ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-10-10561-2010 An overview of current issues in the uptake of atmospheric trace gases by aerosols and clouds Kolb C. E. 1 Cox R. A. 2 Abbatt J. P. D. 3 Ammann M. 4 Davis E. J. 5 Donaldson D. J. 3 Garrett B. C. 6 George C. 7 Griffiths P. T. 2 Hanson D. R. 8 Kulmala M. 9 McFiggans G. 10 Pöschl U. 11 Riipinen I. 9 Rossi M. J. 12 Rudich Y. 13 Wagner P. E. 14 Winkler P. M. 14 15 Worsnop D. R. 1 9 O' Dowd C. D. 16 Center for Aerosol and Cloud Chemistry, Aerodyne Research, Inc., 45 Manning Road, Billerica, MA 01821-3976, USA Centre for Atmospheric Science, Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EP, UK Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON, M5S 3H6, Canada Laboratory of Radiochemistry and Environmental Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland Department of Chemical Engineering, University of Washington, Seattle, WA 98195-1750, USA Fundamental & Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99352, USA IRCELYON, Institut de recherches sur la catalyse et l'environnement de Lyon, CNRS UMR 5256, Université Lyon 1. 2, Av. Albert Einstein, 69626 Villeurbanne Cedex, France Augsburg College, Minneapolis, MN 55454, USA Department of Physical Sciences, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland Centre for Atmospheric Sciences, School of Earth, Atmospheric & Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK Biogeochemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany Laboratorium fuer Atmosphaerenchemie, OFLA008, Paul Scherrer Institute, 5232 Villigen, Switzerland Department of Environmental Sciences, Weizmann Institute, Rehovot 76100, Israel Faculty of Physics, University of Vienna, 1090 Vienna, Austria Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, CO 80305-5602, USA School of Physics and Centre for Climate & Air Pollution Studies, National University of Ireland Galway, University Road, Galway, Ireland 10 11 2010 10 21 10561 10605 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/10/10561/2010/acp-10-10561-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/10561/2010/acp-10-10561-2010.pdf

A workshop was held in the framework of the ACCENT (Atmospheric Composition Change – a European Network) Joint Research Programme on "Aerosols" and the Programme on "Access to Laboratory Data". The aim of the workshop was to hold "Gordon Conference" type discussion covering accommodation and reactive uptake of water vapour and trace pollutant gases on condensed phase atmospheric materials. The scope was to review and define the current state of knowledge of accommodation coefficients for water vapour on water droplet and ice surfaces, and uptake of trace gas species on a variety of different surfaces characteristic of the atmospheric condensed phase particulate matter and cloud droplets. Twenty-six scientists participated in this meeting through presentations, discussions and the development of a consensus review. <br><br> In this review we present an analysis of the state of knowledge on the thermal and mass accommodation coefficient for water vapour on aqueous droplets and ice and a survey of current state-of the-art of reactive uptake of trace gases on a range of liquid and solid atmospheric droplets and particles. The review recommends consistent definitions of the various parameters that are needed for quantitative representation of the range of gas/condensed surface kinetic processes important for the atmosphere and identifies topics that require additional research.

 References Abbatt, J. P. D.: Heterogeneous interactions of BrO and ClO: Evidence for BrO surface recombination and reaction with HSO$_3^-$/SO$_3^2$, Geophys. Res. Lett., 23, 1681–1684, 1996. Abbatt, J. P. D.: Interactions of atmospheric trace gases with ice surfaces: adsorption and reaction, Chem. Rev., 103, 4783–4800, 2003. Abbatt, J. P. D. and Waschewsky, G. C. G.: Heterogeneous interactions of HOBr, HNO<sub>3</sub>, O<sub>3</sub> and NO<sub>2</sub> with deliquescent NaCl aerosols at room temperature, J. Phys. Chem. A., 102, 3719–3725, 1998. Adams, J. W., Holmes, N. S., and Crowley, J. N.: Uptake and reaction of HOBr on frozen and dry NaCl/NaBr surfaces between 253 and 233 K, Atmos. Chem. Phys., 2, 79–91, 2002. Adams, J W., Rodriguez, D., and Cox, R A.: The uptake of SO<sub>2</sub> on Saharan dust: a flow tube study, Atmos. Chem. Phys., 5, 2643–2676, doi:10.5194/acp-5-2643-2005, 2005. Adamson, A. W. and Gast, A. P.: Physical chemistry of surfaces, J. Wiley and Sons, New York, NY, USA, 75–86, 1997. Aguzzi, A. and Rossi, M. J.: The Kinetics of the uptake of HNO<sub>3</sub> on Ice, Solid H<sub>2</sub>SO<sub>4</sub>/H<sub>2</sub>O and Solid Ternary Solutions of H<sub>2</sub>SO<sub>4</sub>/HNO<sub>3</sub>/H<sub>2</sub>O in the Temperature Range 180 to 211 K, Phys. Chem. Chem. Phys., 3, 3707–3716, 2001. Aguzzi, A., Flückiger, B. and Rossi, M. J.: The nature of the interface and the diffusion coefficient of HCl/ice and HBr/ice in the temperature range 190–205 K, Phys. Chem. Chem. Phys., 5, 4157–4169, 2003. Alcala-Jornod, C. and Rossi, M. J.: Chemical kinetics of the interaction of H<sub>2</sub>O vapor with soot in the range 190 = T/K = 300: A diffusion tube study, J. Phys. Chem. A, 108, 10667–10680, 2004. Alejandre, J., Tildesley, D. J., and Chapela, G. A.: Molecular–Dynamics Simulation of the Orthobaric Densities and Surface–Tension of Water, J. Chem. Phys., 102, 4574–4583, 1995. Allen, H. C., Gragson, D. E., and Richmond, G. L.: Molecular structure and adsorption of dimethyl sulfoxide at the surface of aqueous solutions, J. Phys. Chem. B, 103, 660–666, 1999. Allen, M. P., and Tildesley, D. J.: Computer Simulation of Liquids, Oxford University Press, New York, USA, 24–32, 1987. Ammann, M. and Pöschl, U.: Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 2: Exemplary practical applications and numerical simulations, Atmos. Chem. Phys., 7, 6025–6045, doi:10.5194/acp-7-6025-2007, 2007. Ammann, M., Pöschl, U., and Rudich, Y.: Effects of reversible adsorption and Langmuir-Hinshelwood surface reactions on gas uptake by atmospheric particles, Phys. Chem. Chem. Phys., 5, 351–356, 2003. Anonymous Referee #1: Interactive comment on "Alkene ozonolysis SOA: inferences of composition and droplet growth kinetics from Köhler theory analysis" by A. Asa-Awuku et al., Anonymous Referee #1, Atmos. Chem. Phys. Discuss., 7, S4052–S4062, doi:10.5194/acp-7-S4052-2007, 2007. 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<sub>2</sub>O$_5$, J. Phys. Chem. A., 110, 10435–10443, 2006. 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, doi:10.5194/acp-5-2617-2005, 2005. Ardura, D. and Donaldson, D. J.: Where does acid hydrolysis take place?, Phys. Chem. Chem. Phys., 11, 857–863, 2009. Arens, F., Gutzwiller, L., Baltensperger, U., Heinz W. Gäggeler,~H. W.,~and Ammann, M.: Heterogeneous reaction of NO<sub>2</sub> on diesel soot particles, Environ. Sci. Technol., 35, 2191–2199, 2001. Asa-Awuku, A., Engelhart, G. J., Lee, B. H., Pandis, S. N. and Nenes, A.: Relating CCN activity, volatility, and droplet growth kinetics of $\beta-$caryophyllene secondary organic aerosol, Atmos. Chem. Phys., 9, 795–812, doi:10.5194/acp-9-795-2009, 2009. Asa-Awuku, A., Nenes, A., Gao, S., Flagan, R. C., and Seinfeld, J. H.: Water-soluble SOA from Alkene ozonolysis: composition and droplet activation kinetics inferences from analysis of CCN activity, Atmos. Chem. Phys., 10, 1585–1597, doi:10.5194/acp-10-1585-2010, 2010. Aubin, D. G. and Abbatt, J. P. D.: Interaction of NO<sub>2</sub> with Hydrocarbon Soot: Focus on HONO Yield, Surface Modification and Mechanism, J. Phys. Chem. A, 111, 6263–6273, 2007. Ardura, D. and Donaldson, D.J..: Where does acid hydrolysis take place?, Phys. Chem. Chem. Phys., 11, 857–863, 2009. Aumont, B., Madronich, S., Ammann, M., ~Kalberer, M., Baltensperger, U., Hauglustaine, D. and~Brocheton,~F.: On the NO<sub>2</sub> + Soot Reaction in the Atmosphere, J. Geophys. Res., 104, 1729–1736, 1999. Autrey, T., Brown, A. K., Camaioni, D. M., Dupuis, M., Foster, N. S., and Getty, A.: Thermochemistry of aqueous hydroxyl radical from advances in photoacoustic calorimetry and ab initio continuum solvation theory, J. Am. Chem. Soc., 126, 3680–3681, 2004. Baldwin, A. C. and Golden, D. M.: Heterogeneous atmospheric reactions – Sulfuric acid aerosols as tropospheric sinks, Science, 206, 562–563, 1979. Badger, C. L., George, I., Griffiths, P. T., Abbatt, J. P. D., and Cox, R. A.: Reaction uptake of N<sub>2</sub>O$_5$ by aerosol particles containing humic acid and ammonium sulfate, J. Phys. Chem. A., 110, 6986–6994, 2006. Bartels-Rausch, T., Huthwelker, T., Gäggeler, H. W., and Ammann, M.: Atmospheric Pressure Coated-Wall Flow–Tube Study of Acetone Adsorption on Ice, J. Phys. Chem. A, 109, 4531–4539, 2005. Behnke, W., Krüger, H.-U., Scheer, V., and Zetsch, C.: Formation of atomic Cl from sea spray via photolysis of nitryl chloride – determination of the sticking coefficient of N2O5 on NaCl aerosol, J. Aerosol Sci., 22, 609–612, 1991. Ben-Naim, A. and Marcus, Y.: Solvation Thermodynamics of Nonionic Solutes, J. Chem. Phys., 81, 2016–2027, 1984. Benjamin, I.: Theoretical–Study of Ion Solvation at the Water Liquid–Vapor Interface, J. Chem. Phys., 95, 3698–3709, 1991. Benjamin, I.: Structure, thermodynamics, and dynamics of the liquid/vapor interface of water/dimethylsulfoxide mixtures, J. Chem. Phys., 110, 8070–8079, 1999. Berendsen, H. J. C., Postma, J. P. M., van Gunsteren, W. F., and Hermans, J.: Interaction models for water in relation to protein hydration, in: Intermolecular Forces, edited by: Pullman, B., 24, Reidel, Dordrecht, The Netherlands, 331–342, 1981. Berendsen, H. J. C., Grigera, J. R., and Straatsma, T. P.: The Missing Term in Effective Pair Potentials, J. Phys. Chem., 91, 6269–6271, 1987. Bertram, A. K., Ivanov, A. V., Hunter, M., Molina, L. T., and Molina, M. J.: The reaction probability of OH on organic surfaces of tropospheric interest, J. Phys. Chem. A, 105, 9415–9421, 2001. Bertram, T. H., Thornton, J. A., Riedel, T. P., Middlebrook, A. M., Bahreini, R., Bates, T. S., Quinn, P. K. and Coffman, D. J.: Direct observations of N<sub>2</sub>O$_5$ reactivity on ambient aerosol particles, Geophys. Res. Lett., 36, L19803, doi:10.1029/2009GL040248, 2009. Biermann, U. M., Crowley, J. N., Huthwelker, T., Moortgat, G. K., Crutzen, P. J., and Peter, T.: FTIR studies on lifetime prolongation of stratospheric ice particles due to NAT coating, Geophys. Res. Lett., 25, 3939–3942, 1998. Bougiatioti, A., Fountoukis, C., Kalivitis, N., Pandis, S. N., Nenes, A., and Mihalopoulos, N.: Cloud condensation nuclei measurements in the marine boundary layer of the Eastern Mediterranean: CCN closure and droplet growth kinetics, Atmos. Chem. Phys., 9, 7053–7066, 2009. Boy, M., Kulmala, M., Ruuskanen,T., Pihlatie, M., Reissell, A., Aalto, P. P., Keronen, P., Dal Maso, M., Hellen, H., Hakola, H., Janssen, R., Hanke, M., and Arnold, F.: Sulphuric acid closure and contribution to nucleation mode particle growth, Atmos. Chem. Phys., 5, 863–878, doi:10.5194/acp-5-863-2005, 2005. Brigante, M., Cazoir, D., D'Anna, B., George, C., and Donaldson, D. J.: Photoenhanced uptake of NO2 by pyrene solid films, J. Phys. Chem. A, 112, 9503–9508, doi:10.1021/jp802324g, 2008. Broekhuizen, K. E., Thornberry, T., Kumar, P. P., and Abbatt, J. P. D.: Formation of cloud condensation nuclei by oxidative processing: Unsaturated fatty acids, J. Geophys. Res.