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<article language="en">
	<journal>
		<journal_title>Atmospheric Chemistry and Physics</journal_title>
		<journal_url>www.atmos-chem-phys.net</journal_url>
		<issn>1680-7316</issn>
		<eissn>1680-7324</eissn>
		<volume_number>8</volume_number>
		<issue_number>19</issue_number>
		<publication_year>2008</publication_year>
	</journal>
	<doi>10.5194/acp-8-5899-2008</doi>
	<article_url>http://www.atmos-chem-phys.net/8/5899/2008/</article_url>
	<abstract_html>http://www.atmos-chem-phys.net/8/5899/2008/acp-8-5899-2008.html</abstract_html>
	<fulltext_pdf>http://www.atmos-chem-phys.net/8/5899/2008/acp-8-5899-2008.pdf</fulltext_pdf>
	<start_page>5899</start_page>
	<end_page>5917</end_page>
	<publication_date>2008-10-15</publication_date>
	<article_title content_type="html">Consistent simulation of bromine chemistry from the marine boundary layer to the stratosphere â€“ Part 1: Model description, sea salt aerosols and pH</article_title>
	<authors>
		<author numeration="1" affiliations="1,2">
			<name>A. Kerkweg</name>
			<email>akerkweg@mpch-mainz.mpg.de</email>
		</author>
		<author numeration="2" affiliations="1">
			<name>P. JÃ¶ckel</name>
		</author>
		<author numeration="3" affiliations="1">
			<name>A. Pozzer</name>
		</author>
		<author numeration="4" affiliations="1">
			<name>H. Tost</name>
		</author>
		<author numeration="5" affiliations="1">
			<name>R. Sander</name>
		</author>
		<author numeration="6" affiliations="3">
			<name>M. Schulz</name>
		</author>
		<author numeration="7" affiliations="4">
			<name>P. Stier</name>
		</author>
		<author numeration="8" affiliations="5">
			<name>E. Vignati</name>
		</author>
		<author numeration="9" affiliations="5">
			<name>J. Wilson</name>
		</author>
		<author numeration="10" affiliations="1">
			<name>J. Lelieveld</name>
		</author>
	</authors>
	<affiliations>
		<affiliation numeration="1" content_type="html">MPI for Chemistry (Otto Hahn Institute), Atmospheric Chemistry Department, P.O. Box 3060, 55020 Mainz, Germany</affiliation>
		<affiliation numeration="2" content_type="html">Institute for Atmospheric Physics, University of Mainz, Mainz, Germany</affiliation>
		<affiliation numeration="3" content_type="html">Laboratoire des Sciences du Climat et de l&apos;Environnement, CEA-IPSL, Saclay, France</affiliation>
		<affiliation numeration="4" content_type="html">Atmospheric, Oceanic and Planetary Physics, University of Oxford, Oxford, UK</affiliation>
		<affiliation numeration="5" content_type="html">Joint Research Centre, Institute of Environment and Sustainability, Ispra, Italy</affiliation>
	</affiliations>
	<abstract content_type="html">This is the first article of a series presenting a detailed analysis of
bromine chemistry simulated with the atmospheric chemistry general
circulation model ECHAM5/MESSy. Release from sea salt is an important bromine
source, hence the model explicitly calculates aerosol chemistry and phase
partitioning for coarse mode aerosol particles. Many processes including
chemical reaction rates are influenced by the particle size distribution, and
aerosol associated water strongly affects the aerosol pH. Knowledge of the
aerosol pH is important as it determines the aerosol chemistry, e.g., the
efficiency of sulphur oxidation and bromine release. Here, we focus on the
simulated sea salt aerosol size distribution and the coarse mode aerosol pH.
