Geoscientific Model Development Discussions www.geosci-model-dev-discuss.net 1991-9611 1991-962X 2 1 2009 10.5194/gmdd-2-385-2009 http://www.geosci-model-dev-discuss.net/2/385/2009/ http://www.geosci-model-dev-discuss.net/2/385/2009/gmdd-2-385-2009.html http://www.geosci-model-dev-discuss.net/2/385/2009/gmdd-2-385-2009.pdf 385 453 2009-05-07 ECHMERIT V1.0 – a new global fully coupled mercury-chemistry and transport model G. Jung g.jung@cs.iia.cnr.it I. M. Hedgecock N. Pirrone CNR – Institute for Atmospheric Pollution, Division of Rende, 87036 Rende, Italy Mercury is a global pollutant due to its long lifetime in the atmosphere. Its hemispheric transport patterns and eventual deposition are therefore of major concern. For the purpose of global atmospheric mercury chemistry and transport modelling the ECHMERIT model was developed. ECHMERIT, based on the global circulation model ECHAM5 differs from most global mercury models in that the emissions, chemistry (including general tropospheric chemistry and mercury chemistry), transport and deposition are coupled on-line to the GCM. The chemistry mechanism includes an online calculation of photolysis rate constants using the Fast-J photolysis mechanism, the CBM-Z tropospheric gas-phase mechanism and aqueous-phase chemistry based on the MECCA mechanism. Additionally, a mercury chemistry mechanism that incorporates gas and aqueous phase mercury chemistry is included. A detailed description of the model, including the wet and dry deposition modules, and the implemented emissions is given in this technical report. First model testing and evaluation show a satisfactory model performance for surface ozone and mercury concentrations (with a mean bias of 1.46 ppb for ozone and a mean bias of 13.55 ppq for TGM when compared with EMEP station data). Requirements regarding measurement data and emission inventories which could considerably improve model skill are discussed. Ariya, P A., Khalizov, A., and Gidas, A.: Reactions of gaseous mercury with atomic and molecular halogens: kinetics, product studies, and atmospheric implications, J. Phys. Chem. A, 106, 7310–7320, 2002. Ariya, P A., Snider, G., and Amyot, M.: Mercury transformation at environmental surfaces: Feedbacks to the atmosphere, chapter 15, in: Mercury Fate and Transport in the Global Atmosphere: Measurements, Models and Policy Implications; Interim Report of the UNEP Global Partnership on Atmospheric Mercury Transport and Fate Research, 345–376, 2008. Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., and IUPAC Subcommittee, : Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – gas phase reactions of organic species, Atmos. Chem. Phys., 6, 3625–4055, 2006. Bey, I., Jacob, D J., Yantosca, R M., Logan, J A., Field, B D., Fiore, A M., Li, Q., Liu, H Y., Mickley, L J., and Schultz, M G.: Global modeling of tropospheric chemistry with assimilated meteorology – Model description and evaluation, J. Geophys. Res., 106, 23073–23095, 2001. Brinkop, S. and Sausen, R.: A finite difference approximation for convective transports which maintains positive tracer concentrations, Contributions to Atmospheric Physics, 70, 245–248, 1997. Bullock, O R.: Current methods and research strategies for modeling atmospheric mercury, Fuel Process. Technol., 65–66, 459–471, 2000. CAMx: CAMx, user's guide, version 4.40, Environ International