ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-10-1739-2010 Impact of energetic particle precipitation on stratospheric polar constituents: an assessment using monitoring and assimilation of operational MIPAS data Robichaud A. 1 Ménard R. 1 Chabrillat S. 2 de Grandpré J. 1 Rochon Y. J. 3 Yang Y. 3 Charette C. 1 Atmospheric Science and Technology Directorate, Environment Canada, 2121 Trans-Canada Highway, H9P 1J3, Dorval (Québec), Canada Belgium Institute for Space Aeronomy, Avenue Circulaire 3, 1180, Bruxelles, Belgium Atmospheric Science and Technology Directorate, Environment Canada, 4905 Dufferin Street, M3H 5T4, Toronto, Ontario, Canada 16 02 2010 10 4 1739 1757 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/10/1739/2010/acp-10-1739-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/1739/2010/acp-10-1739-2010.pdf

In 2003, strong energetic particle precipitation (EPP) events occurred producing massive amounts of ionization which affected the polar region significantly perturbing its chemical state down to the middle stratosphere. These events and their effects are generally left unaccounted for in current models of stratospheric chemistry and large differences between observations and models are then noted. In this study, we use a coupled 3-D stratospheric dynamical-chemical model and assimilation system to ingest MIPAS temperature and chemical observations. The goal is to gain further understanding of assimilation and monitoring processes during EPP events and their impacts on the stratospheric polar chemistry. Moreover, we investigate the feasibility of assimilating valid "outlier" observations associated with such events. We use <i>OmF</i> (Observation minus Forecast) residuals as they filter out phenomena well reproduced by the model (such as gas phase chemistry, transport, diurnal and seasonal cycles) thus revealing a clear trace of the EPP. Inspection of <i>OmF</i> statistics in both passive (without chemical assimilation) and active (with chemical assimilation) cases altogether provides a powerful diagnostic tool to assess the model and assimilation system. We also show that passive <i>OmF</i> can permit a satisfactory evaluation of the ozone partial column loss due to EPP effects. Results suggest a small but significant loss of 5–6 DU (Dobson Units) during an EPP-IE (EPP Indirect Effects) event in the Antarctic winter of 2003, and about only 1 DU for the SPE (Solar Proton Event) of October/November 2003. Despite large differences between the model and MIPAS chemical observations (NO<sub>2</sub>, HNO<sub>3</sub>, CH<sub>4</sub> and O<sub>3</sub>), we demonstrate that a careful assimilation with only gas phase chemistry included in the model (i.e. no provision for EPP) and with relaxed quality control nearly eliminated the short-term bias and significantly reduced the standard deviation error of the constituents below 1 hPa.

 References Aikin, A. C.: Energetic particle-induced enhancements of stratospheric nitric acid, Geophys. Res. Lett., 21(10), 859–862, 1994. Aikin, A. C.: Production of stratospheric HNO<sub>3</sub> by different ion-molecule reaction mechanisms, J. Geophys. Res., 102(D11), 12921–12925, 1997. Baier, F., Erbertseder, T., Morgenstern, O., Bittner, M., and Brasseur, G.: Assimilation of MIPAS observations using a three-dimensional global chemistry-transport model, Q. J. Roy. Meteor. Soc., 613, 3529–3542, 2005. Baker, D. N., Kanekal, S. G., Li, X., Monk, S. P., Goldstein, J., and Burch, J. L.: An extreme distortion of the Van Allen belt arising from the "Hallowe'en" solar storm in 2003, Nature, 432, 878–880, 2004. Batchelor, R., Strong, K., Lindenmaier, R., Manson, A., Meek, C., Manney, G., Daffer, W., Polavarapu, S., Reszka, M., Neish, M., Robichaud, A., et al.: Understanding the Arctic stratosphere during IPY through a combination of ground-based measurements, models and dynamical analyses, Presentation to AGU~2009, Joint Assembly, 24–27~May, Toronto, Canada, 2009. Baumgaertner, A. J. G., Jöckel, P., and Brühl, C.: Energetic particle precipitation in ECHAM5/MESSy1 - Part~1: Downward transport of upper atmospheric NO<sub>x</sub> produced by low energy electrons, Atmos. Chem. Phys., 9, 2729–2740, 2009. Brasseur, G. and Solomon, S.: Aeronomy of the Middle Atmosphere: Chemistry and Physics of the Stratosphere and Physics of the Stratosphere and Mesosphere, Third revised and enlarged