References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-7-1755-2007

A 3D-CTM with detailed online PSC-microphysics: analysis of the Antarctic winter 2003 by comparison with satellite observations

Daerden

¹ Larsen

² Chabrillat

¹ Errera

¹ Bonjean

¹ Fonteyn

³ Hoppel

⁴ Fromm

⁴

Belgian Institute for Space Aeronomy BIRA-IASB, Brussels, Belgium

Danish Meteorological Institute, Copenhagen, Denmark

Belgian Federal Science Policy, Brussels, Belgium

Naval Research Laboratory, Washington D.C., USA

10 04 2007

7 7 1755 1772

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/7/1755/2007/acp-7-1755-2007.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/7/1755/2007/acp-7-1755-2007.pdf

We present the first detailed microphysical simulations which are performed online within the framework of a global 3-D chemical transport model (CTM) with full chemistry. The model describes the formation and evolution of four types of polar stratospheric cloud (PSC) particles. Aerosol freezing and other relevant microphysical processes are treated in a full explicit way. Each particle type is described by a binned size distribution for the number density and chemical composition. This set-up allows for an accurate treatment of sedimentation and for detailed calculation of surface area densities and optical properties. Simulations are presented for the Antarctic winter of 2003 and comparisons are made to a diverse set of satellite observations (optical and chemical measurements of POAM III and MIPAS) to illustrate the capabilities of the model. This study shows that a combined resolution approach where microphysical processes are simulated in coarse-grained conditions gives good results for PSC formation and its large-scale effect on the chemical environment through processes such as denitrification, dehydration and ozone loss.

References 1

Benson, C. M., Drdla, K., Nedoluha, G. E., Shettle, E. P., Hoppel, K. W., and Bevilacqua, R. M.: Microphysical modeling of southern polar dehydration during the 1998 winter and comparison with POAM III observations, J. Geophys. Res., 111, D07201, doi:10.1029/2005JD006506, 2006.

Carslaw, K. S., Kettleborough, J., Northway, M. J., Davies, S., Gao, R.-S., Fahey, D. W., Baumgardner, D. G., Chipperfield, M. P., and Kleinbohl, A.: A Vortex-Scale Simulation of the Growth and Sedimentation of Large Nitric Acid Hydrate Particles, J. Geophys. Res., 107, 8300, doi:10.1029/2001JD000467, 2002.

Chipperfield, M P.: Multiannual Simulations with a Three-Dimensional Chemical Transport Model, J. Geophys. Res., 104, 1781–1805, 1999.

Damian, V., Sandu, A., Damian, M., Potra, F., and Carmichael, G.: The Kinetic PreProcessor KPP – A Software Environment for Solving Chemical Kinetics, Computers and Chemical Engineering, 26, 1567–1579, 2002.

Davies, S., Mann, G. W., Carslaw, K. S., Chipperfield, M. P., Remedios, J. J., Allen, G., Waterfall, A. M., Spang, R., and Toon, G. C.: Testing our understanding of Arctic denitrification using MIPAS-E satellite measurements in winter 2002/3, Atmos. Chem. Phys., 6, 3149–3161, 2006.

Dessler, A. E.: The chemistry and physics of stratospheric ozone, Academic Press, London, San Diego, 214 pp, 2000.

Deshler, T., Hervig, M. E., Hofmann, D. J., Rosen, J. M., and Liley, J. B.: Thirty years of in situ stratospheric aerosol size distribution measurements from Laramie, Wyoming (41\dg N), using balloon-borne instruments, J. Geophys. Res., 108(D5), 4167, doi:10.1029/2002JD002514, 2003.

Drdla, K.: Applications of a Model of Polar Stratospheric Clouds and Heterogeneous Chemistry, Ph.D. thesis, Univ. of California, Los Angeles, Los Angeles, 1996.

Drdla, K., Schoeberl, M. R., and Browell, E. V.: Microphysical modeling of the 1999–2000 Arctic winter, 1, Polar stratospheric clouds, denitrification, and dehydration, J. Geophys. Res., 107, 8312, doi:10.1029/2001JD000782, 2003.

Errera, Q. and Fonteyn, D.: Four-dimensional variational chemical assimilation of CRISTA stratospheric measurements, J. Geophys. Res., 106, 12 253–12 265, 2001.

