Geoscientific Model Development Discussions www.geosci-model-dev-discuss.net 1991-9611 1991-962X 3 2 2010 10.5194/gmdd-3-769-2010 http://www.geosci-model-dev-discuss.net/3/769/2010/ http://www.geosci-model-dev-discuss.net/3/769/2010/gmdd-3-769-2010.html http://www.geosci-model-dev-discuss.net/3/769/2010/gmdd-3-769-2010.pdf 769 817 2010-06-01 The Lagrangian chemistry and transport model ATLAS: simulation and validation of stratospheric chemistry and ozone loss in the winter 1999/2000 I. Wohltmann ingo.wohltmann@awi.de R. Lehmann M. Rex Alfred Wegener Institute for Polar and Marine Research, Potsdam, Germany ATLAS is a new global Lagrangian Chemistry and Transport Model (CTM), which includes a stratospheric chemistry scheme with 46 active species, 171 reactions, heterogeneous chemistry on polar stratospheric clouds and a Lagrangian denitrification module. Lagrangian (trajectory-based) models have several important advantages over conventional Eulerian models, including the absence of spurious numerical diffusion, efficient code parallelization and no limitation of the largest time step by the Courant-Friedrichs-Lewy criterion. This work describes and validates the stratospheric chemistry scheme of the model. Stratospheric chemistry is simulated with ATLAS for the Arctic winter 1999/2000, with a focus on polar ozone depletion and denitrification. The simulations are used to validate the chemistry module in comparison with measurements of the SOLVE/THESEO 2000 campaign. A Lagrangian denitrification module, which is based on the simulation of the nucleation, sedimentation and growth of a large number of polar stratospheric cloud particles, is used to model the substantial denitrification that occured in this winter. Andrews,~A E., Boering,~K A., Daube,~B C., Wofsy,~S C., Loewenstein,~M., Jost,~H., Podolske,~J R., Webster,~C R., Herman,~R L., Scott,~D C., Flesch,~G J., Moyer,~E J., Elkins,~J W., Dutton,~G S., Hurst,~D F., Moore,~F L., Ray,~E A., Romashkin,~P A., and Strahan,~S E.: Mean ages of stratospheric air derived from in situ observations of \chemCO_2, \chemCH_4, and \chemN_2O, J. Geophys. Res., 106, 32295–32314, 2001. Boering,~K A., Daube,~B C., Wofsy,~S C., Loewenstein,~M., Podolske,~J R., and Keim,~E R.: Tracer-tracer relationships and lower stratospheric dynamics: \chemCO_2 and \chemN_2O during SPADE, Geophys. Res. Lett., 21, 2567–2570, 1994. Burkholder,~J B., Orlando,~J J., and Howard,~C J.: Ultraviolet absorption cross sections of chlorine oxide (\chemCl_2O_2) between 210 and 410 nm, J. Phys. Chem.-US, 94, 687–695, 1990. Carslaw,~K S., Luo,~B., and Peter,~T.: An analytical expression for the composition of aqueous \chemHNO_3-\chemH_2SO_4 stratospheric aerosols including gas phase removal of \chemHNO_3, Geophys. Res. Lett., 22, 1877–1880, 1995. Carslaw,~K S., Kettleborough,~J A., Northway,~M J., Davies,~S., Gao,~R.