References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-11-4505-2011

Detailed heterogeneous oxidation of soot surfaces in a particle-resolved aerosol model

Kaiser

J. C.

¹ ⁴ Riemer

² Knopf

D. A.

Department of Physics and Astronomy, Stony Brook University, Stony Brook, NY, USA

Department of Atmospheric Sciences, University of Illinois at Urbana-Champaign, Urbana, IL, USA

Institute for Terrestrial and Planetary Atmospheres, School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY, USA

currently at: Department of Physics and Astronomy, Universität Würzburg, Würzburg, Germany

12 05 2011

11 9 4505 4520

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/11/4505/2011/acp-11-4505-2011.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/4505/2011/acp-11-4505-2011.pdf

Using the particle-resolved aerosol model PartMC-MOSAIC, we simulate the heterogeneous oxidation of a monolayer of polycyclic aromatic hydrocarbons (PAHs) on soot particles in an urban atmosphere. We focus on the interaction of the major atmospheric oxidants (O3, NO2, OH, and NO3) with PAHs and include competitive co-adsorption of water vapour for a range of atmospheric conditions. For the first time detailed heterogeneous chemistry based on the Pöschl-Rudich-Ammann (PRA) framework is modelled on soot particles with a realistic size distribution and a continuous range of chemical ages. We find PAHs half-lives, τ1/2, on the order of seconds during the night, when the PAHs are rapidly oxidised by the gas-surface reaction with NO3. During the day, τ1/2 is on the order of minutes and determined mostly by the surface layer reaction of PAHs with adsorbed O3. Such short half-lives of surface-bound PAHs may lead to efficient conversion of hydrophobic soot into more hygroscopic particles, thus increasing the particles' aerosol-cloud interaction potential. Despite its high reactivity OH appears to have a negligible effect on PAH degradation which can be explained by its very low concentration in the atmosphere. An increase of relative humidity (RH) from 30 % to 80 % increases PAH half-lives by up to 50 % for daytime degradation and by up to 100 % or more for nighttime degradation. Uptake coefficients, averaged over the particle population, are found to be relatively constant over time for O3 (&sim;2 × 10−7 to &sim;2 × 10−6) and NO2 (&sim;5 × 10−6 to &sim;10−5) at the different levels of NOx emissions and RH considered in this study. In contrast, those for OH and NO3 depend strongly on the surface concentration of PAHs. We do not find a significant influence of heterogeneous reactions on soot particles on the gas phase composition. The derived half-lives of surface-bound PAHs and the time and particle population averaged uptake coefficients for O3 and NO2 presented in this paper can be used as parameterisations for the treatment of heterogeneous chemistry in large-scale atmospheric chemistry models.

References 1

Aklilu, Y A. and Michelangeli, D V.: Box model investigation of the effect of soot particles on ozone downwind from an urban area through heterogeneous reactions, Environ. Sci. Technol., 38, 5540–5547, http://dx.doi.org/10.1021/es035079xdoi:10.1021/es035079x, 2004.

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, http://dx.doi.org/10.5194/acp-7-6025-2007doi:10.5194/acp-7-6025-2007, 2007.

Ammann, M., Kalberer, M., Jost, D T., Tobler, L., Rossler, E., Piguet, D., Gaggeler, H W., and Baltensperger, U.: Heterogeneous production of nitrous acid on soot in polluted air masses, Nature, 395, 157–160, 1998.

Arens, F., Gutzwiller, L., Baltensperger, U., Gaggeler, H W., and Ammann, M.: Heterogeneous reaction of NO2 on diesel soot particles, Environ. Sci. Technol., 35, 2191–2199, 2001.

Arens, F., Gutzwiller, L., Gaggeler, H., and Ammann, M.: The reaction of NO2 with solid anthrarobin (1,2,10-trihydroxy-anthracene), Phys. Chem. Chem. Phys., 4, 3684–3690, http://dx.doi.org/10.1039/b201713jdoi:10.1039/b201713j, 2002.