European Space Agency (2000): Envisat: MIPAS, An instrument for atmospheric chemistry and climate research, ESA SP-1229, Noordwijk, Netherlands, 2000.

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, Th., 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 HNO3-containing particles in the winter Arctic stratosphere, Science, 291, 1026–1031, 2001.

Fischer, H. and Oelhaf, H.: Remote sensing of vertical profiles of atmospheric trace constituents with MIPAS limb emission spectrometers, Appl. Opt., 35(16), 2787–2796, 1996.

Foelsche, U., Borsche, M., Steiner, A. K., Pirscher, B., Lackner, B. C., Gobiet, A., and Kirchengast, G.: CHAMP Radio Occultation Based Climatologies for Global Monitoring of Climate Change, WegCenter Rep. for FFG-ALR No. 3/2006, 52p., Wegener Center, Univ. of Graz, Austria, http://www.uni-graz.at/igam-arsclisys/ – Publications, 2006.

Fonteyn,~D. and~Larsen, N.: Detailed PSC formation in a two-dimensional chemical transport model of the stratosphere, Ann. Geophys., 14, 315–328, 1996.

Fonteyn,~D.,~Bonjean, S.,~Chabrillat, S.,~Daerden, F., and~Errera, Q.: 4D-VAR chemical data assimilation of ENVISAT chemical products (BASCOE): validation support issues, in: Proceedings of the "ENVISAT validation workshop" held at ESRIN, Frascati, Italy, 9–13 December 2002.

Fonteyn, D., Lahoz, W., Geer, A., Dethof, A., Wargan, K., Stajner, L., Pawson, S., Rood, R. B., Bonjean, S., Chabrillat, S., Daerden, F., and Errera, Q.: MIPAS Ozone Assimilation, Proceedings of the Second Workshop on the Atmospheric Chemistry Validation of ENVISAT (ACVE-2), 3-7 May 2004, ESA-ESRIN, Frascati, Italy (ESA SP-562), edited by: Danesy, D., p. 19.1–19.6, published on CDROM, 2004.

Fromm,~M., Bevilacqua, R. M., Hornstein, J., Shettle, E., Hoppel, K., and Lumpe, J. D.: An analysis of Polar Ozone and Aerosol Measurement (POAM) II Arctic polar stratospheric cloud observations, 1993–1996, J. Geophys. Res., 104(D20), 24 341–24 357, 1999.

Fromm,~M.,~Alfred, J., and~Pitts, M.: A unified, long-term, high-latitude stratospheric aerosol and cloud database using SAM II, SAGE II, and POAM II/III data: Algorithm description, database definition, and climatology, J. Geophys. Res., 108(D12), 4366, doi:10.1029/2002JD002772, 2003.

Fuchs, N. A.: The mechanics of aerosols, Pergamon Press, New York, 408 pp, 1964.

Funke, B., Lopez-Puertas, M., Gil-Lopez, S., von Clarmann, T., Stiller, G. P., Fischer, H., and Kellmann, S.: Downward transport of upper atmospheric NOx into the polar stratosphere and lower mesosphere during the Antarctic winter 2003 and Arctic winter 2002/2003, J. Geophys. Res., 110, D24308, doi:10.1029/2005JD006463, 2005.

Gobiet, A., Foelsche, U., Steiner, A. K., Borsche, M., Kirchengast, G., and Wickert, J.: Climatological validation of stratospheric temperatures in ECMWF operational analyses with CHAMP radio occultation data, Geophys. Res. Lett., 32, L12806, doi:10.1029/2005GL022617, 2005.

Grooß, J.-U., Günther, G., Konopka, P., Müller, R., McKenna, D. S., Stroh, F., Vogel, B., Engel, A., Müller, M., Hoppel, K., Beviacqua, 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(D20), 8295, 10.1029/2001JD000456, 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, 2005.

Hairer, E. and Wanner, G.: Solving Ordinary Differential Equations II. Stiff and differential-algebraic problems, vol 14 of Springer series in computational mathematics, Springer, 2 edn., 1996.

Harries, J. E., Russell, J. M., Tuck, A. F., Gordley, L. L., Purcell, P., Stone, K., Bevilacqua, R. M., Gunson, M., Nedoluha, G., and Traub, W. A.: Validation of measurements of water vapor from the halogen occultation experiment (HALOE), J. Geophys. Res., 101(D6), 10 205–10 216, 1996.