-Atmos., 109, D24206, doi:10.1029/2004JD005298, 2004. Brown, R. L.: Tubular Flow Reactors with First Order Kinetics, J. Res. Natl. Bur. Stand., 83, 1–8, 1978. 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. Brown, S. S., Dube, W. P., Fuchs, F., et al.: Reactive uptake coefficients for N<sub>2</sub>O$_5$ determined from aircraft measurements during the Second Texas Air Quality Study: Comparison to current model parameterizations, J. Geophys. Res., 114, D00F10, doi:1029/2008JD011679, 2009. Buajarern, J. Mitchem, L., and Reid, J. P.: Manipulation and Characterization of Aqueous Sodium Dodecyl Sulfate/Sodium Chloride Aerosol Particles, J. Phys. Chem. A, 111, 13038–13045, 2007. Buch, V., Milet, A., Vácha, R., Jungwirth, P., and Devlin, J. P.: Water surface is acidic, Proc. Natl. Acad. Sci., , 104, 7342–7347, 2007. Caloz, F., Fenter, F, Tabor, K. D., and Rossi, M. J.: Paper I: Design and construction of a Knudsen–cell reactor for the study of heterogeneous reactions over the temperature range 130–750 K: Performances and limitations, Rev. Sci. Instrum., 68, 3172–3179, 1997. Canneaux, S., Soetens, J. C., Henon, E., and Bohr, F.: Accommodation of ethanol, acetone and benzaldehyde by the liquid-vapor interface of water: A molecular dynamics study, Chem. Phys., 327, 512–517, 2006. Canonica, S., Hellrung, B., and Wirz, J.: Oxidation of Phenols by Triplet Aromatic Ketones in Aqueous Solution, J. Phys. Chem. A, 104, 1226–1232, 2000. Canonica, S., Kohn, T., Mac, M., Real, F. J., Wirz, J., and Von Gunten, U.: Photosensitizer Method to Determine Rate Constants for the Reaction of Carbonate Radical with Organic Compounds, Environ. Sci. Technol., 39, 9182–9188, 2005. Cantrell, W., Shaw, G., Cass, G. R., Chowdhury, Z., Hughes, L. S., Prather, K. A., Guazzotti, S. A., and Coffee, K. R.: Closure between aerosol particles and cloud condensation nuclei at Kaashidhoo Climate Observatory, J. Geophys. Res., 106, 28711–28718, 2001. Cape, J. N., Hamilton, R., and Heal, M. R.: Reactive uptake of ozone at simulated leaf surfaces: Implications for 'non–stomatal' ozone flux, Atmos. Environ., 43, 1116–1123, 2009. Cappa, C. D., Smith, J. D., Drisdell, W. S., Saykally, R. J., and Cohen, R. C.: Interpreting the H/D isotope fractionation of liquid water during evaporation without condensation, J. Phys. Chem. C, 111, 7011–7020, 2007. Cappa, C.D., Drisdell, W. S., Smith, J. D., Saykally, R. J., and Cohen, R. C.: Isotope Fractionation of Water during Evaporation without Condensation. J. Phys. Chem. B, 109, 24391–24400, 2005. Carignano, M. A., Jacob, M. M., and Avila, E. E.: On the uptake of ammonia by the water/vapor interface, J. Phys. Chem. A, 112, 3676–3679, 2008. Carravetta, V. and Clementi, E.: Water Water Interaction Potential – An Approximation Of The Electron Correlation Contribution By A Functional Of The Scf Density-Matrix, J. Chem. Phys., 81, 2646–2651, 1984. Carslaw, K. S., and Peter, T.: Uncertainties in reactive uptake coefficients for solid stratospheric particles.1. Surface Chemistry, Geophys. Res. Lett., 24, 1743–1746, 1997. Castro, A., Bhattacharyya, K., and Eisenthal, K. B.: Energetics Of Adsorption Of Neutral And Charged Molecules At The Air-Water-Interface By 2nd Harmonic-Generation – Hydrophobic And Solvation Effects, J. Chem. Phys., 95, 1310–1315, 1991. Chandler, D.: Statistical–mechanics of isomerization dynamics in liquids and transition–state approximation, J. Chem. Phys., 68, 2959–2970, 1978. Che, D. L., Smith, J. D., Leone, S. R., Ahmed, M., and Wilson, K. R.: Quantifying the reactive uptake of OH by organic aerosols in a continuous flow stirred tank reactor, Phys. Chem. Chem. Phys., 11, 7885–7895, 2009. Chuang, P. Y.: Measurement of the timescale of hygroscopic growth for atmospheric aerosols, J. Geophys. Res.-Atmos., 108, 4282, doi:10.1029/2002JD002757, 2003. Chughtai, A. R., Jassim, J. A., Peterson, J. H., Stedman, D. H., and Smith, D. M.: Spectroscopic And Solubility Characteristics Of Oxidized Soots, Aerosol Sci. Technol., 15, 112–126, 1991. Clegg, S. L., Seinfeld, J. H., and Brimblecombe, P.: Thermodynamic modelling of aqueous aerosols containing electrolytes and dissolved organic compounds, J. Aerosol. Sci., 32, 713–738, 2001. Clegg, S. M. and Abbatt, J. P. D.: Uptake of gas-phase SO<sub>2</sub> and H<sub>2</sub>O<sub>2</sub> by ice surfaces: dependence on partial pressure, temperature and surface acidity, J. Phys. Chem. A 105, 6630–6636, 2001. Clement, C. F., Kulmala, M., and Vesala, T.: Theoretical consideration on sticking probabilities, J. Aerosol Sci., 27, 869–882, 1996. Cilfford, D., Bartesis–Rausch, T. and Donaldson, D. J.: Suppression of aqueous surface hydrolysis by monolayers of short chain organic amphiphiles, Phys. Chem. Chem. Phys., 9, 1362––1369, 2007. Clifford, D. and Donaldson, D. J.: Direct experimental evidence for a heterogeneous reaction of ozone with bromide at the air-aqueous interface, J. Phys. Chem. A, 111, 9809–9814, 2007. Clifford, D., D. J. Donaldson, D. J., Brigante, M., D'Anna, B., and George, C.: Reactive uptake of ozone by chlorophyll at aqueous surfaces, Environ. Sci. Technol., 42, 1138–1143, 2008. Cooper, P. and Abbatt, J. P. D.: Heterogeneous Interactions of OH and HO<sub>2</sub> Radicals with Surfaces Characteristic of Atmospheric Particulate Matter, J. Phys. Chem., 100, 2249–2254, 1996. Cosman, L. M. and Bertram, A. K.: Reactive uptake of N2O5 on aqueous H2SO4 solutions coated with 1–component and 2-component monolayers, J. Phys. Chem. A, 112, 4625–4635, 2008. Cosman, L. M., Knopf, D. A., and Bertram, A. K.: N2O5 reactive uptake on aqueous sulfuric acid solutions coated with branched and straight-chain insoluble organic surfactants, J. Phys. Chem. A, 112, 2386–2396, 2008. Crowley, J. N., Ammann, M., Cox, R. A., Hynes, R. G., Jenkin, Me. E., Mellouki, A., Rossi, M. J., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume V – heterogeneous reactions on solid substrates, Atmos. Chem. Phys., 10, 9059–9223, doi:10.5194/acp-10-9059-2010, 2010. Cwiertny, D. M., Young, M. A., and Grassian, V. H.: Chemistry and photochemistry of mineral dust aerosol, Ann. Rev. Phys. Chem., 59, 27–51, 2008. D'Anna, B., Jammoul, A., George, C., Stemmler, K., Fahrni, S., Ammann, M., and Wisthaler, A.: Light–induced ozone depletion by humic acid films and submicron aerosol particles, J. Geophys. Res.–Atmos., 114, 12, D12301, doi:10.1029/2008jd011237, 2009. Dabkowski, J., Zagorska, I., Dabkowska, M., Koczorowski, Z., and Trasatti, S.: Adsorption of DMSO at the free surface of water: Surface excesses and surface potential shifts in the low concentration range, J. Chem. Soc.-Faraday Trans., 92, 3873–3878, 1996. Dang, L. X. and Chang, T. M.: Molecular dynamics study of water clusters, liquid, and liquid–vapor interface of water with many–body potentials, J. Chem. Phys., 106, 8149–8159, 1997. Dang, L. X. and Feller, D.: Molecular dynamics study of water-benzene interactions at the liquid/vapor interface of water, J. Phys. Chem. B, 104, 4403–4407, 2000. Dang, L. X. and Garrett, B. C.: Molecular mechanism of water and ammonia uptake by the liquid/vapor interface of water, Chem. Phys. Lett., 385, 309–313, 2004. Danckwerts, P. V.: Gas-Liquid Reactions, McGraw–Hill, New York, NY, USA, 276 pp., 1970. Davidovits, P., Hu, J. H., Worsnop, D. R., Zahniser, M. S., and Kolb, C. E.: Entry of Gas Molecules into Liquids, Faraday Discussions, 100, 65–82, 1995. Davidovits, P., Worsnop, D. R., Williams, L. R., Kolb, C. E., and Gershenzon, M.: Comment on "Mass accommodation coefficient of water: Molecular dynamics simulation and revised analysis of droplet train/flow reactor experiment", J. Phys. Chem. B, 109, 14742–14746, 2005. Davidovits, P., Worsnop, D. R., Jayne, J. T., Kolb, C. E., Winkler, P., Vrtala, A., Wagner, P. E., Kulmala, M., Lehtinen, K. E. J., Vesala, T. and Mozurkewich, M.: Mass accommodation coefficient of water vapor on liquid water, Geophys. Res. Lett. 31, L22111, doi:10.1029/2004GL020835, 2004. Davidovits, P., Kolb, C. E., Williams, L. R., Jayne, J. T., and Worsnop, D. R.: Mass Accommodation and Chemical Reactions at Gas–Liquid Interfaces, Chem. Rev., 106, 1323–1354, doi:10.1021/cr040366k, 2006. Davies, J. A. and Cox, R. A..: Kinetics of the Heterogeneous Reaction of HNO<sub>3</sub> with NaCl: Effect of Water Vapor, J. Phys. Chem. A, 102, 7631–7642, 1998. Davis, E. J.: A History and State-of-the-Art of Accommodation Coefficients, Atmos. Res., 82, 561–578, 2006. Davis, E. J.: Interpretation of Uptake Coefficient Data Obtained with Flow Tubes, J. Phys. Chem. A, 112, 1922–1932, 2008. Decesari, S., Facchini, M. C., Matta, E., Mircea, M., Fuzzi, S., Chughtai, A. R., and Smith, D. M..: Water soluble organic compounds formed by oxidation of soot, Atmos. Environ., 36, 1827–1832, 2002. de Gouw, J. A. and Lovejoy, E. R.: Reactive uptake of ozone by liquid organic compounds, Geophys. Res. Lett., 25, 931–934, 1998. Delval, C., Flückiger, B., and Rossi, M. J.: The rate of water vapor evaporation from ice substrates in the presence of HCl and HBr: implications for the lifetime of atmospheric ice particles, Atmos. Chem. Phys. , 3, 1131–1145, 2003. Delval, C. and Rossi, M. J.: The kinetics of condensation and evaporation of H<sub>2</sub>O from pure ice in the range 173–223 K: A quartz crystal microbalance study, Phys. Chem. Chem. Phys., 6, 4665–4676, 2004. Demou, E. and Donaldson, D. J.: Adsorption of atmospheric gases at the air-water interface. 4: The influence of salts, J. Phys. Chem. A, 106, 982–987, 2002. Dinar, E., Anttila, T., and Rudich, Y.: CCN activity and hygroscopic growth of organic aerosols following reactive uptake of ammonia, Environ. Sci. Technol. 42, 793–799, 2008. Djikaev, Y. S. and Tabazadeh, A.: Effect of adsorption on the uptake of organic trace gas by cloud droplets, J. Geophys. Res.-Atmos., 108, 4689, doi:10.1029/2003JD003741, 2003. Docherty, K. S. and Ziemann, P. J.: Reaction of oleic acid particles with NO<sub>3</sub> radicals: Products, mechanism, and implications for radical-initiated organic aerosol oxidation, J. Phys. Chem. A, 110, 3567–3577, 2006. Donaldson, D. J., Guest, J. A., and Goh, M. C.: Evidence for Adsorbed SO<sub>2</sub> at the Aqueous Air Interface, J. Phys. Chem., 99, 9313–9315, 1995. Donaldson, D. J.: Adsorption of atmospheric gases at the air-water interface. I. NH<sub>3</sub>, J. Phys. Chem. A, 103, 62–70, 1999. Donaldson, D. J. and Anderson, D.: Adsorption of atmospheric gases at the air-water interface. 