmos. Environ., 23, 497–507, 1989. </reference>
		<reference numeration="33" content_type="text"> Meyer, N. K. and Ristovski, Z. D.: Ternary nucleation as a mechanism for the production of diesel nanoparticles: Experimental analysis of the volatile and hygroscopic properties of diesel exhaust using the volatilization and humidification tandem differential mobility analyzer, Environ. Sci. Technol., 41, 7309–7314, 2007. </reference>
		<reference numeration="34" content_type="text"> Ming, Y. and Russell, L. M.: Thermodynamic equilibrium of organic-electrolyte mixtures in aerosol particles, Environmental and Energy Engineering, 48, 1331–1348, 2002. </reference>
		<reference numeration="35" content_type="text"> Novakov, T. and Penner, J. E.: Large contribution of organic aerosols to cloud-condensation-nuclei concentrations, Nature, 365, 823–826, 1993. </reference>
		<reference numeration="36" content_type="text"> Paulsen, D., Dommen, J., Kalberer, M., Prevot, A. S. H., Richter, R., Sax, M., Steinbacher, M., Weingartner, E., and Baltensperger, U.: Secondary organic aerosol formation by irradiation of 1,3,5 trimethylbenzene-NO&lt;sub&gt;x&lt;/sub&gt;-H&lt;sub&gt;2&lt;/sub&gt;O in a new reaction chamber for atmospheric chemistry and physics, Environ. Sci. Technol., 39, 2668–2678, 2005. </reference>
		<reference numeration="37" content_type="text"> Peng, C., Chan, M. N., and Chan, C. K.: The hygroscopic properties of dicarboxylic and multifunctional acids: Measurements and unifac predictions, Environ. Sci. Technol., 35, 4495–4501, 2001. </reference>
		<reference numeration="38" content_type="text"> Peng, C. G. and Chan, C. K.: The water cycles of water-soluble organic salts of atmospheric importance, Atmos. Environ., 35, 1183–1192, 2001. </reference>
		<reference numeration="39" content_type="text"> Petters, M. D. and Kreidenweis, S. M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, 2007. </reference>
		<reference numeration="40" content_type="text"> Prenni, A. J., DeMott, P. J., Kreidenweis, S. M., Sherman, D. E., Russell, L. M., and Ming, Y.: The effects of low molecular weight dicarboxylic acids on cloud formation, J. Phys. Chem. A, 105, 11240–11248, 2001. </reference>
		<reference numeration="41" content_type="text"> Rader, D. J. and McMurry, P. H.: Application of the tandem differential mobility analyzer to studies of droplet growth or evaporation, J. Aerosol Sci., 17, 771–787, 1986. </reference>
		<reference numeration="42" content_type="text"> Ristovski, Z. D., Fletcher, C., D&apos;Anna, B., Johnson, G. R., and Bostrom, J. T.: Characterization of iodine particles with volatilization-humidification tandem differential mobility analyser (VH-TDMA), Raman and Sem techniques, Atmos. Chem. Phys. Discuss., 1481–1508, 2006. </reference>
		<reference numeration="43" content_type="text"> Saxena, P., Hildeman, L. H., McMurry, P. H., and Seinfeld, J. H.: Organics alter hygroscopic behavior of atmospheric particles, J. Geophys. Res, 100, 18755–18770, 1995. </reference>
		<reference numeration="44" content_type="text"> Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: From air pollution to climate change, 2nd ed., Wiley, Hoboken, NJ, USA, 1203 pp., 2006. </reference>
		<reference numeration="45" content_type="text"> Sjogren, S., Gysel, M., Weingartner, E., Alfarra, M. R., Duplissy, J., Cozic, J., Crosier, J., Coe, H., and Baltensperger, U.: Hygroscopicity ofthe submicrometer aerosol at the high-alpine site jungfraujoch, 3850 m a.s.l., Switzerland, Atmos. Chem. Phys. Discuss., 7, 13699–13732, 2007a. </reference>
		<reference numeration="46" content_type="text"> Sjogren, S., Gysel, M., Weingartner, E., Baltensperger, U., Cubison, M. J., Coe, H., Zardini, A. A., Marcolli, C., Krieger, U. K., and Peter, T.: Hygroscopic growth and water uptake kinetics of two-phase aerosol particles consisting of ammonium sulfate, adipic and humic acid mixtures, J. Aerosol Sci., 38, 157–171, 2007b. </reference>
		<reference numeration="47" content_type="text"> Stokes, R. H. and Robinson, R. A.: Interactions in aqueous nonelectrolyte solutions. I. Solute solvent equilibria, J. Phys. Chem, 70, 2126–2130, 1966. </reference>
		<reference numeration="48" content_type="text"> Surratt, J. D., Kroll, J. H., Kleindienst, T. E., Edney, E. O., Claeys, M., Sorooshian, A., Ng, N. L., Offenberg, J. H., Lewandowski, M., Jaoui, M., Flagan, R. C., and Seinfeld, J. H.: Evidence for organosulfates in secondary organic aerosol, Environ. Sci. Technol., 41, 517–527, 2007. </reference>
		<reference numeration="49" content_type="text"> Topping, D. O., McFiggans, G. B., and Coe, H.: A curved multi-component aerosol hygroscopicity model framework: Part 2 – including organic compounds, Atmos. Chem. Phys., 5, 1223–1242, 2005. </reference>
		<reference numeration="50" content_type="text"> Varutbangkul, V., Brechtel, F. J., Bahreini, R., Ng, N. L., Keywood, M. D., Kroll, J. H., Flagan, R. C., Seinfeld, J. H., Lee, A., and Goldstein, A. H.: Hygroscopicity of secondary organic aerosols formed by oxidation of cycloalkenes, monoterpenes, sesquiterpenes, and related compounds, Atmos. Chem. Phys., 6, 2367–2388, 2006. </reference>
		<reference numeration="51" content_type="text"> Virkkula, A., Van Dingenen, R., Raes, F., and Hjorth, J.: Hygroscopic properties of aerosol formed by oxidation of limonene, alpha-pinene, and beta-pinene, J. Geophys. Res.-Atmos., 104, 3569–3579, 1999. </reference>
		<reference numeration="52" content_type="text"> Xiong, J. Q., Zhong, M. H., Fang, C. P., Chen, L. C., and Lippmann, M.: Influence of organic films on the hygroscopicity of ultrafine sulfuric acid aerosol, Environ. Sci. Technol., 32, 3536–3541, 1998. </reference>
	</references>
</article>