Aubin, D G. and Abbatt, J. P D.: Interaction of NO2 with hydrocarbon soot: Focus on HONO yield, surface modification, and mechanism, J. Phys. Chem. A, 111, 6263–6273, http://dx.doi.org/10.1021/jp068884hdoi:10.1021/jp068884h, 2007.

Bedjanian, Y., Lelièvre, S., and Le~Bras, G.: Experimental study of the interaction of HO2 radicals with soot surface, Phys. Chem. Chem. Phys., 7, 334–341, http://dx.doi.org/10.1039/b414217adoi:10.1039/b414217a, 2005.

Bernstein, J A., Alexis, N., Barnes, C., Bernstein, I L., Bernstein, J A., Nel, A., Peden, D., Diaz-Sanchez, D., Tarlo, S M., and Williams, P B.: Health effects of air pollution, J. Allergy Clin. Immunol., 114, 1116–1123, http://dx.doi.org/10.1016/j.jaci.2004.08.030doi:10.1016/j.jaci.2004.08.030, 2004.

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, http://dx.doi.org/10.1021/jp0114034doi:10.1021/jp0114034, 2001.

Bey, I., Jacob, D J., Yantosca, R M., Logan, J A., Field, B D., Fiore, A M., Li, Q B., Liu, H. G Y., Mickley, L J., and Schultz, M G.: Global modeling of tropospheric chemistry with assimilated meteorology: Model description and evaluation, J. Geophys. Res.-Atmos., 106, 23073–23095, 2001.

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, http://dx.doi.org/10.1029/2004JD005298doi:10.1029/2004JD005298, 2004.

Cain, J P., Gassman, P L., Wang, H., and Laskin, A.: Micro-FTIR study of soot chemical composition-evidence of aliphatic hydrocarbons on nascent soot surfaces, Phys. Chem. Chem. Phys., 12, 5206–5218, http://dx.doi.org/10.1039/b924344edoi:10.1039/b924344e, 2010.

Chughtai, A., Miller, N., Smith, D., and Pitts, J.: Carbonaceous particle hydration III, J. Atmos. Chem., 34, 259–279, 1999.

Durant, J L., Busby, W F., Lafleur, A L., Penman, B W., and Crespi, C L.: Human cell mutagenicity of oxygenated, nitrated and unsubstituted polycyclic aromatic hydrocarbons associated with urban aerosols, Mutat. Res.-Genet. Toxicol., 371, 123–157, 1996.

Dusanter, S., Vimal, D., Stevens, P S., Volkamer, R., Molina, L T., Baker, A., Meinardi, S., Blake, D., Sheehy, P., Merten, A., Zhang, R., Zheng, J., Fortner, E C., Junkermann, W., Dubey, M., Rahn, T., Eichinger, B., Lewandowski, P., Prueger, J., and Holder, H.: Measurements of OH and HO2 concentrations during the MCMA-2006 field campaign – Part 2: Model comparison and radical budget, Atmos. Chem. Phys., 9, 6655–6675, http://dx.doi.org/10.5194/acp-9-6655-2009doi:10.5194/acp-9-6655-2009, 2009.

Eisenstat, S C., Gursky, M C., Schultz, M H., and Sherman, A H.: Yale Sparse Matrix Package: II. The Nonsymmetric Codes, 1977.

Eisenstat, S C., Gursky, M C., Schultz, M H., and Sherman, A H.: Yale Sparse Matrix Package: I. The Symmetric Codes, Int. J. Num. Meth. Eng., 18, 1145–1151, 1982.

El~Haddad, I., Marchand, N., Dron, J., Temime-Roussel, B., Quivet, E., Wortham, H., Jaffrezo, J L., Baduel, C., Voisin, D., Besombes, J L., and Gille, G.: Comprehensive primary particulate organic characterization of vehicular exhaust emissions in France, Atmos. Environ., 43, 6190–6198, http://dx.doi.org/10.1016/j.atmosenv.2009.09.001doi:10.1016/j.atmosenv.2009.09.001, 2009.