2. C-1-C-4 alcohols, acids, and acetone, J. Phys. Chem. A, 103, 871–876, 1999. Donaldson, D. J., Mmereki, B. T., Chaudhuri, S. R., Handley, S., and Oh, M.: Uptake and reaction of atmospheric organic vapours on organic films, Faraday Discuss., 130, 227–239, 2005. Donaldson, D. J. and Vaida, V.: The influence of organic films at the air–aqueous boundary on atmospheric processes, Chem. Rev., 106, 1445–1461, 2006. Donaldson, D. J. and Valsaraj, K. T.: Adsorption and Reaction of Trace Gas–Phase Organic Compounds on Atmospheric Water Surfaces: A Critical Review, Environ. Sci. Technol., 44, 865–873, 2010. Drisdell, W. S., Cappa, C. D., Smith, J. D., Saykally, R. J., and Cohen, R. C.: Determination of the evaporation coefficient of D2O, Atmos. Chem. Phys., 8, 6699–6706, doi:10.5194/acp-8-6699-2008, 2008. Eliason, T. L., Aloisio, S., Donaldson, D. J., Cziczo, D. J., and Vaida, V.: Processing of unsaturated organic acid films and aerosols by ozone, Atmos. Environ., 37, 2207–2219, 2003. Engelhart, G. J., Asa-Awuku, A., Nenes, A., and Pandis, S. N.: CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol, Atmos. Chem. Phys., 8, 3937–3949, 2008. Esteve, W., Budzinski, H., and Villenave, E. : Relative rate constants for the heterogeneous reactions of NO<sub>2</sub> and OH radicals with polycyclic aromatic hydrocarbons adsorbed on carbonaceous particles. Part 2: PAHs adsorbed on diesel particulate exhaust SRM 1650a, Atmos. Environ., 40, 201–211, 2006. Ewald, P. P.: The calculation of optical and electrostatic grid potential, Ann. Phys.–Berlin, 64, 253–287, 1921. Falkovich, A. H. and Rudich, Y..: Analysis of semivolatile organic compounds in atmospheric aerosols by direct sample introduction thermal desorption GC/MS, Environ. Sci. Technol., 35, 2326–2333, 2001. Falkovich, A. H., Schkolnik, G., Ganor, E., and Rudich, Y.: Adsorption of organic compounds pertinent to urban environments onto mineral dust particles, J. Geophys. Res., 109, D01201, doi:1029/2003JD003919, 2004. Ferry, D., Suzanne, J., Nitsche, S., Popovitcheva, O. B., and Shonija, N. K.: Water adsorption and dynamics on kerosene soot under atmospheric conditions, J. Geophys. Res.-Atmos., 107(D23), doi:10.1029/2002JD002459, 2002. Finlayson-Pitts, B. J.: The tropospheric chemistry of sea–salt: A molecular level view of the chemistry of NaCl and NaBr, Chem. Rev., 103, 4801–4822, 2003. Finlayson-Pitts, B. J. and Pitts Jr. J. N.: Chemistry of the Upper and Lower Atmosphere: Theory, Experiments, and Applications, Academic Press, San Diego, CA, USA, 969 pp., 1999. Folkers, M., Mentel, T. H., and Wahner, A.: Influence of an organic coating on the reactivity of aqueous aerosols probed by the heterogeneous hydrolysis of N<sub>2</sub>O$_5$, Geophys. Res. Lett., 30, 1644, doi:10.1029/2003GL017168, 2003. 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. Fountoukis C., Nenes, A., Meskhidze, N., et al.: Aerosol-cloud drop concentration closure for clouds sampled during the International Consortium for Atmospheric Research on Transport and Transformation 2004 campaign, J. Geophys. Res., 112, D10S30, doi:10.1029/2006JD007272, 2007. Fried, A., Henry, B. E., Calvert, J. G., and Mozurkewich, M.: The Reaction Probability of N<sub>2</sub>O$_5$ with Sulfuric-Acid Aerosols at Stratospheric Temperatures and Compositions, J. Geophys. Res.-Atmos., 99, 3517–3532, 1994. Frinak, E. and Abbatt, J. P. D.: Br<sub>2</sub> production from the heterogeneous reaction of gas–phase OH with aqueous salt solutions: Impacts of acidity, halide concentration and organic surfactants, J. Phys. Chem. A, 110, 10456–10464, 2006. Frinak, E. K., Wermeille, S. J., Mashburn, C. D., Tolbert, M. A., and Pursell, C. J.: Heterogeneous reaction of gaseous nitric acid on γ –phase iron(III)oxide, J. Phys. Chem., 108, 1560–1566, 2004. Fuchs, N. A. and Sutugin, A. G.: Highly Dispersed Aerosols, Ann Arbor Science Publishers, Ann Arbor, MI, USA, 105 pp., 1970. % %Fuzzi, S., and Andreae, M. O., et al.: Critical Assessment of the Current %State of Scientific Knowledge, Terminology, and Research Needs Concerning %the Role of Organic Aerosols in the Atmosphere, Climate, and Global Change, %Atmos. Chem. Phys., 6, 2017–2038, doi:10.5194/acp-6-2017-2006, 2006. Fuzzi, S., Andreae, M. O., Huebert, B. J., Kulmala, M., Bond, T. C., Boy, M., Doherty, S. J., Guenther, A., Kanakidou, M., Kawamura, K., Kerminen, V.-M., Lohmann, U., Russell, L. M., and Pöschl, U.: Critical Assessment of the Current State of Scientific Knowledge, Terminology, and Research Needs Concerning the Role of Organic Aerosols in the Atmosphere, Climate, and Global Change, Atmos. Chem. Phys., 6, 2017–2038, doi:10.5194/acp-6-2017-2006, 2006. Gao, R. S., Popp, P. J., Fahey, D. W., Marcy, T. P., Herman, R. L., Weinstock, E. M., Baumgardner, D. G., Garrett, T. J., Rosenlof, K. H., Thompson, T. L., Bui, P. T., Ridley, B. A., Wofsy, S. C., Toon, O. B., Tolbert, M. A., Kärcher, B., Peter, T., Hudson, P. K., Weinheimer, A. J., and Heymsfield, A. J.: Evidence that nitric acid increases relative humidity in low-temperature Cirrus clouds, Science, 303, 516–520, 2004. Garrett, B. C., Schenter, G. K., and Morita, A.: Molecular simulations of the transport of molecules across the liquid/vapor interface of water, Chem. Rev., 106, 1355–1374, 2006. Gelencser, A., Hoffer, A., Kiss, G., Tombacz, E., Kurdi, R., and Bencze, L.: In–situ Formation of Light-Absorbing Organic Matter in Cloud Water, J. Atmos. Chem., 45, 25–33, 2003a. Gelencser, A., Hoffer, A., Kiss, G., Tombacz, E., Kurdi, R., and Bencze, L.: In-situ Formation of Light-Absorbing Organic Matter in Cloud Water, J. Atmos. Chem., 45, 25–33, 2003b. George, C., Ponche, J. L., Mirabel, P., Behnke, W., Scheer, V., and Zetzsch, C.: Study of the uptake of N<sub>2</sub>O$_5$ by water and NaCl solutions, J. Phys. Chem., 98, 8780–8784, 1994. George, C., Strekowski, R. S., Kleffmann, J., Stemmler, K., and Ammann, M.: Photoenhanced uptake of gaseous NO2 on solid-organic compounds: a photochemical source of HONO?, Faraday Discuss., 130, 195–210, doi:10.1039/b417888m, 2005. George, I. J., Vlasenko, A., Slowik, J. G., Broekhuizen, K., and Abbatt, J. P. D.: Heterogeneous oxidation of saturated organic aerosols by hydroxyl radicals: Uptake kinetics, condensed-phase products, and particle size change, Atmos. Chem. Phys., 7, 4187–4201, doi:10.5194/acp-7-4187-2007, 2007. George, I, J. Slowik, J. G., and Abbatt, J. P. D.: Chemical aging of ambient organic aerosol from heterogeneous reaction with hydroxyl radicals, Geophys. Res. Lett., 35, L13811, doi:10.1029/2008GL033884, 2008. Ghosal, S., Hemminger, J. C., Bluhm, H., Mun, B. S., Hebenstreit, E. L. D., Ketteler, G., Ogletree, D. F., Requejo, F. G., and Salmeron, M.: Electron Spectroscopy of Aqueous Solution Interfaces Reveals Surface Enhancement of Halides, Science, 307, 563–566, 2005. Giese, B., Napp, M., Jacques, O., Boudebous, H., Taylor, A. M., and Wirz, J.: Multistep electron transfer in oligopeptides: Direct observation of radical cation intermediates, Angew. Chem. Int. Ed., 44, 4073–4075, 2005. Girardet, C. and Toubin, C.: Molecular atmospheric pollutant adsorption on ice: a theoretical survey, Surf. Sci. Rep., 44, 159–238, 2001. Golden, D. M., Spokes, G. N., and Benson, S. W.: Very Low Pressure Pyrolysis (VLPP); a versatile kinetic method, Angew. Chem., 85, 602–614, 1973. Gomez, A. L., Park, J., Walser, M. L., Lin, A., and Nizkorodov, S. A.: UV photodissociation spectroscopy of oxidized undecylenic acid films, J. Phys. Chem. A, 110, 3584–3592, 2006. Gonzalez-Perez, J. A., Gonzalez–Vila, F. J., Almendros, G., and Knicker, H.: The effect of fire on soil organic matter – a review, Environ. Int., 30, 855–870, 2004. Goodman, A. I., Bernard, E. T., and Grassian, V. H.: Spectroscopic study of nitric acid and water adsorption on oxide particles: enhanced nitric acid uptake kinetics in the presence of adsorbed water, J. Phys. Chem. A 105, 6443–6457, 2001. Gopalakrishnan, S., Liu, D. F., Allen, H. C., Kuo, M., and Shultz, M. J.: Vibrational spectroscopic studies of aqueous interfaces: Salts, acids, bases, and nanodrops, Chem. Rev., 106, 1155–1175, 2006. 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. Gross, S. and Bertram, A.: Reactive uptake of NO<sub>3</sub>, N<sub>2</sub>O$_5$, NO<sub>2</sub>, HNO<sub>3</sub> and O<sub>3</sub> on three types of polycyclic hydrocarbon surfaces, J. Phys. Chem. A, 112, 3104–3113, 2008. Gross, S., R. Iannone, Song, X., and Bertram, A.: Reactive uptake studies of NO<sub>3</sub> and N<sub>2</sub>O$_5$ on alkenoic acid, alkanoate, and polyalcohol substrates to probe nighttime aerosol chemistry, Phys. Chem. Chem. Phys., 11, 7792–7803, 2009. Grote, R. T. and Hynes, J. T.: G-H theory, J. Chem. Phys., 73, 2715–2732, 1980. Guimbaud, C., Arens, F., Gutzwiller, L., Gaggeler, H. W., and Ammann, M.: Uptake of HNO<sub>3</sub> to deliquescent sea-salt particles: a study using the short-lived radioactive isotope tracer N-13, Atmos. Chem. Phys., 2, 249–257, 2002. Gustafsson R. J., Orlov, A., Badger, C. L., Griffiths, P. T., Cox, R. A., and Lambert, R. M.: A comprehensive evaluation of water uptake on atmospherically relevant mineral surfaces: DRIFT spectroscopy, thermogravimetric analysis and aerosol growth measurements, Atmos. Chem. Phys., 5, 3415–3421, 2005. Gustafsson, R. J., Orlov, A., Griffiths, P. T., Cox, R. A., and Lambert, R. M.: Reduction of NO<sub>2</sub> to nitrous acid on illuminated titanium dioxide aerosol surfaces: implications for photocatalysis and atmospheric chemistry, Chem. Comm., 37, 3936–3938, 2006. Haag, W. R., Hoigne, J., Gassman, E., and Braun, A. M.: Singlet Oxygen in Surface Waters .2. Quantum Yields of Its Production by Some Natural Humic Materials as a Function of Wavelength, Chemosphere, 13, 641–650, 1984. Hallquist, M., Stewart, D. J., Baker, J., and Cox, R. A.: Hydrolysis of N<sub>2</sub>O$_5$ on sulphuric acid aerosols, J. Phys. Chem. A., 104, 3984–3990, 2000. Hallquist, M., Stewart, D. J., Stephenson, S. K., and Cox, R. A.: Hydrolysis of N2O5 on sub–micron sulphate aerosols, Phys. Chem. Chem. Phys., 5, 3453–3463, 2003. Hanisch, F. and Crowley, J. N.: Heterogeneous reactivity of gaseous nitric acid on Al2O3, CaCO3 and atmospheric dust samples: A Knudsen cell study, J. Phys. Chem. A 105, 3096–3106, 2001a. Hanisch, F. and Crowley, J. N.: The heterogeneous reactivity of gaseous nitric acid on authentic mineral dust samples, and on individual mineral and clay mineral components, Phys. Chem. Chem. Phys., 3, 2474–2482, 2001b. Hanisch, F. and Crowley, J. N.: Ozone: decomposition on Saharan dust: an experimental investigation, Atmos. Chem. Phys.,~3, 119–130, 2003. Hanson, D. and Mauersberger, K.: HCl/H<sub>2</sub>O Solid Phase Vapor Pressures and HCl Solubility in Ice, J. Phys. Chem., 94, 4700–4705, 1990. Hanson, D., Burkholder, J. B., Howard, C. J., and Ravishankara, A. R.: Measurement of OH and HO<sub>2</sub> Radical Uptake Coefficients on Water and Sulfuric Acid Surfaces, J. Phys. Chem., 96, 4979–4985, 