Höpfner, M., Larsen, N., Spang, R., Luo, B. P., Ma, J., Svendsen, S. H., Eckermann, S. D., Knudsen, B., Massoli, P., Cairo, F., Stiller, G., v. Clarmann, T., and Fischer, H.: MIPAS detects Antarctic stratospheric belt of NAT PSCs caused by mountain waves, Atmos. Chem. Phys., 6, 1221–1230, 2006a.

Höpfner, M., Luo, B. P., Massoli, P., Cairo, F., Spang, R., Snels, M., Di Donfrancesco, G., Stiller, G., von Clarmann, T., Fischer, H., and Biermann, U.: Spectroscopic evidence for NAT, STS, and ice in MIPAS infrared limb emission measurements of polar stratospheric clouds, Atmos. Chem. Phys., 6, 1201–1219, 2006b.

Hoppel, K., Bevilacqua, R., Canty, T., Salawitch, R., and Santee, M.: A measurement/model comparison of ozone photochemical loss in the Antarctic ozone hole using POAM observations and the Match technique, J. Geophys. Res., 110, D19304, doi:10.1029/2004JD005651, 2005.

Kawa, S. R., Fahey, D. W., Heidt, L. E., Pollock, W. H., Solomon, S., Anderson, D. E., Loewenstein, M., Proffitt, M. H., Margitan, J. J., and Chan, K. R.: Photochemical partitioning of the reactive nitrogen and chlorine reservoirs in the high-latitude stratosphere, J. Geophys. Res., 97, 7905–7923, 1992.

Kley, D., Russell III, J. M., and Phillips, C. (Eds.): SPARC Assessment of Upper Tropospheric and Stratospheric Water Vapour, WCRP 113, WMO/TD-1043, SPARC Rep. 2, World Clim. Res. Program, Geneva, 2000.

Knopf, D. A., Koop, T., Luo, B. P., et al.: Homogeneous nucleation of NAD and NAT in liquid stratospheric aerosols: insufficient to explain denitrification, Atmos. Chem. Phys., 2, 207–214, 2002.

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 3-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS), J. Geophys. Res., 109(D2), doi:10.1029/2003JD003792, 2004.

Koop, T. and Carslaw, K.: Melting of H2SO4.4H2O particles upon cooling: implications for polar stratopsheric clouds, Science, 272, 1638–1641, 1996.

Koop, T., Luo, B., Tsias, A., and Peter, T.: Water activity as the determinant for homogeneous ice nucleation is aqueous solutions, Nature, 406, 611–614, 2000.

Krieger, U. K., Mössinger, J. C., Luo, B., Weers, U., and Peter, T.: Measurements of the refractive indices of H2SO4-HNO3-H2O solutions to stratospheric temperatures, Appl. Opt., 21, 3691–3703, 2000.

Larsen,~N.: Polar Stratospheric Clouds. Microphysical and optical models, Scientific report 00-06, Danish Meteorological Institute, http://dmiweb.dmi.dk/pub/PSC/, 2000.

Larsen,~N., Svendsen,~S H., Knudsen,~B M., Voigt,~C., Weisser,~C., Kohlmann, ~A., Schreiner,~J., Mauersberger,~J., Deshler,~T., Kröger,~C., Rosen,~J., Kjome,~N., Adriani,~A., Cairo,~F., Di~Donfrancesco,~G., Ovarlez,~J., Ovarlez, ~H., Dörnback,~A., and Birner,~T.: Microphysical mesoscale simulations of polar stratospheric cloud formation constrained by in situ measurements of chemical and optical cloud properties, J. Geophys. Res., 107(D20), 8301, doi:10.1029/2001JD000999, 2002.

Larsen, N., Knudsen, B M., Svendsen, S H., Deshler, T., Rosen, J M., Kivi, R., Weisser, C., Schreiner, J., Mauerberger, K., Cairo, F., Ovarlez, J., Oelhaf, H., and Spang, R.: Formation of solid particles in synoptic-scale Arctic PSCs in early winter 2002/2003, Atmos. Chem. Phys., 4, 2001–2013, 2004.