&lt;br&gt;&lt;br&gt;
A comparison with available field data shows that the simulated aerosol
distributions agree reasonably well within the range of measurements. In
spite of the small number of aerosol pH measurements and the uncertainty in
its experimental determination, the simulated aerosol pH compares well with
the observations. The aerosol pH ranges from alkaline aerosol in areas of
strong production down to pH-values of 1 over regions of medium sea salt
production and high levels of gas phase acids, mostly polluted regions over
the oceans in the Northern Hemisphere.</abstract>
	<references>
		<reference numeration="1" content_type="text"> Balkanski, Y., Schulz, M., Claquin, T., Moulin, C., and Ginoux, P.: Global emissions of mineral aerosol: Formulation and validation using satellite imagery, Emission of Atmospheric Tracer Compounds, Kluwer Academic Publisher, Norwell, 253â€“282, 2003. </reference>
		<reference numeration="2" content_type="text"> Bates, T S., Kapustin, V N., Quinn, P K., Covert, D S., Coffman, D J., Mari, C., Dirkee, P A., Bruyn, W. J D., and Saltzman, E S.: Processes controlling the distribution of aerosol particles in the lower marine boundary layer during the First Aerosol Charaterization Experiment (ACE1), J. Geophys. Res., 103, 16 369â€“16 383, 1998. </reference>
		<reference numeration="3" content_type="text"> Brasseur, G P. and Solomon, S.: Aeronomy of the middle atmosphere, Springer-Verlag, Dordecht, The Netherlends, 2005. </reference>
		<reference numeration="4" content_type="text"> Buchholz, J.: Simulations of Physics and Chemistry of Polar Stratospheric Clouds with a General Circulation Model, Ph.D. thesis, Johannes Gutenberg-UniversitÃ¤t, Fachbereich Physik, http://nbn-resolving.de/urn/resolver.pl?urn=urn:nbn:de:hebis:77-8187, 2005. </reference>
		<reference numeration="5" content_type="text"> Damian, V., Sandu, A., Damian, M., Potra, F., and Carmichael, G R.: The kinetic preprocessor KPP â€“ a software enviroment for solving chemical kinetics, Comput. Chem. Eng., 26, 1567â€“1579, 2002. </reference>
		<reference numeration="6" content_type="text"> Dentener, F., Kinne, S., Bond, T., Boucher, O., Cofala, J., Generoso, S., Ginoux, P., Gong, S., Hoelzemann, J. J., Ito, A., Marelli, L., Penner, J. E., Putaud, J.-P., Textor, C., Schulz, M., van der Werf, G. R., and Wilson, J.: Emissions of primary aerosol and precursor gases in the years 2000 and 1750 prescribed data-sets for AeroCom, Atmos. Chem. Phys., 6, 4321â€“4344, 2006. </reference>
		<reference numeration="7" content_type="text"> Duce, R A.: Sea/air exchange of pollution and natural substances: The SEAREX Program, Proceedings of the WMO Technical Conference on Regional and Global Observation of Atmospheric Pollution Relative to Climate, Report, No 14, WMO No 549, World Meteorological Organization, Geneva, 1982. </reference>
		<reference numeration="8" content_type="text"> Fitzgerald, J W.: Marine Aerosols: A Review, Atmos. Environ., 25A, 533â€“545, 1991. </reference>
		<reference numeration="9" content_type="text"> Fridlind, A. and Jacobson, M.: A study of gas-aerosol equilibrium and aerosol pH in the remote marine boundary layer during the First Aerosol Characterization Experiment (ACE~1), J. Geophys. Res., 105, 17 325â€“17 340, 2000. %% </reference>
		<reference numeration="10" content_type="text"> %%Ganzeveld, L. and Lelieveld, J.: Dry deposition parameterization in a chemistry %% general circulation model and its influence on the distribution of reactive %% trace gases, J. Geophys. Res., 100, 20 999â€“21 012, 1995. </reference>