1992. Hanson, D. R. and Lovejoy, E. R.: The reaction of ClONO<sub>2</sub> with submicometer sulfuric acid aerosol, Science, 267, 1326–1328, 1995. Hanson, D. R. and Lovejoy, E. R.: Heterogeneous reactions in liquid sulfuric acid: HOCl + HCl as a model system, J. Phys. Chem., 100, 6397–6405, 1996. Hanson, D. R. and Kosciuch, E.: Reply to "Comment on "The NH<sub>3</sub> mass accommodation coefficient for uptake onto sulfuric acid solutions"," J. Phys. Chem. A., 108, 8549–8551, 2004. Hanson, D. R.: Surface specific reactions on liquids, J. Phys. Chem. B., 101, 4998–5001, 1997a. Hanson, D. R.: Reaction of N<sub>2</sub>O$_5$ with H<sub>2</sub>O on bulk liquids and on particles and the effect of dissolved HNO<sub>3</sub>, Geophys, Res. Lett., 24, 1087–1090, 1997b. Hanson, D. R.: Reaction of ClONO<sub>2</sub> with H<sub>2</sub>O and HCl in sulfuric acid and HNO<sub>3</sub>/H<sub>2</sub>SO<sub>4</sub>/H<sub>2</sub>O mixtures, J. Phys. Chem. A., 102, 4794–4807, 1998. Hartkopf, A. and Karger, B. L.: Study of Interfacial Properties of Water by Gas–Chromatography, Acc. Chem. Res., 6, 209–216, 1973. Hearn, J. D. and Smith, G. D.: A chemical ionization mass spectrometry method for the online analysis of organic aerosols, Anal. Chem., 76, 2820–2826, 2004. Hearn, J. D., Lovett, A. J., and Smith, G. D.: Ozonolysis of oleic acid particles: evidence for a surface reaction and secondary reactions involving Criegee intermediates, Phys. Chem. Chem. Phys., 7, 501–511, 2005. Henson, B. F., Wilson, K. R., Robinson, J. M., Noble, C. A., Casson, J. L., and Worsnop, D. R.: Experimental isotherms of HCl on H<sub>2</sub>O ice under stratospheric conditions: connections between bulk and interfacial thermodynamics, J. Chem. Phys., 121, 8486–8499., 2004. Hessberg von, P., Pouvesle, N., Winkler, A. K., Schuster, G., and Crowley, J. N.: Interaction of formic and acetic acid with ice surfaces between 187 and 227 K. Investigation of single species- and competitive adsorption, Phys. Chem. Chem. Phys., 10, 2345–2355, 2008. Hoff, J. T., Mackay, D., Gillham, R., and Shiu, W. Y.: Partitioning of Organic-Chemicals at the Air–Water–Interface in Environmental Systems, Environ. Sci. Technol., 27, 2174–2180, 1993. Hu, J. H., Shi, Q., Davidovits, P., Worsnop, D. R., Zahniser, M. S., and Kolb, C. E.: Reactive Uptake of Cl2(G) and Br2(G) by Aqueous Surfaces as a Function of Br– and I– Ion Concentration – the Effect of Chemical-Reaction at the Interface, J. Phys. Chem., 99, 8768–8776, 1995. Hu, J. H. and Abbatt, J. P. D.: Reaction Probabilities for N<sub>2</sub>O$_5$ Hydrolysis on Sulfuric Acid and Ammonium Sulfate Aerosols at Room Temperature, J. Phys. Chem. A, 101, 871–878, 1997. Huff, A. K. and Abbatt, J. P. D.: Gas-Phase Br<sub>2</sub> Production in Heterogeneous Reactions of Cl2, HOCl and BrCl with Halide-Ice Surfaces, J. Phys. Chem. A., 104, 7284–7293, 2000. Huff, A. K. and Abbatt, J. P. D.: Kinetics and Product Yields in the Heterogeneous Reactions of HOBr with Simulated Sea Ice Surfaces, J. Phys. Chem. A., 106, 5279–5287, 2002. Hunt, S. W., Roeselová, M., Wang, W., Wingen, L. M., Knipping, E. M., Tobias, D. J., Dabdub, D., and Finlayson-Pitts, B. J.: Formation of Molecular Bromine from the Reaction of Ozone with Deliquesced NaBr Aerosol: Evidence for Interface Chemistry, J. Phys. Chem. A., 108, 11559–11572, 2004. Huntzicker, J. J., Cary, R. A., and Ling, C. S.: Neutralization of Sulfuric Acid Aerosol by Ammonia, Environ. Sci. Technol., 14, 819–824, 1980. Huthwelker, T., Ammann, M., and Peter, T.: The uptake of acidic gases on ice,~Chem. Rev., 106, 1375–1444, 1980, 2006. Hynes, J. T.: The theory of reactions in solution, in: Theory of Chemical Reaction Dynamics, edited by: Baer, M., CRC Press, Boca Raton, FL, USA, 171–234, 1985. Iinuma, Y., Boge, O. Kahnt, A., et al.: Laboratory chamber studies on the formation of organosulfates from reactive uptake of monoterpene oxides, Phys. Chem. Chem. Phys., 11, 7985–7997, 2009. Ismail, A. E., Grest, G. S., and Stevens, M. J.: Capillary waves at the liquid–vapor interface and the surface tension of water, J. Chem. Phys., 125, 014702, doi:10.1063/1.2209240, 2006. IUPAC: IUPAC Subcommittee for Gas Kinetic Data Evaluation; http://www.iupac-kinetic.ch.cam.ac.uk/ International Union of Pure and Applied Chemistry, 2009. Jammoul, A., Gligorovski, S., George, C., and D'Anna, B.: Photosensitized heterogeneous chemistry of ozone on organic films, J. Phys. Chem. A, 112, 1268–1276, doi:10.1021/jp074348t, 2008. Jang, M., Czoschke, N. M., Lee, S., and Kamens, R. M.: Heterogeneous Atmospheric Aerosol Production by Acid-Catalyzed Particle-Phase Reactions, Science, 298, 814–817, 2002. Jayne, J. T., Davidovits, P., Worsnop, D. R., Zahniser, M. S., and Kolb, C. E.: Uptake of SO<sub>2</sub>(g) by aqueous surfaces as a function of PH – The effect of chemical-reaction at the interface, J. Phys. Chem., 94, 6041–6048, 1990. Jayne, J. T., Duan, S. X., Davidovits, P., Worsnop, D. R., Zahniser, M. S., and Kolb, C. E.: Uptake of Gas-Phase Alcohol and Organic–Acid Molecules by Water Surfaces, J. Phys. Chem., 95, 6329–6336, 1991. Jayne, J.T., Duan, S. X., Davidovits, P., Worsnop, D. R., Zahniser, M. S., and Kolb, C. E.: Uptake of gas–phase aldehydes by water surfaces, J. Phys. Chem., 96, 5452–5460, 1992. Jones, C. C, Chughtai, A. R., Murugaverl, B., and Smith, D. M.: Effects of air/fuel combustion ratio on the polycyclic aromatic hydrocarbon content of carbonaceous soots from selected fuels, Carbon, 42, 2471–2484, 2004. Jorgensen, W. L., Chandrasekhar, J., Madura, J. D., Impey, R. W., and Klein, M. L.: Comparison of Simple Potential Functions for Simulating Liquid Water, J. Chem. Phys., 79, 926–935, 1983. Jungwirth, P. and Tobias, D. J.: Specific ion effects at the air/water interface, Chem. Rev., 106, 1259–1281, 2006. Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A. S. H., Fisseha, R.,Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of Polymers as Major Components of Atmospheric Organic Aerosols, Science, Washington DC, USA, 303, 1659–1662, 2004. Kane, S. M., Caloz, F., and Leu, M.–T.: Heterogeneous Uptake of Gaseous N<sub>2</sub>O$_5$ by (NH$_4)_2$SO<sub>4</sub>, NH<sub>4</sub>HSO<sub>4</sub>, and H<sub>2</sub>SO<sub>4</sub> Aerosols, J. Phys. Chem. A 105, 6465–6470, 2001. Karagulian, F. and Rossi, M. J.: The heterogeneous kinetics of NO<sub>3</sub> on atmospheric mineral dust surrogates, Phys. Chem. Chem. Phys. , 7, 3150–3162, 2005. Karagulian, F., Santschi, C., and Rossi, M. J.: The heterogeneous chemical kinetics of N<sub>2</sub>O$_5$ on CaCO<sub>3</sub> and other atmospheric mineral dust surrogates, Atmos. Chem. Phys., 6, 1373–1388, doi:10.5194/acp-6-1373-2006, 2006a. Karagulian, F. and Rossi, M. J.: The heterogeneous decomposition of ozone on atmospheric mineral dust surrogates at ambient temperatures, Int. J. Chem. Kin., 38, 407–419, 2006b. Karagulian, F. and Rossi, M. J.: Heterogeneous chemistry of the NO<sub>3</sub> free radical and N<sub>2</sub>O$_5$ on decane flame soot at ambient temperature: Reaction products and kinetics, J. Phys. Chem. A, 111, 1914–1926, 2007. Karpovich, D. S. and Ray, D.: Adsorption of dimethyl sulfoxide to the liquid/vapor interface of water and the thermochemistry of transport across the interface, J. Phys. Chem. B, 102, 649–652, 1998. Katrib, Y., Le Calve, S., and Mirabel, P.: Uptake measurements of dibasic esters by water droplets and determination of their Henry's law constants, J. Phys. Chem. A, 107, 11433–11439, 2003. Katrib, Y., Martin, S. T., Hung, H. M., Rudich, Y., Zhang, H. Z., Slowik, J. G., Davidovits, P., Jayne, J. T., and Worsnop, D. R.: Products and mechanisms of ozone reactions with oleic acid for aerosol particles having core–shell morphologies, J. Phys. Chem. A, 108, 6686–6695, 2004. Katrib, Y., Biskos, G., Buseck, P. R., Davidovits, P., Jayne, J. T., Mochida, M., Wise, M. E., Worsnop, D. R., and Martin, S. T.: Ozonolysis of mixed oleic-acid/stearic-acid particles: Reaction kinetics and chemical morphology, J. Phys. Chem. A, 109, 10910–10919, 2005a. Katrib, Y., Martin, S. T., Rudich, Y., Davidovits, P., Jayne, J. T., and Worsnop, D. R.: Density changes of aerosol particles as a result of chemical reaction, Atmos. Chem. Phys., 5, 275–291, doi:10.5194/acp-5-275-2005, 2005b. Kemball, C. and Rideal, E. K.: The Adsorption of Vapours on Mercury .1. Non–Polar Substances, Proc. Roy. Soc. Lond. Math. Phys., 187, 53–73, 1946. King, D. A. and Wells, M. G.: Molecular beam investigation of adsorption kinetics on bulk metal targets: Nitrogen on tungsten, Surf. Sci., 29, 454–482, 1972. Kleffmann, J., Becker, K. H., and Lackhoff, M., et al. : Heterogeneous conversion of NO<sub>2</sub> on carbonaceous surfaces, Phys. Chem. Chem. Phys., 1, 5443–5450, 1999. Knopf, D. A., Anthony, L. M., and Bertram, A. K.: Reactive uptake of O<sub>3</sub> by multicomponent and multiphase mixtures containing oleic acid, J. Phys. Chem. A, 109, 5579–5589, 2005. Knopf, D. A., Mak, J., Gross, S., and Bertram, A. K.: Does Atmospheric Processing of Saturated Hydrocarbon Surfaces by NO Lead to Volatilization? Geophys. Res. Lett., 33, L17816, doi:10.1029/2006GL026884, 2006. Kolb, C. E., Worsnop, D., Zahniser, M. S., Davidovits, P., Keyser, L. F., Leu, M.–T., Molina, M. J., Hanson, D. R., Ravishankara, A. R., Williams, L. R., and Tolbert, M. A.: Laboratory Studies of Atmospheric Heterogeneous Chemistry, in: Progress and Problems in Atmospheric Chemistry, edited by: Barker, J. R., Adv. Series Phys. Chem., 3 C.