Corporation, California, 2006. Chang, J C. and Hanna, S R.: Air quality model performance evaluation, Meteorol. Atmos. Phys., 87, 167–196, 2004. Christensen, J. H., Brandt, J., Frohn, L. M., and Skov, H.: Modelling of Mercury in the Arctic with the Danish Eulerian Hemispheric Model, Atmos. Chem. Phys., 4, 2251–2257, 2004. Clever, H L., Johnson, S A., and Derrick, M E.: The solubility of Mercury and Some Sparingly Soluble Mercury Salts in Water and Aqueous Electrolyte Solutions, J. Phys. Chem. Ref. Data, 14, 631–680, 1985. Damina-Iordache, V., Sandu, A., Damian-Iordache, M., Carmichael, G R., and Potra, F A.: The kinetic preprocessor KPP: a software environment for solving chemical kinetics, Computers Chemical Engineering, 26, 1567–1579, 2002. Dastoor, A P. and Larocque, Y.: Global circulation of atmospheric mercury: a modelling study, Atmos. Environ., 38, 147–161, 2004. Ebinghaus, R., Kock, H H., Coggins, A M., Spain, T G., Jennings, S G., and Temme, C.: Long-term measurements of atmospheric mercury at Mace Head, Irish west coast, between 1995 and 2001, Atmos. Environ., 36, 5267–5276, 2002. Ebinghaus, R., Banic, C., Beauchamp, S., Jaffe, D., Kock, H H., Pirrone, N., Poissant, L., Sprovieri, F., and Weiss, P S.: Spatial coverage and temporal trends of land-based atmospheric mercury measurements in the northern and southern hemispheres, chapter 9, in: Mercury Fate and Transport in the Global Atmosphere: Measurements, Models and Policy Implications; Interim Report of the UNEP Global Partnership on Atmospheric Mercury Transport and Fate Research, 168–219, 2008. Eckhardt, S., Stohl, A., Beirle, S., Spichtinger, N., James, P., Forster, C., Junker, C., Wagner, T., Platt, U., and Jennings, S. G.: The North Atlantic Oscillation controls air pollution transport to the Arctic, Atmos. Chem. Phys., 3, 1769–1778, 2003. Friedli, H R., Arellano, A F., Cinnirella, S., and Pirrone, N.: Mercury emissions from global biomass burning: spatial and temporal distribution, chapter 8, in: Mercury Fate and Transport in the Global Atmosphere: Measurements, Models and Policy Implications; Interim Report of the UNEP Global Partnership on Atmospheric Mercury Transport and Fate Research, 145–167, 2008. 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, 20999–21012, 1995. Ganzeveld, L., Lelieveld, J., and Roelofs, G.-J.: A dry deposition parameterization for sulfur oxides in a chemistry and general circulation model, J. Geophys. Res., 103, 5679–5694, 1998. Ganzeveld, L. N., van Aardenne, J. A., Butler, T. M., Lawrence, M. G., Metzger, S. M., Stier, P., Zimmermann, P., and Lelieveld, J.: Technical Note: Anthropogenic and natural offline emissions and the online EMissions and dry DEPosition submodel EMDEP of the Modular Earth Submodel system (MESSy), Atmos. Chem. Phys. Discuss., 6, 5457–5483, 2006. Gårdfeldt, K. and Jonsson, M.: Is bimolecular reduction of Hg(II) complexes possible in aqueous systems of environmental importance, J. Phys. Chem. A, 107, 4478–4482, 2003. Granier, C., Lamarque, J F., Mieville, A., Muller, J F., Olivier, J., Orlando, J., Peters, J., Petron, G., Tyndall, G., and Wallens, S.: POET, a database of surface emissions of ozone precursors, available at: http://www.aero.jussieu.fr/projet/ACCENT/POET.php, 2005. Hagemann, S.: An improved land surface parameter dataset for global and regional climate models, Max-Planck-Institut