Lin, S.-J. and Rood, R B.: Multi-dimensional Flux-Form Semi-Lagrangian transport schemes, Mon. Wea. Rev., 124(9), 2046–2070, 1996.

Lucke, R. L., Korwan, D. R., Bevilacqua, R. M., Hornstein, J. S., Shettle, E. P., Chen, D. T., Daehler, M., Lumpe, J. D., Fromm, M. D., Debrestian, D., Neff, B., Squire, M., König-Langlo, G., and Davies, J.: The Polar Ozone and Aerosol Measurement (POAM) III instrument and early validation results, J. Geophys. Res., 104(D15), 18 785–18 800, doi:10.1029/1999JD900235, 1999.

Lumpe, J. D., Bevilacqua, R. M., Hoppel, K. W., and Randall, C. E.: POAM III retrieval algorithm and error analysis, J. Geophys. Res., 107(D21), 4575, doi:10.1029/2002JD002137, 2002.

Lumpe, J., Bevilacqua, R., Randall, C., Nedoluha, G., Hoppel, K., Russell, J., Harvey, V. L., Schiller, C., Sen, B., Taha, G., Toon, G., and Vömel, H.: Validation of Polar Ozone and Aerosol Measurement (POAM) III version 4 stratospheric water vapor, J. Geophys. Res., 111(D11), D11301, doi:10.1029/2005JD006763, 2006.

Mann, G. W., Davies, D. S., Carslaw, K. S., Chipperfield, M. P.: Factors controlling Arctic denitrification in cold winters of the 1990s, Atmos. Chem. Phys., 3, 403–416, 2003.

Manney, G. L., Allen, D. R., Krüger, K., Naujokat, B., Santee, M. L., Sabutis, J. L., Pawson, S., Swinbank, R., Randall, C. E., Simmons, A. J., and Long, C.: Diagnostic Comparison of Meteorological Analyses during the 2002 Antarctic Winter, Mon. Wea. Rev., 133, 1261–1278, 2005.

Michelsen, H. A., Manney, G. L., Gunson, M. R., Rinsland, C. P., and Zander, R.: Correlations of stratospheric abundances of CH4 and N2O derived from ATMOS measurements, Geophys. Res. Lett., 25, 2777–2780, 1998.

Mishchenko, M. I. and Travis, L.: Capabilities and limitations of a current Fortran implementation of the T-matrix method for randomly oriented, rotationally symmetric scatterers, J. Quant. Spectrosc. Radiat. Trans., 60, 309–324, 1998.

Müller, R. and Peter, Th.: The numerical modelling of the sedimentation of Polar Stratospheric Cloud particles, Ber. Bunsenges. Phys. Chem., 96, 353–361, 1992.

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.

Oelhaf, H., Fix, A., Schiller, C., Chance, K., Ovarlez, W., Gurlit J., Renard, J.-B., Rohs, S., Wetzel, G., von Clarmann, T., Milz, M., Wang, D.-Y., Remedios, J. J., and Waterfall, A. M.: Validation of MIPAS-ENVISAT Version 4.61 Operational Data with Balloon and Aircraft Measurements: H2O, Proceedings of the Second Workshop on the Atmospheric Chemistry Validation of ENVISAT (ACVE-2), 3-7 May 2004, ESA-ESRIN, Frascati, Italy (ESA SP-562), edited by: Danesy, D., p. 24.1–24.8, published on CDROM, 2004.

Pinnick, R. G., Rosen, J. M., and Hofmann, D. J.: Stratospheric aerosol measurements III: optical model calculations, J. Atmos. Sci., 33, 304–314, 1976.

Pruppacher, H. R. and Klett, J. D., Microphysics of clouds and precipitation, 2nd ed., Kluwer Academic Publishers, Dordrecht, Boston, London, 954 pp, 1997.

Rotman, D. A., Tannahill, J. R., Kinnison, D. E., Connell, P. S., Bergmann, D., Proctor, D., Rodriguez, J. M., Lin, S. J., Rood, R. B., Prather, M. J., Rasch, P. J., Considine, D. B., Ramaroson, R., and Kawa, S. R.: Global Modeling Initiative assessment model: Model description, integration, and testing of the transport shell, J. Geophys. Res., 106, 1669–1691, 2001.