-Y. Ng, series editor, World Scientific, Singapore, 771–875, 1995. Krieger, U. K., Huthwelker, T., Daniel, C., Weers, U., Peter, T., and Lanford, W. A.: Rutherford Backscattering to Study the Near–Surface Region of Volatile Liquids and Solids, Science, 295, 1048–1050, 2002. Krivacsy, Z., Kiss, G., Varga, B., Galambos, I., Sarvari, Z., Gelencser, A., Molnar, A., Fuzzi, S., Facchini, M. C., Zappoli, S., Andracchio, A., Alsberg, T., Hansson, H. C., and Persson, L.: Study of humic-like substances in fog and interstitial aerosol by size–exclusion chromatography and capillary electrophoresis, Atmos. Environ., 34, 4273–4281, 2000. Kulmala, M. and Vesala, T.: Condensation in the Continuum Regime, J. Aerosol Sci., 22, 337–346, 1991. Kulmala, M., Vesala, T., and Wagner, P. E.: An analytical expression for the rate of binary condensational growth, Proc. R. Soc. Lond. A, 441, 589–605, 1993a. Kulmala, M., Laaksonen, A., Korhonen, P., Vesala, T., Ahonen, T., and Barrett, J. C.: The effect of atmospheric nitric acid vapour on CCN activation, J. Geophys Res., 98, 22949–22958, 1993b. Kulmala, M. and Wagner, P. E.: Mass accommodation and uptake coefficients – a quantitative comparison, J. Aerosol Sci., 32, 833–841, 2001. Kuo, I. F. W. and Mundy, C. J.: An ab initio molecular dynamics study of the aqueous liquid-vapor interface, Science, 303, 658–660, 2004. Kwamena, N. O. A., Thornton, J. A., and Abbatt, J. P. D.: Kinetics of surface-bound benzo[α]pyrene and ozone on solid organic and salt aerosols, J. Phys. Chem. A, 108, 11626–11634, 2004. Kwamena, N. O. A., Earp, M. E., Young, C. J., and Abbatt, J. P. D.: Kinetic and product yield study of the heterogeneous gas–surface reaction of anthracene and ozone, J. Phys. Chem. A, 110, 3638–3646, 2006. Kwan, A. J., Crounse, J. D., Clarke, A. D., Shinozuka, Y., Anderson, B. E., Crawford, J. H., Avery, M. A., McNaughton, C. S., Brune, W. H., Singh, H. B., and Wennberg, P. O.: On the Flux of Oxygenated Volatile Organic Compounds from Organic Aerosol Oxidation, Geophys. Res. Lett. 33, L15815, doi:10.1029/2006GL026144, 2006. Laaksonen, A., Vesala. T., Kulmala, M., Winkler, P. M., and Wagner, P. E.: Commentary on cloud modelling and the mass accommodation coefficient of water, Atmos. Chem. Phys., 5, 461–464, doi:10.5194/acp-5-461-2005, 2005. Lambe, A. T., Miracolo, M. A., Hennigan, C. J., Robinson, A. L., and Donahue, N. M.: Effective Rate Constants and Uptake Coefficients for the Reactions of Organic Molecular Markers ($n$–Alkanes, Hopanes, and Steranes) in Motor Oil and Diesel Primary Organic Aerosols with Hydroxyl, Environ. Sci. Technol., 43, 8794–8800, 2009. Lammel, G. and Novakov, T.: Water Nucleation Properties Of Carbon–Black And Diesel Soot particles, Atmos. Environ., 29, 813–823, 1995. Laskin, A., Wang, H., Robertson, W. H., Cowin, J. P., Ezell, M. J., and Finlayson-Pitts, B. J.: A New Approach to Determining Gas-Particle Reaction Probabilities and Application to the Heterogeneous Reaction of Deliquesced Sodium Chloride Particles with Gas–Phase Hydroxyl Radicals, J. Phys. Chem. A, 110 10619–10627, 2006. Lawrence, J. R., Glass, S. V., and Nathanson, G. M.: Evaporation of Water through Butanol Films at the Surface of Supercooled Sulfuric Acid, J. Phys. Chem. A, 109, 7449–7457, 2005a. Lawrence, J. R., Glass, S. V., Park, S.-C., and Nathanson, G. M.: Surfactant Control of Gas Uptake: Effect of Butanol Films on HCl and HBr Entry into Supercooled Sulfuric Acid, J. Phys. Chem. A, 109, 7458–7465, 2005b. Lee, C. Y. and Scott, H. L.: The Surface-Tension Of Water – A Monte-Carlo Calculation Using An Umbrella Sampling Algorithm, J. Chem. Phys., 73, 4591–4596, 1980. Lemberg, H. L. and Stillinger, F. H.: Central-Force Model For Liquid Water, J. Chem. Phys., 62, 1677–1690, 1975. Li, L., Chen, Z. M., Zhang, Y. H., Zhu, T., Li, J. L. and Ding, J.: Kinetics and mechanism of heterogeneous oxidation of sulfur dioxide by ozone on surface of calcium carbonate, Atmos. Chem. Phys., 6, 2453–2464, doi:10.5194/acp-6-2453-2006, 2006. Li, Y., Davidovits, P., Shi, Q., Jayne, J., Kolb, C., and Worsnop, D.: Mass and Thermal Accommodation Coefficients of H<sub>2</sub>O(g) on Liquid Water as a Function of Temperature, J. Phys. Chem. A, 105, 10627–10634, 2001. Lie, G. C., Clementi, E., and Yoshimine, M.: Study of the structure of molecular complexes. XIII. Monte Carlo simulation of liquid water with a configuration interaction pair potential, J. Chem. Phys., 64, 2314–2323, 1976. Lie, G. C., Grigoras, S., Dang, L. X., Yang, D. Y., and McLean, A. D.: Monte–Carlo Simulation of the Liquid–Vapor Interface of Water Using an Ab–Initio Potential, J. Chem. Phys., 99, 3933–3937, 1993. Liu, Y., Gibson, E. R., Cain, J. P., Wang, H., Grassian, V. H., and Laskin, A.: Kinetics of Heterogeneous Reaction of CaCO<sub>3</sub> Particles with Gaseous HNO<sub>3</sub> over a Wide Range of Humidity, J. Phys. Chem. A, 112, 1561–1571, 2008. Livingston, F. E. and George, S. M.: Effect of HNO<sub>3</sub> and HCl on D<sub>2</sub>O Desorption Kinetics from Crystalline D<sub>2</sub>O Ice, J. Phys. Chem. A, 102, 10280–10288, 1998. Longfellow, C. A., Ravishankara, A. R., Hanson, D. R., et al.: Reactive and nonreactive uptake on hydrocarbon soot: HNO<sub>3</sub>, O<sub>3</sub>, and N<sub>2</sub>O$_5$, J. Geophys. Res.-Atmos., 105, 24345–24350, 2000. Lu, H., McCartney, S. A., Chonde, M., Smyla, D., and Sadtchenko, V.: Fast thermal desorption spectroscopy study of morphology and vaporization kinetics of polycrystalline ice films, J. Chem. Phys., 125, 044709, doi:10.1063/1.2212395, 2006. Magee, N., Moyle, A. M., and Lamb, D.: Experimental determination of the deposition coefficient of small cirrus–like ice crystals near −50 °C, Geopyhs. Res. Lett., 33, L17813, doi:10.1029/2006GL026665, 2006. Magi, L., Schweitzer, F., Pallares, C., Cherif, S., Mirabel, P., and George, C.: Investigation of the uptake rate of ozone and methyl hydroperoxide by water surfaces, J. Phys. Chem. A., 101, 4943–4949, 1997. Mahiuddin, S., Minofar, B., Borah, J. M., Das, M. R., and Jungwirth, P.: Propensities of oxalic, citric, succinic, and maleic acids for the aqueous solution/vapour interface: Surface tension measurements and molecular dynamics simulations, Chem. Phys. Lett., 462, 217–221, 2008. Mashburn, C. D., Frinak, E. K., and Tolbert, M. A.: Heterogeneous uptake of nitric acid on Na–montmorillonite clay as a function of relative humidity, J. Geophys. Res., 111, D15213, doi:10.1029/2005JD006525, 2006. Matsumoto, M. and Kataoka, Y.: Study on Liquid Vapor Interface of Water .1. Simulational Results of Thermodynamic Properties and Orientational Structure, J. Chem. Phys., 88, 3233–3245, 1988. Matsumoto, M., Takaoka, Y., and Kataoka, Y.: Liquid Vapor Interface of Water-Methanol Mixture .1. Computer-Simulation, J. Chem. Phys., 98, 1464–1472, 1993. Matsumoto, M.: Molecular dynamics simulation of interphase transport at liquid surfaces, Fluid Phase Equilibria, 125, 195–203, 1996. Matsuoka, O., Clementi, E., and Yoshimine, M.: CI study of the water dimer potential surface, J. Chem. Phys., 64, 1351–1362, 1976. McFiggans, Artaxo, G. P., Baltensperger, U., Coe, H., Facchini, M. C., Feingold, G., Fuzzi, S., Gysel, M., Laaksonen, A., Lohmann, U., Mentel, T. F., Murphy, D. M., O'Dowd, C. D., Snider, J. R., and Weingartner, E.: The Effect of Physical and Chemical Aerosol Properties on Warm Cloud Droplet Activation, Atmos. Chem. Phys., 6, 2593–2649, doi:10.5194/acp-6-2593, -2006m 2006. McMurry, P. H., Takano, H., and Anderson, G. R.: Study of the Ammonia (Gas)–Sulfuric Acid (Aerosol) Reaction Rate, Environ. Sci. Technol., 17, 347–352, 1983. McNeill, V. F., Loerting, T., Geiger, F. M., Trout, B. L., and Molina, M. J.: Hydrogen chloride-induced surface disordering on ice, Proc. Natl. Acad. Sci. USA, 103, 9422–9427, 2006a. 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<sub>2</sub>O$_5$ to aqueous aerosol, Atm. Chem. Phys., 6, 1635–1644, 2006b. McNeill, V. F, Geiger, F. M., Loerting, Th., Trout, B. L., Molina, L. T., and Molina, M. J.: Interaction of hydrogen chloride with ice surfaces: The effects of grain size, surface roughness and surface disorder, J. Phys. Chem. A, 111, 6274–6284, 2007. McNeill, V F.,Yatavelli, R. L. N., Thornton, J. A., Stipe, C. B., and Landgrebe, O.: Heterogeneous OH oxidation of palmitic acid in single component and internally mixed aerosol particles: vaporization and the role of particle phase, Atmos. Chem. Phys., 8, 5465–5476, doi:10.5194/acp-8-5465-2008, 2008. Mentel, T. F., Sohn, M., and Wahner, A.: Nitrate effect in the heterogeneous hydrolysis of dinitrogen pentoxide on aqueous aerosols, Phys. Chem. Chem. Phys., 1, 5451–5457, DOI: 10.1039/a905338g, 1999. Miet, K., Le Menach, K., Flaud, P.-M., Budzinski, H. and Villenave, E.: Heterogeneous reactivity of pyrene and 1–nitropyrene with NO<sub>2</sub>: Kinetics, product yields and mechanism, Atmos. Environ., 43, 837–843, 2009a. Miet, K., Le Menach, K., Flaud, P.-M., Budzinski, H. and Villenave, E.: Heterogeneous reactions of ozone with pyrene, 1-hydroxypyrene and 1–nitropyrene adsorbed on particles, Atmos. Environ., 43, 3699–3707, 2009b. Miller, C. A., Abbott, N. L., and de Pablo, J. J.: Surface Activity of Amphiphilic Helical beta–Peptides from Molecular Dynamics Simulation, Langmuir, 25, 2811–2823, 2009. Miller, R. L., Tegen, I., and Perlwitz, J.: Surface radiative forcing by soil dust aerosols and the hydrologic cycle, J. Geophys. Res. Atmos., 109, D04203, doi:10.1029/2003JD004085, 2004. Minofar, B., Jungwirth, P., Das, M. R., Kunz, W., and Mahiuddin, S.: Propensity of formate, acetate, benzoate, and phenolate for the aqueous solution/vapor interface: Surface tension measurements and molecular dynamics simulations, J. Phys. Chem. C, 111, 8242–8247, 2007. Mmereki, B. T., Hicks, J. M., and Donaldson, D. J.: Adsorption of atmospheric gases at the air-water interface. 3: Methylamines, J. Phys. Chem. A, 104, 10789–10793, 2000. Mmereki, B. T., Chaudhuri, S. R., and Donaldson, D. J.: Enhanced uptake of PAHs by organic–coated aqueous surfaces, J. Phys. Chem. A, 107, 2264–2269, 2003. Mmereki, B. T., Donaldson, D. J., Gilman, J. B., Eliason, T. L., and Vaida, V.: Kinetics and products of the reaction of gas-phase ozone with anthracene adsorbed at the air–aqueous interface, Atmos. Environ., 38, 6091–6103, 2004. Mogili, P. K., Kleiber, P. D., Young, M. A., and Grassian, V. H.: Heterogeneous Uptake of Ozone on Reactive Components of Mineral Dust Aerosol: An Environmental Aerosol reaction Chamber Study. J. Phys. Chem. A, 110, 13799–13807, 2006a.. Mogili, P.K., Kleiber, P. D., Young, M. A., and Grassian, V. H.: N<sub>2</sub>O$_5$ hydrolysis on the components of mineral dust and sea salt aerosol: comparison study in an environmental aerosol reaction chamber, Atmos. Environ., 40, 7401–7408, 2006b. Möhler, 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. Moise, T. and Rudich, Y.: Reactive uptake of ozone by proxies for organic aerosols: Surface versus bulk processes, J. Geophys. Res.-Atmos., 105, 14667–14676, 2000. Moise, T. and Rudich, Y.: Reactive uptake of Cl and Br atoms by organic surfaces – a perspective on the processing of organic aerosols by tropospheric oxidants, Geophys. Res. Lett., 28, 4083–4086, 2001. Moise, T. and Rudich, Y.: Reactive uptake of ozone by aerosol-associated unsaturated fatty acids: Kinetics, mechanism, and products, J. Phys. Chem. A, 106, 6469–6476, 2002. Moise, T., Rudich, Y., Rousse, D., and George, C.: Multiphase decomposition of novel oxygenated organics in aqueous and organic media, Environ. Sci. Technol., 39, 5203–5208, 2005. Molina, M. J., Ivanov, A. V., Trakhtenberg, S., and Molina, L. T.: Atmospheric evolution of organic aerosol, Geophys. Res. Lett., 31, L22104, doi:10.1029/2004GL020910, 2004. Monge, M. E., D'Anna, B., Mazri, L., Giroir–Fendler, A., Ammann, M., Donaldson, D. J., and George, C.: Light changes the atmospheric reactivity of soot, Proc. Nat. Acad. Sci., 107, 6605–609, 2010. Morita, A.: Molecular dynamics study of mass accommodation of methanol at liquid-vapor interfaces of methanol/water binary solutions of various concentrations, Chem. Phys. Lett., 375, 1–8, 2003a. Morita, A. and Garrett, B. C.: Molecular theory of mass transfer kinetics and dynamics at gas-water interface, Fluid Dynam. Res., 40, 459–473, 2008. Morita, A., Sugiyama, M., Kameda, H., Koda, S., and Hanson, D. R.: Mass accommodation coefficient of water: Molecular dynamics simulation and revised analysis of droplet train/flow reactor experiment, J. Phys. Chem. B, 108, 9111–9120, 2004a. Morita, A., Kanaya, Y., and Francisco, J. S.: Uptake of the HO<sub>2</sub> radical by water: Molecular dynamics calculations and their implications for atmospheric modeling, J. Geophys. Res.