		<reference numeration="11" content_type="text"> Giorgetta, M A., Manzini, E., and Roeckner, E.: Forcing of the quasi-biennial oscillation from a broad spectrum of atmospheric waves, Geophys. Res. Lett., 29, 1245, doi:10.1029/2002GL014756, 2002. </reference>
		<reference numeration="12" content_type="text"> Giorgetta, M A., Manzini, E., Roeckner, E., Esch, M., and Bengtson, L.: Climatology and forcing of the quasi-biennial oscillation in the MAECHAM5 model, J. Clim., 19, 3882â€“3901, 2006. </reference>
		<reference numeration="13" content_type="text"> Gong, S L., Barrie, L A., Blanchet, J.-P., von Salzen, K., Lohmann, U., Lesins, G., Spacek, L., Zhang, L M., Girard, E., Lin, H., Leaitch, R., Leighton, H., Chylek, P., and Huang, P.: Canadian Aerosol Module: A size-segregated simulation of atmospheric aerosol processes for climate and air quality models 1. Module development, J. Geophys. Res., 108, 4007, doi:10.1029/2001JD002002, 2003.  </reference>
		<reference numeration="14" content_type="text"> Guazzotti, S A., Coffee, K R., and Parther, K A.: Continuous measurements of size-resolved particle chemistry during INDOEX-Intensive Field Phase~99, J. Geophys. Res., 106, 28 607â€“28 627, 2001. </reference>
		<reference numeration="15" content_type="text"> Guelle, W., Schulz, M., Balkanski, Y., and Dentener, F.: Influence of the source formulation on modeling the atmospheric global distribution of sea salt aerosol, J. Geophys. Res., 106, 27 509â€“27 524, 2001. </reference>
		<reference numeration="16" content_type="text"> Jeuken, A., Siegmund, P., Heijboer, L., Feichter, J., and Bengtson, L.: On the potential of assimilating meteorological analysis in a climate model for the purpose of model validation, J. Geophys. Res., 101, 16 939â€“16 950, 1996. </reference>
		<reference numeration="17" content_type="text"> JÃ¶ckel, P., Sander, R., Kerkweg, A., Tost, H., and Lelieveld, J.: Technical Note: The Modular Earth Submodel System (MESSy) â€“ a new approach towards Earth System Modeling, Atmos. Chem. Phys., 5, 433â€“444, 2005. </reference>
		<reference numeration="18" content_type="text"> JÃ¶ckel, P., Tost, H., Pozzer, A., BrÃ¼hl, C., Buchholz, J., Ganzeveld, L., Hoor, P., Kerkweg, A., Lawrence, M. G., Sander, R., Steil, B., Stiller, G., Tanarhte, M., Taraborrelli, D., van Aardenne, J., and Lelieveld, J.: The atmospheric chemistry general circulation model ECHAM5/MESSy1: consistent simulation of ozone from the surface to the mesosphere, Atmos. Chem. Phys., 6, 5067â€“5104, 2006. </reference>
		<reference numeration="19" content_type="text"> Keene, W C. and Galloway, J.: Consideration Regarding Sources for Formic and Acetic Acids in the Troposphere, J. Geophys. Res., 91, 14 466â€“14 474, 1986. </reference>
		<reference numeration="20" content_type="text"> Keene, W. and Savoie, D.: The pH of deliquesced sea-salt aerosol in polluted air, Geophys. Res. Lett., 25, 2181â€“2184, 1998. </reference>
		<reference numeration="21" content_type="text"> Keene, W. and Savoie, D.: Correction to &quot;The pH of deliquesced sea-salt aerosol in polluted air&quot;, Geophys. Res. Lett., 26, 1315â€“1316, 1999. </reference>
		<reference numeration="22" content_type="text"> Keene, W., Pszenny, A., Maben, J., Stevenson, E., and Wall, A.: Closure evaluation of size-resolved aerosol pH in the New England coastal atmosphere during summer, J. Geophys. Res., 109, D23307, doi:10.1029/2004JD004801, 2004. </reference>
		<reference numeration="23" content_type="text"> Keene, W C., Sander, R., Pszenny, A A., Vogt, R., Crutzen, P J., and Galloway, J N.: Aerosol pH in the marine boundary layer: A review and model evaluation, J. Aerosol Sci., 29, 339â€“356, 1998. </reference>