Emmerson, K M., Carslaw, N., Carpenter, L J., Heard, D E., Lee, J D., and Pilling, M J.: Urban atmospheric chemistry during the PUMA campaign 1: Comparison of modelled OH and HO2 concentrations with measurements, J. Atmos. Chem., 52, 143–164, http://dx.doi.org/10.1007/s10874-005-1322-3doi:10.1007/s10874-005-1322-3, 2005.

Finlayson-Pitts, B J.: Reactions at surfaces in the atmosphere: integration of experiments and theory as necessary (but not necessarily sufficient) for predicting the physical chemistry of aerosols, Phys. Chem. Chem. Phys., 11, 7760–7779, http://dx.doi.org/10.1039/b906540gdoi:10.1039/b906540g, 2009.

Finlayson-Pitts, B J. and Pitts, J N.: Tropospheric air pollution: Ozone, airborne toxics, polycyclic aromatic hydrocarbons, and particles, Science, 276, 1045–1052, 1997.

Finlayson-Pitts, B J. and Pitts, J N.: Chemistry of the upper and lower atmosphere, Academic Press, 525 B Street, Suite 1900, San Diego, CA, USA, 92101–4495, 1st edn., 2000.

Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D., Haywood, J., Lean, J., Lowe, D., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., Van~Dorland, R., and IPCC 2007: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge University Press, Cambridge, UK and New York, NY, USA, http://www.ipcc.ch/publications_and_data/ar4/wg1/en/contents.html, 2007.

Fuchs, N A. and Sutugin, A G.: High-dispersed aerosols, in: Topics in current aerosol research, edited by: Hidy, G M. and Brock, J R., Pergamon, New York, USA, 1–60, 1971.

Gerecke, A., Thielmann, A., Gutzwiller, L., and Rossi, M J.: The chemical kinetics of HONO formation resulting from heterogeneous interaction of NO2 with flame soot, Geophys. Res. Lett., 25, 2453–2456, 1998.

Gross, S. and Bertram, A K.: Reactive uptake of NO3, N2O$_5$, NO2, HNO3, and O3 on three types of polycyclic aromatic hydrocarbon surfaces, J. Phys. Chem. A, 112, 3104–3113, http://dx.doi.org/10.1021/jp7107544doi:10.1021/jp7107544, 2008.

Hallquist, M., Wenger, J C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N M., George, C., Goldstein, A H., Hamilton, J F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M E., Jimenez, J L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, T F., Monod, A., Prévôt, A. S H., Seinfeld, J H., Surratt, J D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, http://dx.doi.org/10.5194/acp-9-5155-2009doi:10.5194/acp-9-5155-2009, 2009.

Harner, T. and Bidleman, T F.: Octanol-air partition coefficient for describing particle/gas partitioning of aromatic compounds in urban air, Environ. Sci. Technol., 32, 1494–1502, 1998.

Hindmarsh, A C.: ODEPACK, A Systematized Collection of ODE Solvers, in: Scientific Computing, edited by: Stepleman, R. S., Carver, M., and Peskin, R., Ames, W. F., and Vichnevetsky, R., North-Holland, Amsterdam, 55–64, 1983.

Huff~Hartz, K E., Rosenorn, T., Ferchak, S R., Raymond, T M., Bilde, M., Donahue, N M., and Pandis, S N.: Cloud condensation nuclei activation of monoterpene and sesquiterpene secondary organic aerosol, J. Geophys. Res.-Atmos., 110, http://dx.doi.org/10.1029/2004JD005754doi:10.1029/2004JD005754, 2005.