-Atmos., 109, D09201, doi:10.1029/2003JD004240, 2004b. Morris, J. W., Davidovits, P., Jayne, J. T., Shi, Q., Kolb, C. E., Worsnop, D. R., Barney, W. S., Jimenez, J., and Cass, G.: Kinetics of submicron oleic acid aerosols with ozone: A novel aerosol mass spectrometric technique, Geophys. Res. Lett., 29, 1357, doi:1029/2002GL014692, 2002. Mozurkewich, M.: Effect of competitive adsorption on polar stratospheric cloud reactions, Geophys. Res. Lett., 20, 355–358, 1993. Mozurkewich, M., McMurry, P. H., Gupta, A., et al.: Mass accommodation coefficient for HO<sub>2</sub> radicals on aqueous particles, J. Geophys. Res., 92, 4163–4170, 1987. Muller, B. and Heal, M. R.: The mass accommodation coefficient of ozone on an aqueous surface, Phys. Chem. Chem. Phys., 4, 3365–3369, 2002. Mundy, C. J., Rousseau, R., Curioni, A., Kathmann, S. M., and Schemer, G. K.: A molecular approach to understanding complex systems: computational statistical mechanics using state-of-the-art algorithms on terascale computational platforms, edited by: Stevens, R. L., SciDAC 2008: Scientific Discovery through Advanced Computing, 012014, 12014–12014, 2008. Nagayama, G. and Tsuruta, T.: A general expression for the condensation coefficient based on transition state theory and molecular dynamics simulation, J. Chem. Phys., 118, 1392–1399, 2003. NASA.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies, JPL Publication No. 06–2; Jet Propulsion Laboratory, National Aeronautics and Space Administration, Pasadena, CA, USA, available online at: http://jpldataeval.jpl.nasa.gov/, 2006. Ndour, M., D'Anna, B., George, C., Ka, O., Balkanski, Y., Kleffmann, J., Stemmler, K., and Ammann, M.: Photoenhanced update of NO<sub>2</sub> on mineral dust: laboratory experiments and model simulations, Geophys. Res. Lett. 35, L05812, doi:10.1029/2007GL032006, 2008. Niesar, U., Corongiu, G., Huang, M. J., Dupuis, M., and Clementi, E.: Preliminary-Observations On A New Water Water Potential, International J. Quant. Chem., 36(S23), 421–443, 1989. Niesar, U., Corongiu, G., Clementi, E., Kneller, G. R., and Bhattacharya, D. K.: Molecular-Dynamics Simulations of Liquid Water Using the Ncc Ab Initio Potential, J. Phys. Chem., 94, 7949–7956, 1990. Nieto-Gligorovski, L., Net, S., Gligorovski, S., Zetzsch, C., Jammoul, A., D'Anna, B., and George, C.: Interactions of ozone with organic surface films in the presence of simulated sunlight: impact on wettability of aerosols, Phys. Chem. Chem. Phys., 10, 2964–2971, doi:10.1039/b717993f, 2008. Nozière, B. and Esteve, W.: Organic reactions increasing the absorption of sulphuric acid aerosols, Geophys. Res. Lett., 32, L03812, doi:10.1029/2004GL02194, 2005. Nozière, B. and Esteve, W.: Light-absorbing aldol condensation products in acidic aerosols: Spectra, kinetics, and contribution to the absorption index, Atmos. Environ., 41, 1150–1163, 2007. Nozière, B., Dziedzic, P., and Córdova, A.: Formation of secondary light–absorbing "fulvic–like" oligomers: A common process in aqueous and ionic atmospheric particles? Geophys. Res. Lett., 34, L21812, doi:10.1029/2007GL031300, 2007. Oppliger, R., Allanic, A., and Rossi, M. J.: Real–time kinetics of the uptake of ClONO<sub>2</sub> on ice and in the presence of HCl in the temperature range 160 K = $T$ = 200 K, J. Phys. Chem. A, 101, 1903–1911, 2007. Oum, K. W., Lakin, M. J., DeHaan, D. O., Brauers, T., and Finlayson–Pitts, B. J.: Formation of Molecular Chlorine from the Photolysis of Ozone and Aqueous Sea–Salt Particles, Science, 279, 74–76, 1998a. Oum, K. W., Lakin, M. J., and Finlayson-Pitts, B. J.: Bromine Activation in the Troposphere by the Dark Reaction of O<sub>3</sub> and Seawater Ice, Geophys. Res. Lett., 25, 3923, doi:10.1029/1998GL900078,1998b. Padró, L. T., Asa–Awuku, A., Morrison, R., and Nenes, A.: Inferring thermodynamic properties from CCN activation experiments: single–component and binary aerosols, Atmos. Chem. Phys., 7, 5263–5274, doi:10.5194/acp-7-5263-2007, 2007. Parent, P. and Laffon, C.: Adsorption of HCl on the water ice surface studied by X–ray absorption spectroscopy, J. Phys. Chem. B, 109, 1547–1553, 2005. Park, J., Gomez, A. L., Walser, M. L., Lin, A., and Nizkorodov, S. A.: Ozonolysis and photolysis of alkene–terminated self-assembled monolayers on quartz nanoparticles: implications for photochemical aging of organic aerosol particles, Phys. Chem. Chem. Phys., 8, 2506–2512, 2006. Park, S.–C., Burden, D. K., and Nathanson, G. M.: The Inhibition of N<sub>2</sub>O$_5$ Hydrolysis in Sulfuric Acid by 1-Butanol and 1-Hexanol Surfactant Coatings, J. Phys. Chem. A., 111, 2921–2929, 2007. Partay, L. B., Jedlovszky, P., Hoang, P. N. M., Picaud, S., and Mezei, M.: Free–energy profile of small solute molecules at the free surfaces of water and ice, as determined by cavity insertion Widom calculations, J. Phys. Chem. C, 111, 9407–9416, 2007. Patel, S., Zhong, Y., Bauer, B. A., and Davis, J. E.: Interfacial Structure, Thermodynamics, and Electrostatics of Aqueous Methanol Solutions via Molecular Dynamics Simulations Using Charge Equilibration Models, J. Phys. Chem. B, 113, 9241–9254, 2009. Paul, S. and Chandra, A.: Dynamics of water molecules at liquid–vapour interfaces of aqueous ionic solutions: effects of ion concentration, Chem. Phys. Lett., 373, 87–93, 2003. Paul, S. and Chandra, A.: Binding of hydrogen bonding solutes at liquid-vapour interfaces of molecular fluids, Chem. Phys. Lett., 400, 515–519, 2004. Pegram, L. M. and Record, M. T.: Partitioning of atmospherically relevant ions between bulk water and the water/vapor interface, Proc. Natl. Acad. Sci., 103, 14278–14281, 2006. Perraudin, E., Budzinski, H., and Villenave, E.: Kinetic study of the reactions of ozone with polycyclic aromatic hydrocarbons adsorbed on atmospheric model particles, J. Atmos. Chem., 56, 57–82, 2007. Persiantseva, N. M., Popovicheva, O. B., Shonija, N. K., et al.: Wetting and hydration of insoluble soot particles in the upper troposphere, J. Environ. Monitor., 6, 939–945, 2004. Peter, T., Marcolli, C., Spichtinger, P., Corti, T., Baker, M. B., and Koop, T.: When dry air is too humid, Science, 314, 1399–1402, 2006. Petersen, P. B., Johnson, J. C., Knutsen, K. P., and Saykally, R. J.: Direct experimental validation of the Jones–Ray effect, Chem. Phys. Lett., 397, 46–50, 2004. Petersen, P. B. and Saykally, R. J.: On the Nature of Ions at the Liquid Water Surface, Ann. Rev. Phys. Chem., 57, 333–364, 2006. Petzold, A., Gysel, M., Vancassel, X.,~Hitzenberger, R.,~Puxbaum, H.,~Vrochticky, S.,~Weingartner, E.,~Baltensperger, U.,~and Mirabel, P.: On the effects of organic matter and sulphur-containing compounds on the CCN activation of combustion particles, Atmos. Chem. Phys., 5, 3187–3203, doi:10.5194/acp-5-3187-2005, 2005. Pfrang, C., Shiraiwa, M., and Pöschl, U.: Coupling aerosol surface and bulk chemistry with a kinetic double layer model (K2–SUB): oxidation of oleic acid by ozone, Atmos. Chem. Phys., 10, 4537–4557, doi:10.5194/acp-10-4537-2010, 2010 Pohorille, A. and Benjamin, I.: Molecular-Dynamics of Phenol at the Liquid Vapor Interface of Water, J. Chem. Phys., 94, 5599–5605, 1991. Pohorille, A. and Benjamin, I.: Structure and Energetics of Model Amphiphilic Molecules at the Water Liquid Vapor Interface – a Molecular–Dynamics Study, J. Phys. Chem., 97, 2664–2670, 1993a. Pohorille, A. and Wilson, M. A.: Molecular Structure of Aqueous Interfaces, Journal of Molecular Structure: Theochem, 284, 271–298, 1993b. Pöschl, U.: Formation and decomposition of hazardous chemical components contained in atmospheric aerosol particles, Journal of Aerosol Medicine–Deposition Clearance and Effects In The Lung, 15, 203–212, 2002. Pöschl, U., Letzel, T., Schauer, C., and Niessner, R.: Interaction of ozone and water vapor with spark discharge soot aerosol particles coated with benzo[a]pyrene: O<sub>3</sub> and H<sub>2</sub>O adsorption, benzo[a]pyrene degradation, and atmospheric implications, J. Phys. Chem. A, 105, 4029–4041, 2001. Pöschl, U., Rudich, Y., and Ammann, M.: Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 1: General equations, parameters, and terminology, Atmos. Chem. Phys., 7, 5989–6023, doi:10.5194/acp-7-5989-2007, 2007. Pradhan, M.,~Kyriakou, G.,~Archibald, A T.,~Papageorgiou, A C.,~Kalberer, M.,~and Lambert, R M.: Heterogeneous uptake of gaseous hydrogen peroxide by Gobi and Saharan dust aerosols: a potential missing sink for H<sub>2</sub>O<sub>2</sub> in the troposphere, Atmos. Chem. Phys.,~10,~7127–7136,~doi:10.5194/acp-10-7127-2010, 2010. Pratt, L. R. and Pohorill e, A.: Hydrophobic effects and modeling of biophysical aqueous solution interfaces, Chem. Rev., 102, 2671–2691, 2002. Pratte, P., van den Bergh, H., and Rossi, M. J.: The kinetics of H<sub>2</sub>O vapor condensation and evaporation on different types of ice in the range 130–210K, J. Phys. Chem. A, 110, 3042–3058, 2006. Preszler Prince, A., Grassian, V. H., Kleiber, P., and Young, M. A.: Heterogeneous conversion of calcite aerosol by nitric acid, Phys. Chem. Chem. Phys., 9, 622–634, 2007. Quinlan, M. A., Reihs, C. M., Golden, D. M., and Tolbert, M. A.: Heterogeneous Reactions on model polar stratospheric cloud surfaces, J. Phys. Chem., 94, 3255–3260, 1990. Rahman, A., Stillinger, F. H., and Lemberg, H. L.: Study of a Central Force Model for Liquid Water by Molecular–Dynamics, J. Chem. Phys., 63, 5223–5230, 1975. Remorov, R. G. and Bradwell, M. W.: Langmuir Approach in the Study of Interfacial Mass Transfer, Surf. Sci., 585, 59–65, 2005. Remorov, R. G. and George, C.: Analysis of chemical kinetics at the gas-aqueous interface for submicron aerosols, Phys. Chem. Chem. Phys., 8, 4897–4901, 2006. Riipinen, I., Koponen, I. K., Frank, G. P., Hyvärinen, A.-P., Vanhanen, J., Lihavainen, H., Lehtinen, K. E. J., Bilde, M. and Kulmala, M.: Adipic and malonic acid aqueous solutions: surface tensions and saturation vapor pressures, J. Phys. Chem. A., 111, 12995–13002, 2007. Robbins, R. C. and Cadle, R. D.: Kinetics of the Reaction Between Gaseous Ammonia and Sufuric Acid Droplets in an Aerosol, J. Phys. Chem., 62, 469–471, 1958. Roberts, J. M., Osthoff, H. D., Brown, S. S., and Ravishankara, A. R.: N<sub>2</sub>O$_5$ Oxidizes Chloride to Cl<sub>2</sub> in Acidic Atmospheric Aerosol, Science, 321, 1059–1059, 2008. Robinson, G. N., Worsnop, D. R., Jayne, J. T., Kolb, C. E., and Davidovits, P.: Heterogeneous uptake of ClONO<sub>2</sub> and N<sub>2</sub>O$_5$ by sulfuric acid solutions, J. Geophys. Res., 102, 3583–3602, 1997. Roeselova, M., Jungwirth, P., Tobias, D. J., and Gerber, R. B.: Impact, trapping, and accommodation of hydroxyl radical and ozone at aqueous salt aerosol surfaces. A molecular dynamics study, J. Phys. Chem. B, 107, 12690–12699, 2003. Roeselova, M., Vieceli, J., Dang, L. X., Garrett, B. C., and Tobias, D. J.: Hydroxyl radical at the air-water interface, J. Am. Chem. Soc., 126, 16308–16309, 2004. Roth, C. M., Goss, K.