		<reference numeration="24" content_type="text"> Keene, W C., Pszenny, A. A P., Maben, J R., and Sander, R.: Variation of marine aerosol acidity with particle size, Geophys. Res. Lett., 29, 1101, doi:10.1029/2001GL013881, 2002. </reference>
		<reference numeration="25" content_type="text"> Kerkweg, A., Buchholz, J., Ganzeveld, L., Pozzer, A., Tost, H., and JÃ¶ckel, P.: Technical Note: An implementation of the dry removal processes DRY DEPosition and SEDImentation in the Modular Earth Submodel System (MESSy), Atmos. Chem. Phys., 6, 4617â€“4632, 2006a. </reference>
		<reference numeration="26" content_type="text"> Kerkweg, A., Sander, R., Tost, H., and JÃ¶ckel, P.: Technical note: Implementation of prescribed (OFFLEM), calculated (ONLEM), and pseudo-emissions (TNUDGE) of chemical species in the Modular Earth Submodel System (MESSy), Atmos. Chem. Phys., 6, 3603â€“3609, 2006b. </reference>
		<reference numeration="27" content_type="text"> Kerkweg, A., Sander, R., Tost, H., JÃ¶ckel, P., and Lelieveld, J.: Technical Note: Simulation of detailed aerosol chemistry on the global scale using MECCA-AERO, Atmos. Chem. Phys., 7, 2973â€“2985, 2007. </reference>
		<reference numeration="28" content_type="text"> Landgraf, J. and Crutzen, P.: An Efficient Method for Online Calculation of Photolysis and Heating Rates, J. Atmos. Sci., 55, 863â€“878, 1998. </reference>
		<reference numeration="29" content_type="text"> Lauer, A., Hendricks, J., Ackermann, I., Schell, B., Hass, H., and Metzger, S.: Simulating aerosol microphysics with the ECHAM/MADE GCM - Part~I: Model description and comparison with observations, Atmos. Chem. Phys., 5, 3251â€“3276, 2005. </reference>
		<reference numeration="30" content_type="text"> Lewis, E R. and Schwartz, S E.: Sea Salt Aerosol Production: Mechanisms, Methods, Measurements and Models â€“ A Critical Review, American Geophysical Union, Washington, D.C., 2004. </reference>
		<reference numeration="31" content_type="text"> Maring, H., Savioe, D., Izaguirre, M., and Custals, L.: Vertical distribution of dust and sea-salt aerosol over Puerto Rico during PRIDE measured from a light aircraft, J. Geophys. Res., 108, 8587, \doi10.1029/2002JD002544, 2003. </reference>
		<reference numeration="32" content_type="text"> Monahan, E C.: The Role of Air-Sea Exchange in Geochemical Cycling, chap. The Ocean as a Source for Atmospheric Particles, D. Reidel Publishing Company, 129â€“163, 1986. </reference>
		<reference numeration="33" content_type="text"> Murphy, D., Thomson, D., Middlebrook, A., and Schein, M.: In situ single-particle characterization at Cape Grim, J. Geophys. Res., 103, 16 485â€“16 491, 1998. </reference>
		<reference numeration="34" content_type="text"> O&apos;Dowd, C D. and Smith, M H.: Physicochemical Properties of Aerosols Over the Northeast Atlantic: Evidence for Wind-Speed-Related Submicron Sea-Salt Aerosol Production, J. Geophys. Res., 98, 1137â€“1149, 1993. </reference>
		<reference numeration="35" content_type="text"> Phinney, L., Leaitch, W R., Lohmann, U., Boudires, H., Worsnop, D R., Jayne, J T., Toom-Sauntry, D., Wadleigh, M., Sharma, S., and Shantz, N.: Characterization of the aerosol over the sub-arctic north east Pacific Ocean, Deep-Sea Res., 53, 2410â€“2433, 2006. </reference>
		<reference numeration="36" content_type="text"> Pierce, J R. and Adams, P J.: Global evaluation of CCN formation by direct emission of sea salt and growth of ultrafine sea salt, J. Geophys. Res., 111, D06203, doi:10.1029/2005JD006186, 2006. </reference>