Ivanov, A V., Trakhtenberg, S., Bertram, A K., Gershenzon, Y M., and Molina, M J.: OH, HO2, and ozone gaseous diffusion coefficients, J. Phys. Chem. A, 111, 1632–1637, http://dx.doi.org/10.1021/jp066558wdoi:10.1021/jp066558w, 2007.

Jimenez, J L., Canagaratna, M R., Donahue, N M., Prévôt, A. S H., Zhang, Q., Kroll, J H., DeCarlo, P F., Allan, J D., Coe, H., Ng, N L., Aiken, A C., Docherty, K S., Ulbrich, I M., Grieshop, A P., Robinson, A L., Duplissy, J., Smith, J D., Wilson, K R., Lanz, V A., Hueglin, C., Sun, Y L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J M., Collins, D R., Cubison, M J., Dunlea, E J., Huffman, J A., Onasch, T B., Alfarra, M R., Williams, P I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J Y., Zhang, Y M., Dzepina, K., Kimmel, J R., Sueper, D., Jayne, J T., Herndon, S C., Trimborn, A M., Williams, L R., Wood, E C., Middlebrook, A M., Kolb, C E., Baltensperger, U., and Worsnop, D R.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, http://dx.doi.org/10.1126/science.1180353doi:10.1126/science.1180353, 2009.

Kanakidou, M., Seinfeld, J H., Pandis, S N., Barnes, I., Dentener, F J., Facchini, M C., Van~Dingenen, R., Ervens, B., Nenes, A., Nielsen, C J., Swietlicki, E., Putaud, J., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G K., Winterhalter, R., Myhre, C. E L., Tsigaridis, K., Vignati, E., Stephanou, E G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, http://dx.doi.org/10.5194/acp-5-1053-2005doi:10.5194/acp-5-1053-2005, 2005.

Kashiwakura, K. and Sakamoto, K.: Emission Characteristics and Cancer Risks of Polycyclic Aromatic Hydrocarbon Emissions from Diesel-fueled Vehicles Complying with Recent Regulations, J. Health Sci., 56, 200–207, 2010.

Khoder, M I.: Diurnal, seasonal and weekdays-weekends variations of ground level ozone concentrations in an urban area in greater Cairo, Environ. Monit. Assess., 149, 349–362, http://dx.doi.org/10.1007/s10661-008-0208-7doi:10.1007/s10661-008-0208-7, 2009.

Kittelson, D B., Watts, W F., and Johnson, J P.: On-road and laboratory evaluation of combustion aerosols–Part1: Summary of diesel engine results, J. Aerosol Sci., 37, 913–930, http://dx.doi.org/10.1016/j.jaerosci.2005.08.005doi:10.1016/j.jaerosci.2005.08.005, 2006.

Kleffmann, J., Becker, K H., Lackhoff, M., and Wiesen, P.: Heterogeneous conversion of NO2 on carbonaceous surfaces, PCCP Phys. Chem. Chem. Phys., 1, 5443–5450, 1999.

Knopf, D A., Mak, J., Gross, S., and Bertram, A K.: Does atmospheric processing of saturated hydrocarbon surfaces by NO3 lead to volatilization?, Geophys. Res. Lett., 33, L17816, http://dx.doi.org/10.1029/2006GL026884doi:10.1029/2006GL026884, 2006.

Knopf, D A., Wang, B., Laskin, A., Moffet, R C., and Gilles, M K.: Heterogeneous nucleation of ice on anthropogenic organic particles collected in Mexico City, Geophys. Res. Lett., 37, L11803, http://dx.doi.org/10.1029/2010GL043362doi:10.1029/2010GL043362, 2010.

Kolb, C E., Cox, R A., Abbatt, J. P D., Ammann, M., Davis, E J., Donaldson, D J., Garrett, B C., George, C., Griffiths, P T., Hanson, D R., Kulmala, M., McFiggans, G., Pöschl, U., Riipinen, I., Rossi, M J., Rudich, Y., Wagner, P E., Winkler, P M., Worsnop, D R., and O'~Dowd, C D.: An overview of current issues in the uptake of atmospheric trace gases by aerosols and clouds, Atmos. Chem. Phys., 10, 10561–10605, http://dx.doi.org/10.5194/acp-10-10561-2010doi:10.5194/acp-10-10561-2010, 2010.