-U., and Schwarzenbach, R. P.: Adsorption of a diverse set of organic vapors on the bulk water surface, J. Coll. Int. Sci., 252, 21–30, 2002. Rudich, Y.: Laboratory perspectives on the chemical transformations of organic matter in atmospheric particles, Chem. Rev., 103, 5097–5124, 2003. Rudich, Y., Donahue, N. M., and Menache, M. G.: Aging of Organic Aerosol: Bridging the Gap Between Laboratory and Field Studies, Ann. Rev. Phys. Chem., 58: 321–352, 2007. Rudich, Y., Talukdar, R., and Ravishankara, A. R.: Reactive uptake of NO<sub>3</sub> on pure water and ionic solutions, J. Geophys. Res., 101, 21023–21032, 1996. Rudolf, R., Vrtala, A., Kulmala, M., Vesala, T., and Wagner, P. E.: Experimental study of sticking probabilities for condensation of nitric acid-water vapor mixtures, J. Aerosol Sci., 32, 913–932, 2001. Reutter, P. H. Su, Trentmann, J., Simmel, M., Rose, D., Gunthe, S. S., H. Wernli, H., Andreae, M. O., and Pöschl, U.: Aerosol- and updraft-limited regimes of cloud droplet formation: in?uence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN), Atmos. Chem. Phys., 9, 7067–7080, doi:10.5194/acp-9-7067-2009, 2009. Russell, L. M. Hawkins, L. N. Frossard, A. A., Quinn, P. K., and Bates, T. S.: Carbohydrate-like composition of submicron atmospheric particles and their production from ocean bubble bursting, Proc. Natl. Acad. Sci., 107, 6652–6657, 2010. Saathoff, H., Naumann, K.-H., Riemer, N., et al.: The loss of NO<sub>2</sub>, HNO<sub>3</sub>, NO<sub>3</sub>/N<sub>2</sub>O$_5$, and HO<sub>2</sub>/HOONO<sub>2</sub> on soot aerosol: A chamber and modeling study, Geophys. Res. Lett., 28, 1957–1960, 2001. Sage, A. M., Weitkamp, E. A., Robinson, A. L., and Donahue, N. M.: Reactivity of oleic acid in organic particles: changes in oxidant uptake and reaction stoichiometry with particle oxidation, Phys. Chem. Chem. Phys., 11, 7951–7962, 2009. Salgado, M. S. and Rossi, M. J.: Flame soot generated under controlled combustion conditions: Heterogeneous reaction of NO<sub>2</sub> on hexane soot, Int. J. Chem. Kin., 34, 620–631, 2002. Sander, R.: Compilation of Henry's Law Constants for Inorganic and Organic Species of Potential Importance in Environmental Chemistry: http://www.mpch-mainz.mpg.de/~sander/res/henry.html, 1999. Santschi, C. and Rossi, M. J.: The uptake of CO<sub>2</sub>, SO<sub>2</sub>, HNO<sub>3</sub> and HCl on CaCO<sub>3</sub> at 300K: mechanism and the role of adsorbed water, J. Phys. Chem. A 110, 6789–6802, 2006. Saul, T. D., Tolocka, M. P., and Johnston, M. V.: Reactive uptake of nitric acid onto sodium chloride aerosols across a wide range of humidities, J. Phys. Chem. A, 110, 7614–7620, 2006. Schenter, G. K., Garrett, B. C., and Truhlar, D. G.: Generalized transition state theory in terms of the potential of mean force, J. Chem. Phys., 119, 5828–5833, 2003. Schutze, M. and Herrmann, H.: Determination of phase transfer parameters for the uptake of HNO<sub>3</sub>, N<sub>2</sub>O$_5$ and O<sub>3</sub> on single aqueous drops, Phys. Chem. Chem. Phys., 4, 60–67, 2002. Schweitzer, F., Mirabel, P., and George, C.: Multiphase Chemistry of N<sub>2</sub>O$_5$, ClNO<sub>2</sub> and BrNO<sub>2</sub>, J. Phys. Chem. A, 102, 3942–3952, 1998. Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: from air pollution to climate change, Wiley, New York, USA, 610–611, 1998. Seisel, S., Börensen, C., Vogt, R., and Zellner, R.: The heterogeneous reaction of HNO<sub>3</sub> on mineral dust and $\gamma $ alumina surfaces : a combined Knudsen cell and DRIFTS study, Phys. Chem. Chem. Phys., 6, 5498–5508, 2004. Shantz, N. C., Chang, R. Y.-W., Slowik, J. G., Vlasenko, A., Abbatt, J. P. D., and Leaitch, W. R.: Slower CCN growth kinetics of anthropogenic aerosol compared to biogenic aerosol observed at a rural site, Atmos. Chem. Phys., 10, 299–312, 2010. Shaw, R. A. and Lamb, D.: Experimental determination of the thermal accommodation and condensation co–efficients of water, J. Chem. Phys., 111, 10659–10663, 1999. Shi, Q., Li, Y. Q., Davidovits, P., Jayne, J. T., Worsnop, D. R., Mozurkewich, M., and Kolb, C. E.: Isotope exchange for gas-phase acetic acid and ethanol at aqueous interfaces: A study of surface reactions, J. Phys. Chem. B, 103, 2417–2430, 1999. Shilling, J. E., Tolbert, M. A., Toon, O. B., Jensen, E. J., Murray, B. J., and Bertram, A. K.: Measurements of the vapor pressure of cubic ice and their implications for atmospheric ice clouds, Geophys. Res. Lett., 33, L17801, doi:10.1029/2006GL026671, 2006. Shin, J. Y. and Abbott, N. L.: Combining molecular dynamics simulations and transition state theory to evaluate the sorption rate constants for decanol at the surface of water, Langmuir, 17, 8434–8443, 2001. Shiraiwa, M., Garland, R. M. and Pöschl, U.: Kinetic double–layer model of aerosol surface chemistry and gas–particle interactions (K2–SURF): Degradation of polycyclic aromatic hydrocarbons exposed to O<sub>3</sub>, NO<sub>2</sub>, H<sub>2</sub>O, OH and NO<sub>3</sub>, Atmos. Chem. Phys., 9, 9571–9586, doi:10.5194/acp-9-9571-2009, 2009. Shiraiwa, M., Pfrang, C., and Pöschl, U.: Kinetic multi–layer model of aerosol surface and bulk chemistry (KM–SUB): the influence of interfacial transport and bulk diffusion on the oxidation of oleic acid by ozone, Atmos. Chem. Phys., 10, 3673–3691, 2010. Shonija, N. K., Popovicheva, O. B., Persiantseva, N. M., et al.: Hydration of aircraft engine soot particles under plume conditions: Effect of sulfuric and nitric acid processing, J. Geophys. Res.–Atmos., 112, D02208, doi:10.1029/2006JD007217, 2007. Simpson, A. J., Lam, B., Diamond, M. L., Donaldson, D. J., Lefebvre, B. A., Moser, A. Q., Williams, A. J., Larin, N. I., and Kvasha, M. P.: Assessing the organic composition of urban surface films using nuclear magnetic resonance spectroscopy, Chemosphere, 63, 142–152, 2006. Sjostedt, S., and Abbatt, J. P. D.: Release of gas–phase halogens from sodium halide substrates: heterogeneous oxidation of frozen solutions and desiccated salts by hydroxyl radicals, Environ. Res. Lett., 3, 045007, doi:10.1088/1748-9326/3/4/045007, 2008. Smith, J. D., Cappa, C. D., Drisdell, W. S., Cohen, R. C., and Saykally, R. J.: Raman Thermometry Measurements of Free Evaporation from Liquid Water Droplets, J. Amer. Chem. Soc., 128, 12892–12898, 2006. Sokhan, V. P. and Tildesley, D. J.: Molecular dynamics simulation of the non–linear optical susceptibility at the phenol/water/air interface, Faraday Discussions, 104, 193–208, 1996. Sprik, M. and Klein, M. L.: A Polarizable Model For Water Using Distributed Charge Sites, J. Chem. Phys., 89, 7556–7560, 1988. Stadler, D., and Rossi, M. J.: The reactivity of NO<sub>2</sub> and HONO on flame soot at ambient temperature: The influence of combustion conditions, Phys. Chem. Chem. Phys., 2, 5420–5429, 2000. Stemmler, K., Ammann, M., Donders, C., Kleffmann, J., and George, C.: Photosensitized reduction of nitrogen dioxide on humic acid as a source of nitrous acid, Nature, 440, 195–198, 2006. Stemmler, K., Ndour, M., Elshorbany, Y., Kleffmann, J., D'Anna, B., George, C., Bohn, B., and Ammann, M.: Light induced conversion of nitrogen dioxide into nitrous acid on submicron humic acid aerosol, Atmos. Chem. Phys., 7, 4237–4248, doi:10.5194/acp-7-4237-2007, 2007. Stemmler, K.,~Vlasenko, A.,~Guimbaud, C and Ammann, M.: The effect of fatty acid surfactants on the uptake of nitric acid to deliquesced NaCl aerosol, Atmos. Chem. Phys., 8, 5127–5141, 2008. Stewart, D. J., Griffiths, P. T., and Cox, R. A.: Reactive uptake coefficients for heterogeneous reaction of N<sub>2</sub>O$_5$ with submicron aerosols of NaCl and natural sea salt, Atmos. Chem. Phys., 4, 1381–1388, 2004. Stewart, E., Shields, R. L., and Taylor, R. S.: Molecular dynamics simulations of the liquid/vapor interface of aqueous ethanol solutions as a function of concentration, J. Phys. Chem. B, 107, 2333–2343, 2003. Stillinger, F. H. and Rahman, A.: ST2 potential, J. Chem. Phys., 60, 1545–1557, 1974. Stillinger, F. H. and Rahman, A.: Revised central force potentials for water, J. Chem. Phys., 68, 666–670, 1978. Stipp, S. L. S., Eggleston, C. M., and Nielsen, B. S.: Calcite surface structure observed at microphotographic and molecular scales with atomic force microscopy (AFM), Geochim. Cosmochim. Acta, 58, 3023–3033, 1994. Styler, S.A., Brigante, M., D'Anna, B., George, C. H., and Donaldson, D. J.: Photoenhanced ozone loss on solid pyrene films, Phys. Chem. Chem. Phys., 11, 7876–7884, 2009. Sullivan, R. C., Moore, M. J. K., Petters, M. D., Kreidenweis, S. M., Roberts, G. C., and Prather, K. A.: Timescale for hygroscopic conversion of calcite mineral particles through heterogeneous reaction with nitric acid, Phys. Chem. Chem. Phys., 11, 7826–7837, 2009. Sumner, A. L., Menke, E. J., Dubowski, Y., Newberg, J. T., Penner, R. M., Hemminger, J. C., Wingen, L. M., Brauers, T., and Finlayson-Pitts, B. J.: The nature of water on surfaces of laboratory systems and implications for heterogeneous chemistry in the troposphere, Phys. Chem. Chem. Phys., 6, 604–613, 2004. Sun, X. Q., Chang, T. M., Cao, Y., Niwayama, S., Hase, W. L., and Dang, L. X.: Solvation of Dimethyl Succinate in a Sodium Hydroxide Aqueous Solution. A Computational Study, J. Phys. Chem. B, 113, 6473–6477, 2009. Symington, A.: The Heterogeneous Interaction of Organic Acids with Ice Surfaces at Temperatures of the Upper Troposphere, CPGS Dissertation, Newham College, University of Cambridge, 2006. Tabazadeh, A. and Turco, R.: A model for heterogeneous chemical processes on the surfaces of ice and nitric acid trihydrate particles, J. Geophys. Res., 98, 12727–12740, 1993. Takami, A., Kato, S., Shimono, A., and Koda, S.: Uptake coefficient of OH radical on aqueous surface, Chem. Phys. 231, 215–227, 1998. Taketani, F., Kanaya, Y., and Akimoto, H.: Kinetics of heterogeneous reactions of HO<sub>2</sub> radical at ambient concentration levels with (NH$_4)_2$SO<sub>4</sub> and NaCl aerosol particles, J. Phys. Chem. A, 112, 2370–2377, 2008. Taketani, F., Kanaya, Y., Akimoto, H..: Heterogeneous loss of HO<sub>2</sub> by KCl, synthetic sea salt, and natural seawater aerosol particles, Atmos. Environ., 43, 1660–1665, 2009. Tarek, M., Tobias, D. J., and Klein, M. L.: Molecular dynamics investigation of an ethanol–water solution, Physica A, 231, 117–122, 1996a. Tarek, M., Tobias, D. J., and Klein, M. L.: Molecular dynamics investigation of the surface/bulk equilibrium in an ethanol–water solution, Journal of the Chemical Society-Faraday Transactions 92, 559–563, 1996b. Taylor, R. S., Dang, L. X., and Garrett, B. C.: Molecular dynamics simulations of the liquid/vapor interface of SPC/E water, J. Phys. Chem., 100, 11720–11725, 1996. Taylor, R. S., Ray, D., and Garrett, B. C.: Understanding the mechanism for the mass accommodation of ethanol by a water droplet, J. Phys. Chem. B, 101, 5473–5476, 1997. Taylor, R. S. and Garrett, B. C.: Accommodation of alcohols by the liquid/vapor interface of water: Molecular dynamics study, J. Phys. Chem. B, 103, 844–851, 1999. Taylor, R. S. and Shields, R. L.: Molecular-dynamics simulations of the ethanol liquid–vapor interface, J. Chem. Phys., 119, 12569–12576, 2003. Tervahattu, H, Hartonen, K, Kerminen, VM, Kupiainen, K, Aarnio, P; Koskentalo, T, Tuck, AF and Vaida, V,: New evidence of an organic layer on marine aerosols:, J. Geophys. Res. 107(D7), 4053, doi:10.1029/2000JD000282, 2002. Thibert, E. and Dominé, F.: Thermodynamics and Kinetics of the Solid Solution of HNO<sub>3</sub> in Ice. J. Phys. Chem. B, 102, 4432–4439, 1998. Thomas, E. R., Frost, G. J., and Rudich, Y.: Reactive uptake of ozone by proxies for organic aerosols: Surface–bound and gas–phase products, J. Geophys. Res.