-S., Fahey,~D W., Baumgardner,~D G., Chipperfield,~M P., and Kleinböhl,~A.: A~vortex-scale simulation of the growth and sedimentation of large nitric acid hydrate particles, J. Geophys. Res., 107, 8300, \doi10.1029/2001JD000467, 2002. Chipperfield,~M P., Feng,~W., and Rex,~M.: Arctic ozone loss and climate sensitvity: updated three-dimensional model study, Geophys. Res. Lett., 32, 11813, \doi10.1029/2005GL022674, 2005. Collins,~W J., Stevenson,~D S., Johnson,~C E., and Derwent,~R G.: Tropospheric ozone in a~global-scale three-dimensional Lagrangian model and its response to NO_x emission controls, J. Atmos. Chem., 26, 223–274, 1997. Dhaniyala,~S., Flagan,~R C., McKinney,~K A., and Wennberg,~P O.: Novel aerosol/gas inlet for aircraft-based measurements, Aerosol Sci. Tech., 37, 828–840, 2003. Dorf, M., Butz, A., Camy-Peyret, C., Chipperfield, M. P., Kritten, L., and Pfeilsticker, K.: Bromine in the tropical troposphere and stratosphere as derived from balloon-borne BrO observations, Atmos. Chem. Phys., 8, 7265–7271, \doi10.5194/acp-8-7265-2008, 2008. Eyring,~V., Chipperfield,~M., Giorgetta,~M A., Kinnison,~D E., Manzini,~E., Matthes,~K., Newman,~P A., Pawson,~S., Shepherd,~T G., and Waugh,~D W.: Overview of the new CCMVal reference and sensitivity simulations in support of upcoming ozone and climate assessments and the planned SPARC CCMVal report, SPARC News Lett., 30, 20–26, 2008. Fahey,~D W., Kelly,~K K., Ferry,~G V., Poole,~L R., Wilson,~J C., Murphy,~D M., Loewenstein,~M., and Chan,~K R.: In situ measurements of total reactive nitrogen, total water and aerosol in a~polar stratospheric cloud in the Antarctic, J. Geophys. Res., 94, 11299–11315, 1989. Fahey,~D W., Gao,~R S., Carslaw,~K S., Kettleborough,~J., Popp,~P J., Northway,~M J., Holecek,~J C., Ciciora,~S C., McLaughlin,~R J., Thompson,~T L., Winkler,~R H., Baumgardner,~D G., Gandrud,~B., Wennberg,~P O., Dhaniyala,~S., McKinney,~K., Peter,~T., Salawitch,~R J., Bui,~T P., Elkins,~J W., Webster,~C R., Atlas,~E L., Jost,~H., Wilson,~J C., Herman,~R L., Kleinböhl,~A., and von König,~M.: The detection of large \chemHNO_3-containing particles in the winter Arctic stratosphere, Science, 291, 1026–1031, 2001. Grooß, J.-U. and Russell III, James M.: Technical note: A stratospheric climatology for \chemO_3, \chemH_2O, \chemCH_4, NO_x, \chemHCl and \chemHF derived from HALOE measurements, Atmos. Chem. Phys., 5, 2797–2807, \doi10.5194/acp-5-2797-2005, 2005. Grooß,~J.-U., Günther,~G., Konopka,~P., Müller,~R., McKenna,~D S., Stroh,~F., Vogel,~B., Engel,~A., Müller,~M., Hoppel,~K., Bevilacqua,~R., Richard,~E., Webster,~C R., Elkins,~J W., Hurst,~D F., Romashkin,~P A., and Baumgardner,~D G.: Simulation of ozone depletion in spring 2000 with the Chemical Lagrangian Model of the Stratosphere (CLaMS), J. Geophys. Res., 107, 8295, \doi10.1029/2001JD000456, 2002. Grooß, J.