Kotamarthi, V R., Gaffney, J S., Marley, N A., and Doskey, P V.: Heterogeneous NOx chemistry in the polluted PBL, Atmos. Environ., 35, 4489–4498, 2001.

Kotzick, R., Panne, U., and Niessner, R.: Changes in condensation properties of ultrafine carbon particles subjected to oxidation by ozone, J. Aerosol. Sci., 28, 725–735, 1997.

Kroll, J H., Donahue, N M., Jimenez, J L., Kessler, S H., Canagaratna, M R., Wilson, K R., Altieri, K E., Mazzoleni, L R., Wozniak, A S., Bluhm, H., Mysak, E R., Smith, J D., Kolb, C E., and Worsnop, D R.: Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol, Nat. Chem., 28, 133–139, http://dx.doi.org/10.1038/nchem.948doi:10.1038/nchem.948, 2011.

Kwamena, N. O A., Thornton, J A., and Abbatt, J. P D.: Kinetics of surface-bound benzo[\textita]pyrene and ozone on solid organic and salt aerosols, J. Phys. Chem. A, 108, 11626–11634, http://dx.doi.org/10.1021/jp046161xdoi:10.1021/jp046161x, 2004.

Liu, Y., Liu, C., Ma, J., Ma, Q., and He, H.: Structural and hygroscopic changes of soot during heterogeneous reaction with O3, Phys. Chem. Chem. Phys., 12, 10896–10903, http://dx.doi.org/10.1039/c0cp00402bdoi:10.1039/c0cp00402b, 2010.

Maria, S F., Russell, L M., Gilles, M K., and Myneni, S. C B.: Organic aerosol growth mechanisms and their climate-forcing implications, Science, 306, 1921–1924, http://dx.doi.org/10.1126/science.1103491doi:10.1126/science.1103491, 2004.

Matthias, V., Aulinger, A., and Quante, M.: CMAQ simulations of the benzo(\textita)pyrene distribution over Europe for 2000 and 2001, Atmos. Environ., 43, 4078–4086, http://dx.doi.org/10.1016/j.atmosenv.2009.04.058doi:10.1016/j.atmosenv.2009.04.058, 2009.

Molina, M J., Ivanov, A V., Trakhtenberg, S., and Molina, L T.: Atmospheric evolution of organic aerosol, Geophys. Res. Lett., 31, L22104, http://dx.doi.org/10.1029/2004GL020910doi:10.1029/2004GL020910, 2004.

Nguyen, M L., Bedjanian, Y., and Guilloteau, A.: Kinetics of the reactions of soot surface-bound polycyclic aromatic hydrocarbons with NO2, J. Atmos. Chem., 62, 139–150, http://dx.doi.org/10.1007/s10874-010-9144-3doi:10.1007/s10874-010-9144-3, 2009.

Nishino, J.: Adsorption of water Vapor and carbon dioxide at carboxylic functional groups on the surface of coal, Fuel, 80, 757–764, 2001.

Pakbin, P., Ning, Z., Schauer, J J., and Sioutas, C.: Characterization of Particle Bound Organic Carbon from Diesel Vehicles Equipped with Advanced Emission Control Technologies, Environ. Sci. Technol., 43, 4679–4686, http://dx.doi.org/10.1021/es8030825doi:10.1021/es8030825, 2009.

Petters, M D., Prenni, A J., Kreidenweis, S M., DeMott, P J., Matsunaga, A., Lim, Y B., and Ziemann, P J.: Chemical aging and the hydrophobictohydrophilic conversion of carbonaceous aerosol, Geophys. Res. Lett., 33, http://dx.doi.org/10.1029/2006GL027249doi:10.1029/2006GL027249, 2006.

