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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>21</issue_number>
		<publication_year>2009</publication_year>
	</journal>
	<doi>10.5194/acp-9-8351-2009</doi>
	<article_url>http://www.atmos-chem-phys.net/9/8351/2009/</article_url>
	<abstract_html>http://www.atmos-chem-phys.net/9/8351/2009/acp-9-8351-2009.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys.net/9/8351/2009/acp-9-8351-2009.pdf</fulltext_pdf>
	<start_page>8351</start_page>
	<end_page>8363</end_page>
	<publication_date>2009-11-03</publication_date>
	<article_title content_type="html">Toward a general parameterization of N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt; reactivity on aqueous particles: the competing effects of particle liquid water, nitrate and chloride</article_title>
	<authors>
		<author numeration="1" affiliations="1,2">
			<name>T. H. Bertram</name>
		</author>
		<author numeration="2" affiliations="1">
			<name>J. A. Thornton</name>
			<email>thornton@atmos.washington.edu</email>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA</affiliation>
		<affiliation numeration="2" content_type="html">now at: Department of Chemistry, University of California San Diego, La Jolla, CA</affiliation>
	</affiliations>
	<abstract content_type="html">The heterogeneous reaction of N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt; on mixed organic-inorganic
aerosol particles was investigated using an entrained aerosol flow tube
coupled to a custom-built chemical ionization mass spectrometer. Laboratory
results on aqueous particles confirm a strong dependence of the reactive
uptake coefficient (γ) on particle liquid water, for particle water
concentrations below 15 M, and the molar ratio of particle water to nitrate.
Measurements of &amp;gamma; (N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt;) on mixed chloride-nitrate
particles indicate that the presence of trace chloride can negate the
suppression of γ(N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt;) at high nitrate loadings with
implications for polluted coastal regions. These results are used to
construct a new parameterization for &amp;gamma; (N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt;), that when
coupled to an aerosol thermodynamics model, can be used within regional
and/or global chemical transport models.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Anttila, T., Kiendler-Scharr, A., Tillmann, R., and Mentel, T. F.: On the reactive uptake of gaseous compounds by organic-coated aqueous aerosols: Theoretical analysis and application to the heterogeneous hydrolysis of N&lt;sub&gt;2&lt;/sub&gt;O$_5$, J. Phys. Chem. A, 110, 10435–10443, 2006. </reference>
		<reference numeration="2" content_type="text"> Badger, C. L., Griffiths, P. T., George, I., Abbatt, J. P. D., and Cox, R. A.: Reactive uptake of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ by aerosol particles containing mixtures of humic acid and ammonium sulfate, J. Phys. Chem. A, 110, 6986-6994, 2006. </reference>
		<reference numeration="3" content_type="text"> Behnke, W., George, C., Scheer, V., and Zetzsch, C.: Production and decay of ClNO&lt;sub&gt;2&lt;/sub&gt;, from the reaction of gaseous N&lt;sub&gt;2&lt;/sub&gt;O$_5$ with NaCl solution: Bulk and aerosol experiments, J. Geophys. Res., 102, 3795–3804, 1997. </reference>
		<reference numeration="4" content_type="text"> Bertram, T. H., Thornton, J. A. and Riedel, T. P.: An experimental technique for the direct measurement of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ reactivity on ambient particles, Atmos. Meas. Tech., 2, 231–242, 2009. </reference>