-Atmos., 106, 3045–3056, 2001. Thornberry, T. and Abbatt, J. P. D.: Heterogeneous reaction of ozone with liquid unsaturated fatty acids: detailed kinetics and gas–phase product studies, Phys. Chem. Chem. Phys., 6, 84–93, 2004. Thornberry, T. D. and Abbatt, J. P. D.: Detailed analysis of the kinetics and products of the reaction of ozone with condensed phase oleic acid, Abstracts of Papers Am. Chem. Soc., 224, U328–U328, 2002. Thornton, J. A. and Abbatt, J. P. D.: N<sub>2</sub>O$_5$ reaction on sub–micron sea–salt aerosols: Kinetics, products and the effect of surface active organics, J. Phys. Chem. A., 109, 10004–10012, 2005a. Thornton, J. A. and Abbatt, J. P. D.: Measurements of HO<sub>2</sub> uptake to aqueous aerosol: Mass accommodation coefficients and net reactive loss, J. Geophys. Res., 110, D08309, doi:10.1029/2004JD005402, 2005b. Thornton, J. A., Braban, C. F., and Abbatt, J. P. D.: N<sub>2</sub>O$_5$ hydrolysis on sub-micron organic aerosols: the effect of relative humidity, particle phase, and particle size, Phys. Chem. Chem. Phys., 5, 4593–4603, 2003. Townsend, R. M., Gryko, J., and Rice, S. A.: Structure of the Liquid Vapor Interface of Water, J. Chem. Phys., 82, 4391–4392, 1985. Tsuruta, T. and Nagayama, G.: Molecular dynamics studies on the condensation coefficient of water, J. Phys. Chem. B., 108, 1736–1743, 2004. Ullerstam, M., Vogt, R., Langer, S., and Ljungström, E.: The kinetics and mechanism of SO<sub>2</sub> oxidation by O<sub>3</sub> on mineral dust, Phys. Chem. Chem. Phys., 4, 4694–4699, 2002. Ullerstam, M., Thornberry, T., and Abbatt, J. P. D.: Uptake of gas–phase nitric acid to ice at low partial pressures: Evidence for unsaturated surface coverage, Faraday Discuss., 130, 211–226, 2005. Ullerstam, M., Johnson, M. S., Vogt, R., and Ljungström, E.: DRIFTS and Knudsen cell study of the heterogeneous reactivity of SO<sub>2</sub> and NO<sub>2</sub> on mineral dust, Atmos. Chem. Phys., 3, 2043–2051, doi:10.5194/acp-3-2043-2003, 2003. Underwood, G. M., Li, P., Al-Abadleh, H., and Grassian, V. H.: A Knudsen cell study of the heterogeneous reactivity of nitric acid on oxide and mineral dust particles, J. Phys. Chem. A, 105, 6609–6620, 2001. Usher, C. R., Michel, A. E., and Grassian, V. H.: Reactions on mineral dust, Chem. Rev. , 103, 4883–4939, 2003. Utter, R. G., Burkholder, J. B., Howard, C. J., and Ravishankara, A. R.: Measurement of the Mass Accommodation Coefficient of Ozone on Aqueous Surfaces, J. Phys. Chem., 96, 4973–4979, 1992. Vacha, R., Slavicek, P., Mucha, M., Finlayson–Pitts, B. J., and Jungwirth, P.: Adsorption of atmospherically relevant gases at the air/water interface: Free energy profiles of aqueous solvation of N<sub>2</sub>, O<sub>2</sub>, O<sub>3</sub>, OH, H<sub>2</sub>O, HO<sub>2</sub>, and H<sub>2</sub>O<sub>2</sub>, J. Phys. Chem. A, 108, 11573–11579, 2004. Vazquez, G., Alvarez, E., Cancela, A., and Navaza, J. M.: Density, Viscosity, and Surface–Tension of Aqueous–Solutions of Sodium–Sulfite and Sodium-Sulfite Plus Sucrose from 25–Degrees–C to 40–Degrees–C, J. Chem. Eng. Data, 40, 1101–1105, 1995. Vesala, T., Kulmala, M., Rudolf, R., Vrtala, A., and Wagner, P. E.: Models for condensational growth and evaporation of binary aerosol particles, J. Aerosol Sci., 28, 565–598, 1997. Vieceli, J., Roeselova, M., and Tobias, D. J.: Accommodation coefficients for water vapor at the air/water interface, Chem. Phys. Lett., 393, 249–255, 2004. Vieceli, J., Roeselova, M., Potter, N., Dang, L. X., Garrett, B. C., and Tobias, D. J.: Molecular dynamics simulations of atmospheric oxidants at the air-water interface: Solvation and accommodation of OH and O<sub>3</sub>, J. Phys. Chem. B., 109, 15876–15892, 2005. Vlasenko, A., George, I. J., and Abbatt, J. P. D.: Formation of Volatile Organic Compounds in the Heterogeneous Oxidation of Condensed–Phase Organic Films by Gas–Phase OH, J. Phys. Chem. A, 112, 1552–1560, 2008. Vlasenko, A., Huthwelker, T., Gaggeler, H. W., and Ammann, M.: Kinetics of the heterogeneous reaction of nitric acid with mineral dust particles: an aerosol flowtube study, Phys. Chem. Chem. Phys., 11, 7921–7930, 2009. Vlasenko, A., Sjogren, S., Weingartner, E., Stemmler, K., Gäggeler, H. W., and Ammann, M.: Effect of humidity on nitric acid uptake to mineral dust aerosol particles, Atmos. Chem. Phys., 6, 2147–2160, doi:10.5194/acp-6-2147-2006, 2006. Voigtländer, J., Stratmann, F., Niedermeier, D., Wex, H., and Kiselev, A.: Mass Accommodation coefficient of water: A combined computational fluid dynamics and experimental analysis, J. Geophys. Res., 112, D2028, doi:10.1029/2007JD008604, 2007. Wachsmuth, M., Gäggeler, H. W., von Glasow, R., and Ammann, M.: Accommodation coefficient of HOBr on deliquescent NaBr aerosol particles, Atmos. Chem. Phys., 2, 121–131, doi:10.5194/acp-2-121-2002, 2002. Wadia, Y., Tobias, D. J., Stafford, R., and Finlayson-Pitts, B. J.: Real–time monitoring of the kinetics and gas–phase products of the reaction of ozone with an unsaturated phospholipid at the air-water interface, Langmuir, 16, 9321–9330, 2000. Wagner, C., Hanisch, F., Holmes, N., de Coninck, H., Schuster, G. and Crowley, J. N.: The interaction of N<sub>2</sub>O$_5$ with mineral dust: aerosol flow tube and Knudsen reactor studies, Atmos. Chem. Phys., 8, 91–109, doi:10.5194/acp-8-91-2008, 2008. Wagner, C., Schuster, G., and Crowley, J. N.: An aerosol flow tube study of the interaction of N<sub>2</sub>O$_5$ with calcite, Arizona dust and quartz, Atmos. Environ., 43, 5001–5008, 2009. Wagner, P. E.: A constant-angle Mie scattering method (CAMS) for investigation of particle formation processes, J. Coll. Interf. Sci., 105, 456–467, 1985. Wahner, A., Mentel, T. F., Sohn, M., and Stier, J.: Heterogeneous reaction of N<sub>2</sub>O$_5$ on sodium nitrate aerosol, J. Geophys. Res., 193, 31103–31112, doi:10.1029/1998JD100022, 1998. Walser, M. L., Park, J., Gomez, A. L., Russell, A. R., and Nizkorodov, S.: Photochemical aging of secondary organic aerosol particles generated from the oxidation of d–limonene, Phys. Chem. A, 111, 1907–1913, 2007. Walser, M. L., Desyaterik, Y., Laskin, J., Laskin, A., and Nizkorodov, S.: High–resolution mass spectrometric analysis of secondary organic aerosol produced by ozonation of limonene, Phys. Chem. Chem. Phys., 10, 1009–1022, 2008. Wei, X., Miranda, P. B., and Shen, Y. R.: Surface vibrational spectroscopic study of surface melting ice, Phys. Rev. Lett. , 86, 1554–1557, 2001. Wilson, M., Pohorille, A., and Pratt, L. R.: Molecular–Dynamics of the Water Liquid Vapor Interface, J. Phys. Chem. , 91, 4873–4878, 1987a. Wilson, M. A., Pohorille, A., and Pratt, L. R.: Molecular–Dynamics of the Water Liquid-Vapor Interface, Journal of the Electrochemical Society, 134, C505–C505, 1987b. Wilson, M. A. and Pohorille, A.: Adsorption and solvation of ethanol at the water liquid-vapor interface: A molecular dynamics study, J. Phys. Chem. B, 101, 3130–3135, 1997. Winkler, A. K., Holmes, N. S., Crowley, J. N., et al.: Interaction of methanol, acetone, and formaldehyde with ice surfaces between 198 and 223 K, Phys. Chem. Chem. Phys., 4, 5270–5275, 2002. Winkler, P. M., Vrtala, A., Wagner, P. E., Kulmala, M., Lehtinen, K. E. J., and Vesala, T.: Mass and thermal accommodation during gas–liquid condensation of water, Phys. Rev. Lett., 93, 075701, doi:10.1103/PhysRevLett.93.075701, 2004. Winkler, P.M., Vrtala, A., Rudolf, R., Wagner, P. E., Riipinen, I., Vesala, T., Lehitnen, K. E. J., Viisanen, Y., and Kulmala, M.: Condensation of water vapor: Experimental determination of mass and thermal accommodation coefficients, J. Geophys. Res., 111, D19202, doi:10.1029/2006JD007194, 2006. Wooldridge, P., Zhang, R., and Molina, M. J.: Phase equilibria of H<sub>2</sub>SO<sub>4</sub>, HNO<sub>3</sub> and HCl hydrates and the composition of polar stratospheric clouds, J. Geophys. Res., 100, 1389–1396, 1995. Worsnop, D. R., Zahniser, M. S., Kolb, C. E., Gardner, J. A., Watson, L. R., Van Doren, J. M., Jayne, J. T., and Davidovits, P.: Temperature dependence of mass accommodation of sulfur dioxide and hydrogen peroxide on aqueous surfaces, J. Phys. Chem., 93, 1159–1172, 1989. Worsnop, D. R., Fox, L. E., Zahniser, M. S., and Wofsy, S. C.: Vapor pressures of solid hydrates of nitric acid: implications for polar stratospheric clouds, Science, 259, 71–74, 1993. Worsnop, D. R., Shi Q., Jayne, J. T., Kolb, C. E., Swartz, E., and Davidovits, P.: Gas Phase Diffusion in Droplet Train Measurements of Uptake Coefficients, J. Aerosol Sci., 32, 877–881, 2001. Worsnop, D. R., Williams, L. R., Kolb, C. E., Mozurkewich, M., Gershenzon, M., and Davidovits, P.: Comment on "The NH<sub>3</sub> mass accommodation coefficient for uptake onto sulfuric acid solution", J. Phys. Chem. A., 108, 8546–8548, 2004a. Worsnop, D. R., Williams, L. R., Kolb, C. E., Mozurkewich, M., Gershenzon, M., and Davidovits, P.: Comment on "Gas–phase flow and diffusion analysis of the droplet–train/flow–reactor technique for the mass accommodation process, J. Phys. Chem. A, 108: 8542–8543, 2004b. Wren, S. N. and Donaldson, D. J.: Glancing-Angle Raman Spectroscopic Probe for Reaction Kinetics at Water Surfaces, Phys. Chem. Chem. Phys., 12, 2648–2654, 2010. Zafiriou, O. C., Joussotdubien, J., Zepp, R. G., and Zika, R. G.: Photochemistry of Natural–Waters, Environ. Sci. Technol., 18, A358–A371, 1984. Zhu, S. B., Fillingim, T. G., and Robinson, G. W.: Flexible Simple Point–Charge Water In A Self–Supporting Thin–Film, J. Phys. Chem., 95, 1002–1006, 1991. Ziemann, P. J.: Aerosol products, mechanisms, and kinetics of heterogeneous reactions of ozone with oleic acid in pure and mixed particles, Faraday Discussions, 130, 469–490, 2005. Zientara, M., Jakubczyk, D., Kolwas, K., and Kolwas, M.: Temperature Dependence of the Evaporation Coefficient of Water in Air and Nitrogen under Atmospheric Pressure: Study in Water Droplets, J. Phys. Chem. A, 112, 5152–5158, 2008. Zondlo, M. A., Hudson, P. K., Prenni, A. J., and Tolbert, M. A.: Chemistry and microphysics of polar stratospheric clouds and Cirrus clouds, Ann. Rev. Phys. Chem., 51, 473–499, 2000.