für Meteorologie, 2002. Hall, B.: The gas phase oxidation of elemental mercury by ozone, Water Air Soil Poll., 80, 301–315, 1995. Hall, B. and Bloom, N S.: Report to the Electric Power Research Institute, Palo Alto, CA, 1993. Hedgecock, I M. and Pirrone, N.: Chasing quicksilver: Modeling the atmospheric lifetime of \chemHg^0(g) in the marine boundary layer at various latitudes, Environ. Sci. Technol., 38, 69–76, 2004. Hedgecock, I M., Trunfio, G A., Pirrone, N., and Sprovieri, F.: Mercury chemistry in the MBL: Mediterranean case and sensitivity studies using the AMCOTS (Atmospheric Mercury Chemistry over the Sea) model, Atmos. Environ., 39, 7217–7230, \doi10.1016/j.atmosenv.2005.09.002, 2005. Hedgecock, I M., Pirrone, N., Trunfio, G A., and Sprovieri, F.: Integrated mercury cycling, transport, and air-water exchange (MECAWEx) model, J. Geophys. Res., 111, D20302, \doi10.1029/2006JD007117, 2006. Horowitz, L W., Walters, S., Mauzerall, D L., Emmons, L K., Rasch, P J., Granier, C., Tie, X., Lamarque, J F., Schultz, M G., Tyndall, G S., et~al.: A global simulation of tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2, J. Geophys. Res., 108(D24), 4784, \doi10.1029/2002JD002853, 2003. Hynes, A J., Donohoue, D L., Goodsite, M E., and Hedgecock, I M.: Our current understanding of major chemical and physical processes affecting mercury dynamics in the atmosphere and at the air-water/terrestrial interfaces, chapter 14, in: Mercury Fate and Transport in the Global Atmosphere: Measurements, Models and Policy Implications Interim Report of the UNEP Global Partnership on Atmospheric Mercury Transport and Fate Research, 322–344, 2008. Jacobson, M Z.: Fundamentals of Atmospheric Modeling, Cambridge University Press, 1999. Jaeglé, L., Strode, S A., Selin, N E., and Jacob, D J.: The GEOS-chem model, chapter 18, in: Mercury Fate and Transport in the Global Atmosphere: Measurements, Models and Policy Implications; Interim Report of the UNEP Global Partnership on Atmospheric Mercury Transport and Fate Research, 401–410, 2008. Kerkweg, A., Buchholz, J., Ganzeveld, L., Pozzer, A., Tost, H., and Jöckel, 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, 4617–4632, 2006. Liang, Q., Jaeglé, L., Jaffe, D A., Weiss-Penzias, P., Heckman, A., and Snow, J A.: Long-range transport of Asian pollution to the northeast Pacific: Seasonal variations and transport pathways of carbon monoxide, J. Geophys. Res., 109, D23S07, doi:10.1029/2003JD004402, 2004. Lin, C.-J. and Pehkonen, S O.: Aqueous free radical chemistry of mercury in the presence of iron oxides and ambient aerosol, Atmos. Environ., 31, 4125–4137, 1997. Lin, C.-J. and Pehkonen, S O.: Aqueous Phase Reactions of Mercury with Free Radicals and Chlorine: Implications for Atmospheric Mercury Chemistry, Chemosphere, 38, 1253–1263, 1999. Lin, S J. and Rood, R B.: Multidimensional Flux-Form Semi-Lagrangian Transport Schemes, Mon. Weather Rev., 124, 2046–2070, 1996. Lindberg, S., Bullock, R., Ebinghaus, R., Engstrom, D., Feng, X., Fitzgerald, W., Pirrone, N., Prestbo, E., and Seigneur, C.: A synthesis of progress and uncertainties in attributing the sources of mercury in deposition, AMBIO: A Journal of the Human Environment, 36, 19–33, 2007. Lohman, K., Seigneur, C., Gustin, M., and Lindeberg, S.: Sensitivity of the global atmospheric cycle of mercury to emissions, Appl. Geochem., 23, 