		<reference numeration="37" content_type="text"> Pozzer, A., JÃ¶ckel, P., Sander, R., Williams, J., Ganzeveld, L., and Lelieveld, J.: Technical Note: The MESSy-submodel AIRSEA calculating the air-sea exchange of chemical species, Atmos. Chem. Phys., 6, 5435â€“5444, 2006. </reference>
		<reference numeration="38" content_type="text"> Pozzer, A., JÃ¶ckel, P., Tost, H., Sander, R., Ganzeveld, L., Kerkweg, A., and Lelieveld, J.: Simulating organic species with the global atmospheric chemistry general circulation model ECHAM5/MESSy1: a comparison of model results with observations, Atmos. Chem. Phys., 7, 2527â€“2550, 2007. </reference>
		<reference numeration="39" content_type="text"> Pszenny, A. A. P., MoldanovÃ¡, J., Keene, W. C., Sander, R., Maben, J. R., Martinez, M., Crutzen, P. J., Perner, D., and Prinn, R. G.: Halogen cycling and aerosol pH in the Hawaiian marine boundary layer, Atmos. Chem. Phys., 4, 147â€“168, 2004. </reference>
		<reference numeration="40" content_type="text"> Roeckner, E., BÃ¤uml, G., Bonaventura, L., Brokopf, R., Esch, M., Giorgetta, M., Hagemann, S., Kirchner, I., Kornblueh, L., Manzini, E., Rhodin, A., Schlese, U., Schulzweida, U., and Tompkins, A.: The atmospheric general circulation model ECHAM5, Tech. Rep. MPI-Report~349, Max Planck-Institute for Meteorology, Hamburg, http://www.mpimet.mpg.de/fileadmin/publikationen/Reports/max_scirep_349.pdf , 2003. </reference>
		<reference numeration="41" content_type="text"> Roeckner, E., Brokopf, R., Esch, M., Giorgetta, M., Hagemann, S., Kornblueh, L., Manzini, E., Schlese, U., and Schulzweida, U.: The atmospheric general circulation model ECHAM5. PART II: Sensitivity of Simulated Climate to Horizontal and Vertical Resolution, Tech. Rep. MPI-Report~354, MPI for Meteorology, Hamburg, http://www.mpimet.mpg.de/fileadmin/publikationen/Reports/max_scirep_354.pdf , 2004. </reference>
		<reference numeration="42" content_type="text"> Sander, R. and Crutzen, P.: Model study indicating halogen activation and ozone destruction in polluted air masses transported to the sea, J. Geophys. Res., 101, 9121â€“9138, 1996. </reference>
		<reference numeration="43" content_type="text"> Sander, R., Keene, W. C., Pszenny, A. A. P., Arimoto, R., Ayers, G. P., Baboukas, E., Cainey, J. M., Crutzen, P. J., Duce, R. A., H\&quot;önninger, G., Huebert, B. J., Maenhaut, W., Mihalopoulos, N., Turekian, V. C., and Van~Dingenen, R.: Inorganic bromine in the marine boundary layer: a critical review, Atmos. Chem. Phys., 3, 1301â€“1336, 2003. </reference>
		<reference numeration="44" content_type="text"> Sander, R., Kerkweg, A., J\&quot;öckel, P., and Lelieveld, J.: Technical note: The new comprehensive atmospheric chemistry module MECCA, Atmos. Chem. Phys., 5, 445â€“450, 2005. </reference>
		<reference numeration="45" content_type="text"> Sandu, A. and Sander, R.: Technical note: Simulating chemical systems in Fortran90 and Matlab with the Kinetic PreProcessor KPP-2.1, Atmos. Chem. Phys., 6, 187â€“195, 2006. </reference>
		<reference numeration="46" content_type="text"> Schulz, M., de~Leeuw, G., and Balkanski, Y.: Emission of atmospheric trace compounds, Sea-salt aerosol source functions and emissions, Kluwer Academic, 333â€“359, 2004. </reference>
		<reference numeration="47" content_type="text"> Smith, M H. and Harrison, M.: The Sea Spray Generation Function, J. Aerosol Sci., 29, Suppl 1, S189â€“S190, 1998. </reference>
		<reference numeration="48" content_type="text"> Spracklen, D. V., Pringle, K. J., Carslaw, K. S., Chipperfield, M. P., and Mann, G. W.: A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties, Atmos. Chem. Phys., 5, 2227â€“2252, 2005. </reference>