-U., Günther, G., Müller, R., Konopka, P., Bausch, S., Schlager, H., Voigt, C., Volk, C.M., and Toon, G. C.: Simulation of denitrification and ozone loss for the Arctic winter 2002/2003, Atmos. Chem. Phys., 5, 1437–1448, \doi10.5194/acp-5-1437-2005, 2005. Hanisco,~T F., Smith,~J B., Stimpfle,~R M., Wilmouth,~D M., Anderson,~J G., Richard,~E C., and Bui,~T P.: In situ observations of \chemHO_2 and \chemOH obtained on the NASA ER-2 in the high-ClO conditions of the 1999/2000 Arctic polar vortex, J. Geophys. Res., 107, 8283, \doi10.1029/2001JD001024, 2002. Hanson,~D. and Mauersberger,~K.: Laboratory studies of the nitric acid trihydrate: Implications for the south polar stratosphere, Geophys. Res. Lett., 15, 855–858, 1988. Herman,~R L., Drdla,~K., Spackman,~J R., Hurst,~D F., Popp,~P J., Webster,~C R., Rosmashkin,~P A., Elkins,~J W., Weinstock,~E M., Gandrud,~B W., Toon,~G C., Schoeberl,~M R., Jost,~H., Atlas,~E L., and Bui,~T P.: Hydration, dehydration, and the total hydrogen budget of the 1999/2000 winter Arctic stratosphere, J. Geophys. Res., 107, 8320, \doi10.1029/2001JD001257, 2002. IPCC: Climate Change 2001: The scientific basis. Contribution of working group I to the third assessment report of the Intergovernmental Panel on Climate Change, Cambridge University Press, Cambridge, UK and New York, NY, USA, 2001. Jones,~A., Walker,~K A., Jin,~J., Taylor,~J R., Boone,~C D., Bernath,~P F., Manney,~G L., McLeod,~S., and Hughes,~R.: A~description of the ACE-FTS global climatological datasets, in preparation, 2010. Konopka,~P., Steinhorst,~H.-M., Grooß,~J.-U., Günther,~G., Müller,~R., Elkins,~J W., Jost,~H.-J., Richard,~E., Schmidt,~U., Toon,~G., and McKenna,~D S.: Mixing and ozone loss in the 1999–2000 Arctic vortex: simulations with the three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS), J. Geophys. Res., 109, D02315, \doi10.1029/2003JD003792, 2004. Konopka, P., Günther, G., Müller, R., dos Santos, F. H. S., Schiller, C., Ravegnani, F., Ulanovsky, A., Schlager, H., Volk, C. M., Viciani, S., Pan, L. L., McKenna, D.-S., and Riese, M.: Contribution of mixing to upward transport across the tropical tropopause layer (TTL), Atmos. Chem. Phys., 7, 3285–3308, \doi10.5194/acp-7-3285-2007, 2007. Krämer,~M., Müller,~R., Bovensmann,~H., Burrows,~J., Brinkmann,~J., Röth,~E P., Grooß,~J.-U., Müller,~R., Woyke,~T., Ruhnke,~R., Günther,~G., Hendricks,~J., Lippert,~E., Carslaw,~K S., Peter,~T., Zieger,~A., Brühl,~C., Steil,~B., Lehmann,~R., and McKenna,~D S.: Intercomparison of stratospheric chemistry models under polar vortex conditions, J. Atmos. Chem., 45, 51–77, 2003. Laube, J. C., Engel, A., Bönisch, H., Möbius, T., Sturges, W. T., Braß, M., and Röckmann, T.: Fractional release factors of long-lived halogenated organic compounds in the tropical stratosphere, Atmos. Chem. Phys., 10, 1093–1103, \doi10.5194/acp-10-1093-2010, 2010. Loewenstein,~M., Jost,~H., Grose,~J., Eilers,~J., Lynch,~D., Jensen,~S., and Marmie,~J.: Argus: a~new instrument for the measurement of the stratospheric dynamical tracers, \chemN_2O and \chemCH_4, Spectrochim. Acta A, 58, 2329–2345, 2002. Madronich,~S. and Flocke,~S.: The role of solar radiation in atmospheric chemistry, in: Handbook of Environmental Chemistry, edited by: Boule,~P., Springer-Verlag, Heidelberg, 1–26, 