454–466, \doi10.1016/j.apgeochem.2007.12.022, 2008. Lott, F. and Miller, M.: The Representation of Sub-Grid Scale Orography in GCMs, NATO ASI SERIES I, Global Environ. Chang., 50, 275–290, 1997. Lubick, N.: Ocean mercury on the increase, Nature, published online, \doi10.1038/news.2009.218, 2009. Mason, R P.: Mercury emissions from natural sources and their importance in the global mercury cycle, chapter 7, in: Mercury Fate and Transport in the Global Atmosphere: Measurements, Models and Policy Implications; Interim Report of the UNEP Global Partnership on Atmospheric Mercury Transport and Fate Research, 130–144, 2008. Mueller, J.-F. and Brasseur, G.: IMAGES: a three-dimensional chemical transport model of the global troposphere, J. Geophys. Res., 100, 16445–16490, 1995. Munthe, J.: The aqueous oxidation of elemental mercury by ozone, Atmos. Environ., 26A, 1461–1468, 1992. Nordeng, T E.: Extended Versions of the Convective Parametrization Scheme at ECMWF and Their Impact on the Mean and Transient Activity of the Model in the Tropics, European Centre for Medium-Range Weather Forecasts, 1994. Pacyna, E G., Pacyna, J M., Steenhuisen, F., and Wilson, S.: Global anthropogenic mercury emission inventory for 2000, Atmos. Environ., 40, 4048–4063, 2006. Pacyna, J M., Pacyna, E G., and Aas, W.: Changes of emissions and atmospheric deposition of mercury, lead, and cadmium, Atmos. Environ. International, 43, 117–127, 2009. Pai, P., Karamchandani, P., and Seigneur, C.: Simulation of the regional atmospheric transport and fate of mercury using a comprehensive Eulerian model, Atmos. Environ., 31, 2717–2732, 1997. Pal, B. and Ariya, P A.: Studies of ozone initiated reactions of gaseous mercury: kinetics, product studies, and atmospheric implications, Phys. Chem. Chem. Phys., 6, 572–579, 2004. Pehkonen, S O. and Lin, C.-J.: Aqueous photochemistry of mercury with organic acids, JAPCA J. Air Waste Ma. (1995), 48, 144–150, 1998. Peters, J. A. H W. and Olivier, J. G J.: EDGAR3/POET Enussuibs; 1997 emissions and scenarios for 1995–2020; Technical background infromation on global and regional sectoral emissions, RIVM, Bilthoven, report no. 773301003, 2003. Pirrone, N. and Mason, R.: Mercury Fate and Transport in the Global Atmosphere: Measurements, Models and Policy Implications Interim Report of the UNEP Global Partnership on Atmospheric Mercury Transport and Fate Research, 2008. Pirrone, N. and Mason, R. (Eds.): Mercury Fate and Transport in the Global Atmosphere: Emissions, Measurements and Models, Springer, USA, 2009. Pirrone, N., Keeler, G J., and Nriagu, J O.: Regional differences in worldwide emissions of mercury to the atmosphere, Atmos. Environ., 17, 2981–2987, 1996. Pleijel, K. and Munthe, J.: Modelling the Atmospheric Mercury Cycle – Chemistry in Fog Droplets, Atmos. Environ., 29, 1441–1457, 1995. Pongprueksa, P., Lin, C J., Lindberg, S E., Jang, C., Braverman, T., Russell~Bullock, O., Ho, T C., and Chu, H W.: Scientific uncertainties in atmospheric mercury models III: Boundary and initial conditions, model grid resolution, and Hg (II) reduction mechanism, Atmos. Environ., 42, 1828–1845, 2007. Roeckner, E., Baeuml, G., Bonventura, 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. PART I: Model description, Report 349, Max Planck Institute for Meteorology, Hamburg, Germany, 