Pöschl, U.: Formation and decomposition of hazardous chemical components contained in atmospheric aerosol particles, J. Aerosol Med.-Depos. Clear. Eff. Lung, 15, 203–212, 2002.

Pöschl, U.: Atmospheric aerosols: Composition, transformation, climate and health effects, Angew. Chem.-Int. Edit., 44, 7520–7540, http://dx.doi.org/10.1002/anie.200501122doi:10.1002/anie.200501122, 2005.

Pöschl, U., Letzel, T., Schauer, C., and Niessner, R.: Interaction of ozone and water vapor with spark discharge soot aerosol particles coated with benzo[\textita]pyrene: O3 and H2O adsorption, benzo[\textita]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, http://dx.doi.org/10.5194/acp-7-5989-2007doi:10.5194/acp-7-5989-2007, 2007.

Ramanathan, V., Crutzen, P J., Kiehl, J T., and Rosenfeld, D.: Atmosphere – Aerosols, climate, and the hydrological cycle, Science, 294, 2119–2124, 2001.

Reisen, F. and Arey, J.: Atmospheric reactions influence seasonal PAH and nitro-PAH concentrations in the Los Angeles basin, Environ. Sci. Technol., 39, 64–73, http://dx.doi.org/10.1021/es035454l10.1021/es035454l, 2005.

Riemer, N., West, M., Zaveri, R A., and Easter, R C.: Simulating the evolution of soot mixing state with a particle-resolved aerosol model, J. Geophys. Res.-Atmos., 114, D09202, http://dx.doi.org/10.1029/2008JD011073doi:10.1029/2008JD011073, 2009.

Rogaski, C A., Golden, D M., and Williams, L R.: Reactive uptake and hydration experiments on amorphous carbon treated with NO2, SO2, O3, HNO3, and H2SO4, Geophys. Res. Lett., 24, 381–384, 1997.

Rogge, W F., Hildemann, L M., Mazurek, M A., Cass, G R., and Simoneit, B. R T.: Sources of Fine Organic Aerosol. 2. Noncatalyst and Catalyst-Equipped Automobiles and Heavy-Duty Diesel Trucks, Environ. Sci. Technol., 27, 636–651, 1993.

Rudich, Y.: Laboratory perspectives on the chemical transformations of organic matter in atmospheric particles, Chem. Rev., 103, 5097–5124, http://dx.doi.org/10.1021/cr020508fdoi:10.1021/cr020508f, 2003.

Rudich, Y., Talukdar, R K., Imamura, T., Fox, R W., and Ravishankara, A R.: Uptake of NO3 on KI solutions: rate coefficient for the NO3 + I$^-$ reaction and gas-phase diffusion coefficients for NO3, Chem. Phys. Lett., 261, 467–473, 1996.

Rudich, Y., Donahue, N M., and Mentel, T F.: Aging of organic aerosol: Bridging the gap between laboratory and field studies, Annu. Rev. Phys. Chem., 58, 321–352, http://dx.doi.org/10.1146/annurev.physchem.58.032806.104432doi:10.1146/annurev.physchem.58.032806.104432, 2007.

Saathoff, H., Naumann, K H., Riemer, N., Kamm, S., Mohler, O., Schurath, U., Vogel, H., and Vogel, B.: The loss of NO2, HNO3, NO3/N2O$_5$, and HO2/HOONO2 on soot aerosol: A chamber and modeling study, Geophys. Res. Lett., 28, 1957–1960, 2001.

Seinfeld, J H. and Pandis, S N.: Atmospheric chemistry and physics, John Wiley & Sons, Inc., 111 River Street, Hoboken, NJ 07030, USA, 2nd edn., 2006.