		<reference numeration="5" content_type="text"> Braban, C. F. and Abbatt, J. P. D.: A study of the phase transition behavior of internally mixed ammonium sulfate-malonic acid aerosols, Atmos. Chem. Phys., 4, 1451–1459, 2004. </reference>
		<reference numeration="6" content_type="text"> Brown, R. L.: Tubular Flow Reactors with 1st-Order Kinetics, J. Res. Nat. Bureau Stand., 83, 1–8, 1978. </reference>
		<reference numeration="7" content_type="text"> Brown, S. S., Ryerson, T. B., Wollny, A. G., Brock, C. A., Peltier, R., Sullivan, A. P., Weber, R. J., Dube, W. P., Trainer, M., Meagher, J. F., Fehsenfeld, F. C., and Ravishankara, A. R.: Variability in nocturnal nitrogen oxide processing and its role in regional air quality, Science, 311, 67–70, 2006. </reference>
		<reference numeration="8" 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;-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, Including Solubilities of HBr, from Less Than 200 to 328 K, J. Phys. Chem., 99, 11557–11574, 1995. </reference>
		<reference numeration="9" content_type="text"> Clegg, S. L., Brimblecombe, P., and Wexler, A. S.: Thermodynamic model of the system H$^ + $-NH$_4^+$-Na$^ + $-SO$_4^2-$-NO$_3^-$-Cl$^-$-H&lt;sub&gt;2&lt;/sub&gt;O at 298.15 K, J. Phys. Chem. A, 102, 2155–2171, 1998. </reference>
		<reference numeration="10" content_type="text"> Cosman, L. M. and Bertram, A. K.: Reactive uptake of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ on aqueous H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt; solutions coated with 1-component and 2-component monolayers, J. Phys. Chem. A, 112, 4625–4635, 2008. </reference>
		<reference numeration="11" content_type="text"> Cosman, L. M., Knopf, D. A., and Bertram, A. K.: N&lt;sub&gt;2&lt;/sub&gt;O$_5$ reactive uptake on aqueous sulfuric acid solutions coated with branched and straight-chain insoluble organic surfactants, J. Phys. Chem. A, 112, 2386–2396, 2008. </reference>
		<reference numeration="12" content_type="text"> Cziczo, D. J., Nowak, J. B., Hu, J. H., and Abbatt, J. P. D.: Infrared spectroscopy of model tropospheric aerosols as a function of relative humidity: Observation of deliquescence and crystallization, J. Geophys. Res., 102, 18843–18850, 1997. </reference>
		<reference numeration="13" content_type="text"> Davis, J. M., Bhave, P. V., and Foley, K. M.: Parameterization of N2O5 reaction probabilities on the surface of particles containing ammonium, sulfate, and nitrate, Atmos. Chem. Phys., 8, 5295–5311, 2008. </reference>
		<reference numeration="14" content_type="text"> Dentener, F. J. and Crutzen, P. J.: Reaction of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ on tropospheric aerosols - Impact on the global distributions of NO&lt;sub&gt;x&lt;/sub&gt;, O&lt;sub&gt;3&lt;/sub&gt;, and OH, J. Geophys. Res., 98, 7149–7163, 1993. </reference>
		<reference numeration="15" content_type="text"> Evans, M. J. and Jacob, D. J.: Impact of new laboratory studies of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ hydrolysis on global model budgets of tropospheric nitrogen oxides, ozone, and OH, Geophys. Res. Lett., 32, L09813, doi:10.1029/2005GL022469, 2005. </reference>
		<reference numeration="16" content_type="text"> Finlayson-Pitts, B. J., Ezell, M. J., and Pitts, J. N.: Formation of chemically active chlorine compounds by reactions of atmospheric NaCl particles with gaseous N&lt;sub&gt;2&lt;/sub&gt;O$_5$ and ClONO&lt;sub&gt;2&lt;/sub&gt;, Nature, 337, 241–244, 1989. </reference>
		<reference numeration="17" content_type="text"> Folkers, M., Mentel, T. F., and Wahner, A.: Influence of an organic coating on the reactivity of aqueous aerosols probed by the heterogeneous hydrolysis of N&lt;sub&gt;2&lt;/sub&gt;O$_5$, Geophys. Res. Lett., 30(12), 1644, doi:10.1029/2003GL017168, 2003. </reference>