2003. Roeckner, E., Brokopf, R., Esch, M., Giorgetta, M., Hagemann, S., Kornblueh, L., Manzini, E., Schlese, U., and Schulzweida, U.: Sensitivity of Simulated Climate to Horizontal and Vertical Resolution in the ECHAM5 Atmosphere Model, J. Climate, 19, 3771–3791, 2005. Sander, R.: Modeling Atmosheric Chemistry: Interactions between Gas-Phase Species and Liquid Cloud/Aerosol Particles, Survey of Geophysics, 20, 1–31, 1999. Sander, R., Kerkweg, A., Jöckel, P., and Lelieveld, J.: Technical note: The new comprehensive atmospheric chemistry module MECCA, Atmos. Chem. Phys., 5, 445–450, 2005. Sander, S P., Friedl, R R., Golden, D M., Kurylo, M J., Moortgat, G K., Keller-Rudek, H., Wine, P H., Ravishankara, A R., Kolb, C E., Molina, M J., Finlayson-Pitts, B J., Huie, R E., and Orkin, V L.: Chemical kinetics and photochemical data for use in atmospheric studies evaluation number 15, National Aeronautics and Space Administration, Jet Propulsion Laboratory, California Institute of Technology, 2006. 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, 187–195, 2006. Schroeder, W H., Anlauf, K.-G., Barrie, L A., Lu, J Y., Steffen, A., Schneeberger, D R., and Berg, T.: Arctic springtime depletion of mercury, Nature, 394, 331–332, 1998. Schulzweida, U., Kornblueh, L., and Quast, R.: CDO User's Guede, Climate Data Operators, Version 1.0.7, Tech. rep., www.mpimet.mpg.de/fileadmin/software/cdo/, 2007. Schwartz, S E.: Mass-transport considerations pertinent to aqueous phase reactions of gases in liquid-water clouds, in: Chemistry of Multiphase Atmospheric Systems NATO ASI Series G6, edited by: Jaeschle, W., Springer Berlin Heidelberg, Germany, 415–471, 1986. Seigneur, C., Lohman, K., Vijayaraghavan, K., and Shia, R.-L.: Multiscale modeling of the atmospheric fate and transport of mercury, J. Geophys. Res., 106(D21), 27795–27809, 2001. Seigneur, C., Karamchandani, P., Vijayaraghavan, K., Lohman, K., Shia, R L., and Levin, L.: On the effect of spatial resolution on atmospheric mercury modeling, Sci. Total Environ., 304, 73–81, 2003. Seigneur, C., Vijayaraghavan, K., Lohmann, K., Karamchandani, P., and Scott, C.: Global source attribution for mercury deposition in the United States, Environ. Sci. Technol., 38, 555–569, 2004. Seigneur, C., Vijayaraghavan, K., and Lohman, K.: Atmospheric mercury chemistry: Sensitivity of global model simulations to chemical reactions, J. Geophys. Res., 111, D22306, \doi10.1029/2005JD006780, 2006. Seinfeld, C P. and Pandis, S N.: Atmospheric Chemistry and Physics, From Air Pollution to Climate Change, John Wiley and Sons Inc, ISBN 0-4 71-17816-0, 1998. Selin, N E., Jacob, D J., Park, R J., Yantosca, R M., Strode, S., Jaeglé, L., and Jaffe, D.: Chemical cycling and deposition of atmospheric mercury: Global constraints from observations, J. Geophys. Res., 112, D02308, \doi10.1029/2006JD007450, 2007. Sellers, P J., Mintz, Y., Sud, Y C., and Dalcher, A.: A simple biosphere model (SiB) for use within general circulation models, Journal of Atmospheric Sciences, 43, 505–531, 1986. Slemr, F. and Scheel, H E.: Trends in atmospheric mercury concentrations at the summit of the Wank mountain, Southern Germany, Atmos. Environ., 32, 845–853, 1998. Slemr, F., Brunke, E G., Ebinghaus, R., Temme, C., Munthe, J., Wängberg, I., Schroeder, W., Steffen, A., and Berg, T.: Worldwide trend of atmospheric mercury since 1977, Geophys. Res. Lett., 30, 1516, \doi10.1029/2003GL016954, 