		<reference numeration="49" content_type="text"> Stier, P., Feichter, J., Kinne, S., Kloster, S., Vignati, E., Wilson, J., Ganzeveld, L., Tegen, I., Werner, M., Balkanski, Y., Schulz, M., Boucher, O., Minikin, A., and Petzold, A.: The aerosol-climate model ECHAM5-HAM, Atmos. Chem. Phys., 5, 1125â€“1156, 2005. </reference>
		<reference numeration="50" content_type="text"> Textor, C., Schulz, M., Guibert, S., Kinne, S., Balkanski, Y., Bauer, S., Berntsen, T., Berglen, T., Boucher, O., Chin, M., Dentener, F., Diehl, T., Easter, R., Feichter, H., Fillmore, D., Ghan, S., Ginoux, P., Gong, S., Grini, A., Hendricks, J., Horowitz, L., Huang, P., Isaksen, I., Iversen, I., Kloster, S., Koch, D., Kirkev&amp;aring;g, A., Kristjansson, J. E., Krol, M., Lauer, A., Lamarque, J. F., Liu, X., Montanaro, V., Myhre, G., Penner, J., Pitari, G., Reddy, S., Seland, Ã˜., Stier, P., Takemura, T., and Tie, X.: Analysis and quantification of the diversities of aerosol life cycles within AeroCom, Atmos. Chem. Phys., 6, 1777â€“1813, 2006.  </reference>
		<reference numeration="51" content_type="text"> Tost, H., JÃ¶ckel, P., Kerkweg, A., Sander, R., and Lelieveld, J.: Technical note: A new comprehensive SCAVenging submodel for global atmospheric chemistry modelling, Atmos. Chem. Phys., 6, 565â€“574, 2006. </reference>
		<reference numeration="52" content_type="text"> Tost, H., JÃ¶ckel, P., and Lelieveld, J.: Influence of different convection parameterisations in a GCM, Atmos. Chem. Phys., 6, 5475â€“5493, 2006. </reference>
		<reference numeration="53" content_type="text"> Tost, H., JÃ¶ckel, P., and Lelieveld, J.: Lightning and convection parameterisations â€“ uncertainties in global modelling, Atmos. Chem. Phys., 7, 4553â€“4568, 2007. </reference>
		<reference numeration="54" content_type="text"> VehkamÃ¤ki, H., nad I Napari, M K., Lehtinen, K., Timmreck, C., Noppel, M., and Laaksonen, A.: An improved parameterization for sulfuric acid-water nucleation rates for tropospheric and stratospheric conditions, J. Geophys. Res., 107, 4622, doi:10.1029/2002JD002184, 2002. </reference>
		<reference numeration="55" content_type="text"> Vignati, E., Wilson, J., and Stier, P.: M7: An efficient size-resolved aerosol microphysics module for large-scale aerosol transport, J. Geophys. Res., 109, D22202, doi:10.1029/2003JD004486, 2004. </reference>
		<reference numeration="56" content_type="text"> von~Glasow, R. and Sander, R.: Variation of sea salt aerosol pH with relative humidity, Geophys. Res. Lett., 28, 247â€“250, 2001. </reference>
		<reference numeration="57" content_type="text"> von~Glasow, R., Sander, R., Bott, A., and Crutzen, P.: Modeling halogen chemistry in the marine boundary layer~1. Cloud-free MBL, J. Geophys. Res., 107, 4341, doi:10.1029/2001JD000942, 2002. </reference>
		<reference numeration="58" content_type="text"> Wagner, T., Leue, C., Wenig, M., Pfeilsticker, K., and Platt, U.: Spatial and temporal distribution of enhanced boundary layer BrO concentrations measured by GOME instrument onboard ERS-2, J. Geophys. Res., 106, 24 225â€“24 235, 2001. %% </reference>
		<reference numeration="59" content_type="text"> %% Wesely, M.: Parameterization of the surface resistances to gaseous dry %% depposition in regional-scale numerical models, Atmos. Environ., 23, %% 1293â€“1304, 1989. </reference>
		<reference numeration="60" content_type="text"> Wilson, J., Cuvelier, C., and Raes, F.: A modeling study of global mixed aerosol fields, J. Geophys. Res., 106, 34 081â€“34 108, 2001. </reference>
	</references>
</article>