		<reference numeration="18" content_type="text"> Fountoukis, C. and Nenes, A.: ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K + -Ca&lt;sub&gt;2&lt;/sub&gt; + -Mg&lt;sub&gt;2&lt;/sub&gt; + -Nh(4)( + )-Na + -SO$_4^2$–NO&lt;sub&gt;3&lt;/sub&gt;–Cl–H&lt;sub&gt;2&lt;/sub&gt;O aerosols, Atmos. Chem. Phys., 7, 4639–4659, 2007. </reference>
		<reference numeration="19" content_type="text"> Fried, A., Henry, B. E., Calvert, J. G., and Mozurkewich, M.: The reaction probability of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ with sulfuric-acid aerosols at stratospheric temperatures and compositions, J. Geophys. Res., 99, 3517–3532, 1994. </reference>
		<reference numeration="20" content_type="text"> Griffiths, P. T., Badger, C. L., Cox, R. A., Folkers, M., Henk, H. H., and Mentel, T. F.: Reactive Uptake of N2O5 by Aerosols Containing Dicarboxylic Acids. Effect of Particle Phase, Composition, and Nitrate Content, J. Phys. Chem. A, 113, 5082–5090, 2009. </reference>
		<reference numeration="21" content_type="text"> Hallquist, M., Stewart, D. J., Stephenson, S. K., and Cox, R. A.: Hydrolysis of N2O5 on sub-micron sulfate aerosols, PCCP, 5, 3453–3463, 2003. </reference>
		<reference numeration="22" content_type="text"> Hanson, D. and Kosciuch, E.: The NH&lt;sub&gt;3&lt;/sub&gt; mass accommodation coefficient for uptake onto sulfuric acid solutions, J. Phys. Chem. A, 107, 2199–2208, 2003. </reference>
		<reference numeration="23" content_type="text"> Hu, J. H. and Abbatt, J. P. D.: Reaction probabilities for N&lt;sub&gt;2&lt;/sub&gt;O$_5$ hydrolysis on sulfuric acid and ammonium sulfate aerosols at room temperature, J. Phys. Chem. A, 101, 871–878, 1997. </reference>
		<reference numeration="24" content_type="text"> Kane, S. M., Caloz, F. and Leu, M. T.: Heterogeneous uptake of gaseous N2O5 by (NH4)(2)SO4, NH4HSO4, and H2SO4 aerosols, J. Phys. Chem. A, 105, 6465–6470, 2001. </reference>
		<reference numeration="25" content_type="text"> Kercher, J. P., Reidel, T., and Thornton, J. A.: Chlorine activation by N&lt;sub&gt;2&lt;/sub&gt;O$_5$: In situ detection of ClNO&lt;sub&gt;2&lt;/sub&gt; and N&lt;sub&gt;2&lt;/sub&gt;O$_5$ by chemical ionization mass spectrometry, Atmos. Meas. Tech., 2, 193–204, 2009. </reference>
		<reference numeration="26" content_type="text"> Knopf, D. A., Cosman, L. M., Mousavi, P., Mokamati, S., and Bertram, A. K.: A novel flow reactor for studying reactions on liquid surfaces coated by organic monolayers: Methods, validation, and initial results, J. Phys. Chem. A, 111, 11021–11032, 2007. </reference>
		<reference numeration="27" content_type="text"> McNeill, V. F., Patterson, J., Wolfe, G. M., and Thornton, J. A.: The effect of varying levels of surfactant on the reactive uptake of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ to aqueous aerosol, Atmos. Chem. Phys., 6, 1635–1644, 2006. </reference>
		<reference numeration="28" content_type="text"> Mentel, T. F., Sohn, M., and Wahner, A.: Nitrate effect in the heterogeneous hydrolysis of dinitrogen pentoxide on aqueous aerosols, PCCP, 1, 5451–5457, 1999. </reference>
		<reference numeration="29" content_type="text"> Mozurkewich, M. and Calvert, J. G.: Reaction probability of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ on aqueous aerosols, J. Geophys. Res., 93, 15889–15896, 1988. </reference>
		<reference numeration="30" 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., 111, D23S32, doi:10.1029/2006JD007340, 2006. </reference>
		<reference numeration="31" content_type="text"> Osthoff, H. D., Roberts, J. M., Ravishankara, A. R., Williams, E. J., Lerner, B. M., Sommariva, R., Bates, T. S., Coffman, D., Quinn, P. K., Dibb, J. E., Stark, H., Burkholder, J. B., Talukdar, R. K., Meagher, J., Fehsenfeld, F. C., and Brown, S. S.: High levels of nitryl chloride in the polluted subtropical marine boundary layer, Nature Geoscience, 1, 324–328, 2008. </reference>