Shilling, J E., King, S M., Mochida, M., and Martin, S T.: Mass spectral evidence that small changes in composition caused by oxidative aging processes alter aerosol CCN properties, J. Phys. Chem. A, 111, 3358–3368, http://dx.doi.org/10.1021/jp068822rdoi:10.1021/jp068822r, 2007.

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 O3, NO2, H2O, OH and NO3, Atmos. Chem. Phys., 9, 9571–9586, http://dx.doi.org/10.5194/acp-9-9571-2009doi: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, http://www.atmos-chem-phys.net/10/3673/2010/doi:10.5194/acp-10-3673-2010, 2010.

Shiraiwa, M., Sosedova, Y., Rouvière, A., Yang, H., Zhang, Y., Abbatt, J P D., Ammann, M., and Pöschl, U.: The role of long-lived reactive oxygen intermediates in the reaction of ozone with aerosol particles, Nat. Chem., 3, 291–295, http://dx.doi.org/10.1038/nchem.988doi:10.1038/nchem.988, 2011.

Smekens, A., Godoi, R. H M., Berghmans, P., and Van~Grieken, R E.: Characterisation of soot emitted by domestic heating, aircraft and cars using diesel or biodiesel, J. Atm. Chem., 52, 45–62, http://dx.doi.org/10.1007/s10874-005-6903-7doi:10.1007/s10874-005-6903-7, 2005.

Springmann, M., Knopf, D A., and Riemer, N.: Detailed heterogeneous chemistry in an urban plume box model: reversible co-adsorption of O3, NO2, and H2O on soot coated with benzo[\textita]pyrene, Atmos. Chem. Phys., 9, 7461–7479, http://dx.doi.org/10.5194/acp-9-7461-2009doi:10.5194/acp-9-7461-2009, 2009.

Tabor, K., Gutzwiller, L., and Rossi, M J.: Heterogeneous chemical kinetics of NO2 on amorphous carbon at ambient temperature, J. Phys. Chem., 98, 6172–6186, 1994.

Tie, X., Brasseur, G., Emmons, L., Horowitz, L., and Kinnison, D.: Effects of aerosols on tropospheric oxidants: A global model study, J. Geophys. Res.-Atmos., 106, 22931–22964, 2001.

Vione, D., Barra, S., De~Gennaro, G., De~Rienzo, M., Gilardoni, S., Perrone, M G., and Pozzoli, L.: Polycyclic aromatic hydrocarbons in the atmosphere: monitoring, sources, sinks and fate. II: Sinks and fate, Ann. Chim., 94, 257–268, 2004.

Wang, J., Cubison, M J., Aiken, A C., Jimenez, J L., and Collins, D R.: The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols, Atmos. Chem. Phys., 10, 7267–7283, http://dx.doi.org/10.5194/acp-10-7267-2010doi:10.5194/acp-10-7267-2010, 2010.

Weingartner, E., Burtscher, H., and Baltensperger, U.: Hygroscopic properties of carbon and diesel soot particles, Atmos. Environ., 31, 2311–2327, 1997.

Zaveri, R A. and Peters, L K.: A new lumped structure photochemical mechanism for large-scale applications, J. Geophys. Res.-Atmos., 104, 30387–30415, 1999.

Zaveri, R A., Easter, R C., and Peters, L K.: A computationally efficient multicomponent equilibrium solver for aerosols (MESA), J. Geophys. Res.-Atmos., 110, D24203, \doi10.1029/2004JD005618, 2005a.

Zaveri, R A., Easter, R C., and Wexler, A S.: A new method for multicomponent activity coefficients of electrolytes in aqueous atmospheric aerosols, J. Geophys. Res.-Atmos., 110, D02201, \doi10.1029/2004JD004681, 2005b.

Zaveri, R A., Easter, R C., Fast, J D., and Peters, L K.: Model for Simulating Aerosol Interactions and Chemistry (MOSAIC), J. Geophys. Res.-Atmos., 113, D13204, http://dx.doi.org/10.1029/2007JD008782doi:10.1029/2007JD008782, 2008.