Sander, S P., Friedl, R R., Golden, D M., Kurylo, M J., Huie, R E., Orkin, V L., Moortgaat, G K., Ravishankara, A R., Kolb, C E., and Molina, M J.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies, Evaluation Number 14, Publication 00–3, JPL, 2003.

Sankey, D. and Shepherd, T. G.: Correlations of long-lived chemical species in a middle atmosphere general circulation model, J. Geophys. Res., 108, 4494, doi:10.1029/2002JD002799, 2003.

Scarchilli, C., Adriani, A., Cairo, F., Di Donfrancesco, G., Buontempo, C., Snels, M., Moriconi, M. L., Deshler, T., Larsen, N., Luo, B., Mauersberger, K., Ovarlez, J., Rosen, J., and Schreiner, J.: Determination of PSC particle refractive indices using in situ optical measurements and T-matrix calculations, Appl. Opt., 16, 3302–3311, 2005.

Solomon, S.: Stratospheric ozone depletion: A review of concepts and history, Rev. Geophys., 37, 275–316, l999.

Spang, R., Remedios, J. J., Kramer, L. J., Poole, L. R., Fromm, M. D., Müller, M., Baumgarten, G., and Konopka, P.: Polar stratospheric cloud observations by MIPAS on ENVISAT: detection method, validation and analysis of the northern hemisphere winter 2002/2003, Atmos. Chem. Phys., 5, 679–692, 2005.

Stiller, G. P., Mengistu Tsidu, G., von Clarmann, T., Glatthor, N., Höpfner, M., Kellmann, S., Linden, A., Ruhnke, R., Fischer, H., Lopez-Puertas, M., Funke, B., and Gil-Lopez, S.: An enhanced HNO3 second maximum in the Antarctic midwinter upper stratosphere 2003, J. Geophys. Res., 110, D20303, doi:10.1029/2005JD006011, 2005.

Strahan, S. E. and Polansky, B. C.: Meteorological implementation issues in chemistry and transport models, Atmos. Chem. Phys., 6, 2895–2910, 2006.

Svendsen, S. H., Larsen, N., Knudsen, B., Eckermann, S. D., and Browell, E. V.: Influence of mountain waves and NAT nucleation mechanisms on Polar Stratospheric Cloud formation at local and synoptic scales during the 1999–2000 Arctic winter, Atmos. Chem. Phys. Discuss., 4, S2071–S2078, p. S2073, 2004.

Tabazadeh, A., Santee, M. L., Danilin, M. Y., Pumphrey, H. C., Newman, P. A., Hamill, P. J., and Mergenthaler, J. L.: Quantifying denitrification and its effect on ozone recovery, Science, 288, 1407–1411, 2000.

Tabazadeh, A., Djikaev, Y. S., Hamill, P., and Reiss, H.: Laboratory evidence for surface nucleation of solid polar stratospheric cloud particles, J. Phys. Chem. A, 106, 10 238–10 246, 2002.

Tolbert, M. A. and Toon, O. B.: Solving the PSC mystery, Science, 292, 61–63, 2001.

Voigt, C., Schreiner, J., Kohlman, A., Zink, P., Mauersberger, K., Larsen, N., Deshler, T., Kröger, C., Rosen, J., Adriani, A., Cairo, F., Di Donfrancesco, G., Viterbini, M., Ovarlez, J., Ovarlez, H., David, C., and Dörnbrack, A.: Nitric Acid Trihydrate (NAT) in Polar Stratospheric Clouds, Science, 290, 1756–1758, 2000.

Voigt, C., Schlager, H., Luo, B. P., Dörnbrack, A., Roiger, A., Stock, P., Curtius, J., Vössing, H., Borrmann, S., Davies, S., Konopka, P., Schiller, C., Shur, G., and Peter, T.: Nitric Acid Trihydrate (NAT) formation at low NAT supersaturation in Polar Stratospheric Clouds (PSCs), Atmos. Chem. Phys., 5, 1371–1380, 2005.

WMO: Scientific Assesment of Ozone Depletion: 1998, Global Ozone Research and Monitoring Project – Report No. 44, World Meteorological Organization, 1999.

Zhang, R., Leu, M.-T., and Molina, M. J.: Formation of polar stratospheric clouds on preactivated background aerosols, Geophys. Res. Lett., 23, 1669–1672, 1996.