		<reference numeration="32" content_type="text"> Park, S. C., Burden, D. K., and Nathanson, G. M.: The inhibition of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ hydrolysis in sulfuric acid by 1-butanol and 1-hexanol surfactant coatings, J. Phys. Chem. A, 111, 2921–2929, 2007. </reference>
		<reference numeration="33" content_type="text"> Quinn, P. K., Bates, T. S., Baynard, T., Clarke, A. D., Onasch, T. B., Wang, W., Rood, M. J., Andrews, E., Allan, J., Carrico, C. M., Coffman, D., and Worsnop, D.: Impact of particulate organic matter on the relative humidity dependence of light scattering: A simplified parameterization, Geophys. Res. Lett., 32, L22809, doi:10.1029/2005GL024322, 2005. </reference>
		<reference numeration="34" content_type="text"> Riemer, N., Vogel, H., Vogel, B., Schell, B., Ackermann, I., Kessler, C., and Hass, H.: Impact of the heterogeneous hydrolysis of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ on chemistry and nitrate aerosol formation in the lower troposphere under photosmog conditions, J. Geophys. Res., 108(D4), 4144, doi:10.1029/2002JD002436, 2003. </reference>
		<reference numeration="35" content_type="text"> Riemer, N., Vogel, H., Vogel, B., Anttila, T., Kiendler-Scharr, A., and Mentel, T. F.: The relative importance of organic coatings for the heterogeneous hydrolysis of N&lt;sub&gt;2&lt;/sub&gt;O$_5$, 114, D17307, doi:10.1029/2008JD011369, 2009. </reference>
		<reference numeration="36" content_type="text"> Robinson, G. N., Worsnop, D. R., Jayne, J. T., Kolb, C. E., and Davidovits, P.: Heterogeneous uptake of ClONO&lt;sub&gt;2&lt;/sub&gt; and N&lt;sub&gt;2&lt;/sub&gt;O$_5$ by sulfuric acid solutions, J. Geophys. Res., 102, 3583–3601, 1997. </reference>
		<reference numeration="37" content_type="text"> Schweitzer, F., Mirabel, P., and George, C.: Multiphase chemistry of N&lt;sub&gt;2&lt;/sub&gt;O$_5$, ClNO&lt;sub&gt;2&lt;/sub&gt;, and BrNO&lt;sub&gt;2&lt;/sub&gt;, J. Phys. Chem. A, 102, 3942–3952, 1998. </reference>
		<reference numeration="38" content_type="text"> Thornton, J. A. and Abbatt, J. P. D.: N&lt;sub&gt;2&lt;/sub&gt;O$_5$ reaction on submicron sea salt aerosol: Kinetics, products, and the effect of surface active organics, J. Phys. Chem. A, 109, 10004–10012, 2005. </reference>
		<reference numeration="39" content_type="text"> Thornton, J. A., Braban, C. F., and Abbatt, J. P. D.: N&lt;sub&gt;2&lt;/sub&gt;O$_5$ hydrolysis on sub-micron organic aerosols: the effect of relative humidity, particle phase, and particle size, PCCP, 5, 4593–4603, 2003. </reference>
		<reference numeration="40" content_type="text"> Wagner, C., Hanisch, F., Holmes, N., de Coninck, H., Schuster, G., and Crowley, J. N.: The interaction of N2O5 with mineral dust: aerosol flow tube and Knudsen reactor studies, Atmos. Chem. Phys., 8, 91–109, 2008. </reference>
		<reference numeration="41" content_type="text"> Wahner, A., Mentel, T. F., Sohn, M. and Stier, J.: Heterogeneous reaction of N&lt;sub&gt;2&lt;/sub&gt;O$_5$ on sodium nitrate aerosol, J. Geophys. Res., 103, 31103–31112, 1998. </reference>
		<reference numeration="42" content_type="text"> Wexler, A. S. and Clegg, S. L.: Atmospheric aerosol models for systems including the ions H$^ + $, NH$_4^+$, Na$^ + $, SO$_4^2-$, NO$_3^-$,Cl$^-$, Br$^-$, and H&lt;sub&gt;2&lt;/sub&gt;O, J. Geophys. Res., 107(D14), 4207, doi:10.1029/2001JD000451, 2002. </reference>
		<reference numeration="43" content_type="text"> Zaveri, R. A., Easter, R. C., Fast, J. D. and Peters, L. K.: Model for Simulating Aerosol Interactions and Chemistry (MOSAIC), J. Geophys. Res., 113, D13204, doi:10.1029/2007JD008782, 2008. </reference>
	</references>
</article>