1999. Mann, G.W., Davies, S., Carslaw, K. S., and Chipperfield, M. P.: Factors controlling Arctic denitrification in cold winters of the 1990s, Atmos. Chem. Phys., 3, 403–416, \doi10.5194/acp-3-403-2003, 2003. Marti,~J. and Mauersberger,~K.: A~survey and new measurements of ice vapor pressure at temperatures between 170 and 250 K, Geophys. Res. Lett., 20, 363–366, 1993. May,~R D.: Open-path, near-infrared tunable diode laser spectrometer for atmospheric measurements of \chemH_2O, J. Geophys. Res., 103, 19161–19172, 1998. McKenna,~D S., Grooß,~J.-U., Günther,~G., Konopka,~P., and Müller,~R.: A~new Chemical Lagrangian Model of the Stratosphere (CLaMS) 2. Formulation of chemistry scheme and initialization, J. Geophys. Res., 107, 4256, \doi10.1029/2000JD000113, 2002. McKinney,~K A., Wennberg,~P O., Dhaniyala,~S., Fahey,~D W., Northway,~M J., Künzi,~K F., Kleinböhl,~A., Sinnhuber,~M., Küllmann,~H., Bremer,~H., Mahoney,~M J., and Bui,~T P.: Trajectory studies of large \chemHNO_3-containing PSC particles in the Arctic: evidence for the role of NAT, Geophys. Res. Lett., 31, L05110, \doi10.1029/2003GL018430, 2004. Nash,~E R., Newman,~P A., Rosenfield,~J E., and Schoeberl,~M R.: An objective determination of the polar vortex using Ertel's potential vorticity, J. Geophys. Res., 101, 9471–9478, 1996. Newman,~P., Harris,~N R P., Adriani,~A., Amanatidis,~G T., Anderson,~J G., Braathen,~G O., Brune,~W H., Carslaw,~K S., Craig,~M S., DeCola,~P L., Guirlet,~M., Hipskind,~R S., Kurylo,~M J., Küllmann,~H., Larsen,~N., Mégie,~G J., Pommereau,~\hboxJ.-P., Poole,~L R., Schoeberl,~M R., Stroh,~F., Toon,~O B., Trepte,~C R., and Roozendael,~M V.: An overview of the SOLVE-THESEO 2000 campaign, J. Geophys. Res., 107, 8259, \doi10.1029/2001JD001303, 2002. Popp,~P J., Northway,~M J., Holecek,~J C., Gao,~R S., Fahey,~D W., Elkins,~J W., Hurst,~D F., Romashkin,~P A., Toon,~G C., Sen,~B., Schauffler,~S M., Salawitch,~R J., Webster,~C R., Herman,~R L., Jost,~H., Bui,~T P., Newman,~P A., and Lait,~L R.: Severe and extensive denitrification in the 1999–2000 Arctic winter stratosphere, Geophys. Res. Lett., 28, 2875–2878, 2001. Proffitt,~M H. and McLaughlin,~R J.: Fast-response dual-beam UV-absorption ozone photometer suitable for use on stratospheric balloons, Rev. Sci. Instrum., 54, 1719–1728, 1983. Ray,~E A., Moore,~F L., Elkins,~J W., Hurst,~D F., Romashkin,~P A., Dutton,~G S., and Fahey,~D W.: Descent and mixing in the 1999–2000 northern polar vortex inferred from in situ tracer measurements, J. Geophys. Res., 107, 8285, \doi10.1029/2001JD000961, 2002. Reithmeier,~C. and Sausen,~R.: ATTILA: atmospheric tracer transport in a~Lagrangian model, Tellus~B, 54, 278–299, 2002. Rex,~M., Salawitch,~R J., Harris,~N R P., von~der Gathen,~P., Braathen,~G O., Schulz,~A., Deckelmann,~H., Chipperfield,~M., Sinnhuber,~B.