2003. Slinn, S A. and Slinn, W. G N.: Prediction for particle deposition of natural waters, Atmos. Environ., 14, 1013–1016, 1980. Sommar, J., Hallquist, M., Ljungström, E., and Lindqvist, O.: On the gas phase reactions between volatile biogenic mercury species and the nitrate radical, J. Atmos. Chem., 27, 233–247, 1997. Sommar, J., Gårdfeldt, K., Strömberg, D., and Feng, X.: A kinetic study of the gas-phase reaction between the hydroxyl radical and atomic mercury, Atmos. Environ., 35, 3049–3054, 2001. Sprovieri, F., Pirrone, N., Hedgecock, I M., Landis, M S., and Stevens, R K.: Intensive atmospheric mercury measurements at Terra Nova Bay in Antarctica during November and December 2000, J. Geophys. Res., 107(D23), 4722, \doi10.1029/2002JD002057, 2002. Stohl, A., Eckhardt, S., Forster, C., James, P., and Spichtinger, N.: On the pathways and timescales of intercontinental air pollution transport, J. Geophys. Res, 107(D23), 4684, \doi10.1029/2001JD001396, 2002. Taylor, K E., Williamson, D., and Zwiers, F.: AMIPII Sea Surface Temperature and Sea Ice Concentration Boundary Conditions, 1997. Tiedtke, M.: A Comprehensive Mass Flux Scheme for Cumulus Parameterization in Large-Scale Models, Mon. Weather Rev., 117, 1779–1800, 1989. Tokos, J. J S., Hall, B., Calhoun, J A., and Prestbo, E M.: Homogeneous gas-phase reaction of \chemHg^0 with \chemH_2O_2, \chemO_3, \chemCH_3I, and \chem(CH_3)_2S: Implications for atmospheric Hg cycling, Atmos. Environ. (1994), 32, 823–827, 1998. Tost, H., Jöckel, P., and Lelieveld, J.: Influence of different convection parameterisations in a GCM, Atmos. Chem. Phys., 6, 5475–5493, 2006. Travnikov, O.: Contribution of the intercontinental atmospheric transport to mercury pollution in the Northern Hemisphere, Atmos. Environ., 39, 7541–7548, 2005. Van~Loon, L L., Mader, E A., and Scott, S L.: Sulfite Stabilization and Reduction of the Aqueous Mercuric Ion: Kinetic Determination of Sequential Formation Constants, J. Phys. Chem. A, 105, 3190–3195, 2001. Vijayaraghavan, K., Karamchandani, P., Seigneur, C., Balmori, R., and Chen, S Y.: Plume-in-grid modeling of atmospheric mercury, J. Geophys. Res.-Atmos., 113, D24305, \doi10.1029/2008JD010580, 2008. Wang, Z. and Pehkonen, S O.: Oxidation of elemental mercury by aqueous bromine: atmospheric implications, Atmos. Environ., 38, 3675–3688, 2004. Wesely, M L.: Parameterization of the surface resistances to gaseous dry deposition in regional-scale numerical models, Atmos. Environ., 23, 1293–1304, 1989. Wesely, M L. and Hicks, B B.: Some factors that affect the deposition rates of sulfur dioxide and similar gases on vegetation, Journal of Air Pollution Control Assessment, 27, 1110–1116, 1977. Wesely, M L. and Hicks, B B.: A review of the current status of knowledge on dry deposition, Atmos. Environ., 34, 2261–2282, 2000. Wild, O., Zhu, X., and Prather, M J.: Fast-J: Accurate Simulation of In-and Below-Cloud Photolysis in Tropospheric Chemical Models, J. Atmos. Chem., 37, 245–282, 2000. Yang, X., Cox, R., Warwick, N., Pyle, J., Carver, G., O'Connor, F., and Savage, N.: Tropospheric bromine chemistry and its impacts on ozone: A model study, J. Geophys. Res.-Atmos., 110, D23311, \doi10.1029/2005JD006244, 2005. Zaveri, R A. and Peters, L K.: A new lumped structure photochemical mechanism for large-scale applications, J. Geophys. Res., 104, 30387–30415, 1999.