-M., Reimer,~E., Alfier,~R., Bevilacqua,~R., Hoppel,~K., Fromm,~M., Lumpe,~J., Küllmann,~H., Kleinböhl,~A., Bremer,~H., von König,~M., Künzi,~K., Toohey,~D., Vömel,~H., Richard,~E., Aikin,~K., Jost,~H., Greenblatt,~J B., Loewenstein,~M., Podolske,~J R., Webster,~C R., Flesch,~G J., Scott,~D C., Herman,~R L., Elkins,~J W., Ray,~E A., Moore,~F L., Hurst,~D F., Romashkin,~P., Toon,~G C., Sen,~B., Margitan,~J J., Wennberg,~P., Neuber,~R., Allart,~M., Bojkov,~B R., Claude,~H., Davies,~J., de~Backer,~H., Dier,~H., Dorokhov,~V., Fast,~H., Kondo,~Y., Kyrö,~E., Litynska,~Z., Mikkelsen,~I S., Molyneux,~M J., Moran,~E., Nagai,~T., Nakane,~H., Parrondo,~C., Ravegnani,~F., Skrivankova,~P., Viatte,~P., and Yushkov,~V.: Chemical depletion of Arctic ozone in winter 1999/2000, J. Geophys. Res., 107, 8276, \doi10.1029/2001JD000533, 2002. Richard,~E C., Aikin,~K C., Andrews,~A E., Daube, Jr.,~B C., Gerbig,~C., Wofsy,~S C., Romashkin,~P A., Hurst,~D F., Ray,~E A., Moore,~F L., Elkins,~J W., Deshler,~T., and Toon,~G C.: Severe chemical ozone loss inside the Arctic polar vortex during winter 1999–2000 inferred from in situ airborne measurements, Geophys. Res. Lett., 28, 2197–2200, 2001. Romashkin,~P A., Hurst,~D F., Elkins,~J W., Dutton,~G S., Fahey,~D W., Dunn,~R E., Moore,~F L., Myers,~R C., and Hall,~B D.: In situ measurements of long-lived trace gases in the lower stratosphere by gas chromatography, J. Atmos. Oceanic Technol., 18, 1195–1204, 2001. Sander,~S P., Friedl,~R R., Ravishankara,~A R., Golden,~D M., Kolb,~C E., Kurylo,~M J., Molina,~M J., Moortgat,~G K., Finlayson-Pitts,~B J., Wine,~P H., Huie,~R E., and Orkin,~V L.: Chemical kinetics and photochemical data for use in atmospheric studies, Evaluation Number 15, JPL Publication 06-2, Jet Propulsion Laboratory, California Institute of Technology, Pasadena, available at: http://jpldataeval.jpl.nasa.gov (last access: May~2010), 2006. Sander,~S P., Friedl,~R R., Abatt,~J., Barker,~J R., Burkholder,~J B., Golden,~D M., Kolb,~C E., Kurylo,~M J., Moortgat,~G K., Wine,~P H., Huie,~R E., and Orkin,~V L.: Chemical kinetics and photochemical data for use in atmospheric studies, Evaluation Number 16, JPL Publication 09-31, Jet Propulsion Laboratory, California Institute of Technology, Pasadena, available at: http://jpldataeval.jpl.nasa.gov (last access: May~2010), 2009. 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, \doi10.5194/acp-6-187-2006, 2006. Shampine,~L F. and Reichelt,~M W.: The MATLAB ODE Suite, SIAM J. Sci. Comput., 18, 1–22, 1997. Simmons,~A J., Uppala,~S M., Dee,~D., and Kobayashi,~S.: ERA-Interim: new ECMWF reanalysis products from 1989 onwards, ECMWF News Lett., 110, 25–35, 2006. Simmons,~A J., Uppala,~S M., and Dee,~D.: Update on ERA-Interim, ECMWF News Lett., 111, 5, 2007. Stachnik,~R A., Hardy,~J C., Tarsala,~J A., and Waters,~J W.: Submillimeterwave heterodyne measurements of stratospheric \chemClO, \chemHCl, \chemO_3 and \chemHO_2: first results, Geophys. Res. Lett., 19, 1931–1934, 1992. Stimpfle,~R M., Cohen,~R C., Bonne,~G P., Voss,~P B., Perkins,~K K., Koch,~L C., Anderson,~J G., Salawitch,~R J., Lloyd,~S A., Gao,~R S., DelNegro,~L A., Keim,~E R., and Bui,~T P.: The coupling of \chemClONO_2, ClO, and \chemNO_2 in the lower stratosphere from in situ observations using the NASA ER-2 aircraft, J. Geophys. Res., 104, 26705–26714, 1999. Stimpfle,~R M., Wilmouth,~D M., Salawitch,~R J., and Anderson,~J G.: First measurements of ClOOCl in the stratosphere: the coupling of ClOOCl and ClO in the Arctic polar vortex, J. Geophys. Res., 109, D03301, \doi10.1029/2003JD003811, 2004. Thompson,~A M., Witte,~J C., McPeters,~R D., Oltmans,~S J., Schmidlin,~F J., Logan,~J A., Fujiwara,~M., Kirchhoff,~V W J H., Posny,~F., Coetzee,~G J R., Hoegger,~B., Kawakami,~S., Ogawa,~T., Johnson,~B., Vömel,~H., and Labow,~G.: Southern Hemisphere Additional Ozonesondes (SHADOZ) 1998–2000 tropical ozone climatology 1. Comparison with Total Ozone Mapping Spectrometer (TOMS) and ground-based measurements, J. Geophys. Res., 108, 8238, \doi10.1029/2001JD000967, 2003. Toon,~G C.: The JPL MklV interferometer, Opt. Photonics News, 2, 19–21, 1991. Tripathi,~O P., Godin-Beekmann,~S., Lefèvre,~F., Marchand,~M., Pazmiño,~A., Hauchecorne,~A., Goutail,~F., Schlager,~H., Volk,~C M., Johnson,~B., König-Langlo,~G., Balestri,~S., Stroh,~F., Bui,~T P., Jost,~H J., Deshler,~T., and von~der Gathen,~P.: High resolution simulation of recent Arctic and Antarctic stratospheric chemical ozone loss compared to observations, J. Atmos. Chem., 55, 205–226, \doi10.1007/s10874-006-9028-8, 2006. Webster,~C R., May,~R D., Trimble,~C A., Chave,~R G., and Kendall,~J.: Aircraft (ER-2) laser infrared absorption spectrometer (ALIAS) for in-situ stratospheric measurements of HCI, \chemN_2O, \chemCH_4, \chemNO_2, and \chemHNO_3, Appl. Optics, 33, 454–472, 1994. Weinstock,~E M., Hintsa,~E J., Dessler,~A E., Oliver,~J F., Hazen,~N L., Demusz,~J N., Allen,~N T., Lapson,~L B., and Anderson,~J G.: New fast response photofragment fluorescence hygrometer for use on the NASA ER-2 and the Perseus remotely piloted aircraft, Rev. Sci. Instrum., 65, 3544–3554, 1994. White,~F M.: Viscous Fluid Flow, McGraw-Hill, New York, 1991. WMO: World Meteorological Organization (WMO)/United Nations Environment Programme (UNEP), Scientific assessment of ozone depletion: 2006, Global Ozone Research and Monitoring Project – Report No. 50, 2007. Wofsy,~S C., Gobbi,~G P., Salawitch,~R J., and McElroy,~M B.: Nucleation and growth of \chemHNO_3·3\chemH_2O particles in the polar stratosphere, J. Atmos. Sci., 47, 2004–2012, 1990. Wohltmann, I. and Rex, M.: The Lagrangian chemistry and transport model ATLAS: validation of advective transport and mixing, Geosci. Model Dev., 2, 153–173, \doi10.5194/gmd-2-153-2009, 2009. Woodbridge,~E L., Elkins,~J W., Fahey,~D W., Heidt,~L E., Solomon,~S., Baring,~T J., Gilpin,~T M., Pollock,~W H., Schauffler,~S M., Atlas,~E L., Loewenstein,~M., Podolske,~J R., Webster,~C R., May,~R D., Gilligan,~J M., Montzka,~S A., Boering,~K A., and Salawitch,~R J.: Estimates of total organic and inorganic chlorine in the lower stratosphere from in situ and flask measurements during AASE II, J. Geophys. Res., 100, 3057–3064, 1995.