ed., Springer, ISBN~978-1-4020-3284-4, 2005. Callis, L. B., Baker, D. N., Natarajan, M., Blake, J. B., Mewaldt, R. A., Selesnick, R., and Cummings, J. R.: A 2-D model simulation of downward transport of NO<sub>y</sub> into the stratosphere: Effects on the 1994 austral spring O<sub>3</sub> and NO<sub>y</sub>, Geophys. Res. Lett., 23, 1905–1908, 1996. Cortesi, U., Lambert, J. C., De Clercq, C., Bianchini, G., Blumenstock, T., Bracher, A., Castelli, E., Catoire, V., Chance, K. V., De Mazière, M., Demoulin, P., Godin-Beekmann, S., Jones, N., Jucks, K., Keim, C., Kerzenmacher, T., Kuellmann, H., Kuttippurath, J., Iarlori, M., Liu, G. Y., Liu, Y., McDermid, I. S., Meijer, Y. J., Mencaraglia, F., Mikuteit, S., Oelhaf, H., Piccolo, C., Pirre, M., Raspollini, P., Ravegnani, F., Reburn, W. J., Redaelli, G., Remedios, J. J., Sembhi, H., Smale, D., Steck, T., Taddei, A., Varotsos, C., Vigouroux, C., Waterfall, A., Wetzel, G., and Wood, S.: Geophysical validation of MIPAS-ENVISAT operational ozone data, Atmos. Chem. Phys., 7, 4807–4867, 2007. Côté, J., Gravel, S., Méthot, A., Patoine, A., Roch, M., and Staniforth, A. N.: The operational CMC-MRB Global Environmental Multiscale (GEM) model, Part~I: design considerations and formulation, Mon. Weather Rev., 126, 1373-1395, 1998. Daley, R.: Atmospheric data analysis, Cambridge University Press, 1991. Damian, V., Sandu, A., Damian, M., Potra, F., and Carmichael, G. R.: The kinetic preprocessor KPP – a software environment for solving chemical kinetics, Comput. Chem. Eng., 26, 1567–1579, 2002. Dee, D. P. and da Silva, A. M.: Data assimilation in the presence of forecast bias, Q. J. Roy. Meteor. Soc., 124, 269–295, 1998. de Grandpré, J., Ménard, R., Rochon, Y. J., Charrette, C., Chabrillat, S., and Robichaud, A.: Predictability of coupled chemistry-dynamics data assimilation, Mon. Weather Rev., 137, 679–692, 2009. Dethof, A.: Assimilation of ozone retrievals from the MIPAS instrument on board ENVISAT, ECMWF Technical Memorandum, 428, 2003. Dethof, A., Geer, A., Lahoz, W., Goutail, F., Bazureau, A., Wang, D. Y., and von Clarmann, T.: MIPAS temperature validation by the MASI group, ESA, in: Proceedings of the Second Workshop on the Atmospheric Chemistry Validation of ENVISAT (ACVE-2), ESA-ESRIN, Frascati, Italy (ESA SP-562), 3–7~May~2004, 23.1–23.5, 2004. de Zafra, R. and Smyshlyaev, S. P.: On the formation of HNO<sub>3</sub> in the Antarctic mid to upper stratosphere in winter, 106(23), 23115–23125, 2001. Errera, Q. and Fonteyn, D.: Four-dimensional variational chemical assimilation of CRISTA stratospheric measurements, J. Geophys. Res., 106, 12253–12265, 2001. Errera, Q., Daerden, F., Chabrillat, S., Lambert, J. C., Lahoz, W. A., Viscardy, S., Bonjean, S., and Fonteyn, D.: 4D-Var assimilation of MIPAS chemical observations: ozone and nitrogen dioxide analyses, Atmos. Chem. Phys., 8, 6169–6187, 2008. ESA (European Space Agency): ENVISAT, MIPAS, An instrument for atmospheric chemistry and climate research, ESA Publications Division, ESTEC, P.O Box~299, 2200~AG~Noordwijk, The Netherlands, SP-1229, 2000. Fischer, H. and Oelhaf, H.: Remote sensing of vertical profiles of atmospheric trace constituents with MIPAS limb-emission spectrometers, Appl. Optics, 35, 2787–2796, 1996. Fischer, H., Birk, M., Blom, C., Carli, B., Carlotti, M., von Clarmann, T., Delbouille, L., Dudhia, A., Ehhalt, D., Endemann, M., Flaud, J. M., Gessner, R., Kleinert, A., Koopman, R., Langen, J., López-Puertas, M., Mosner, P., Nett, H., Oelhaf, H., Perron, G., Remedios, J., Ridolfi, M., Stiller, G., and Zander, R.: MIPAS: an instrument for atmospheric and climate research, Atmos. Chem. Phys., 8, 2151–2188, 2008. Funke, B., López-Puertas, M., Gil-López, S., von Clarmann, T., Stiller, G. P., Fischer, H., and Kellmann, S.: Downward transport of upper atmospheric NO<sub>x</sub> into the polar stratosphere and lower mesosphere during the Antarctic~2003 and Arctic~2002/2003 winters, J. Geophys. Res., 110, D24308, doi:10.10129/2005JD006463, 2005. Gauthier, P., Charrette, C., Fillion, L., Koclas, P., and Laroche, S: Implementation of a 3D variational data assimilation system at the Canadian Meteorological Centre, Part~I: The global analysis, Atmos. Ocean, 37, 103–156, 1999. Gauthier, P., Chouinard, C., and Brasnett, B.: Quality control: Methodology and applications, in: Data Assimilation for the Earth System, edited by: Swinbank, R., Shutyaev, V., and Lahoz, W. A., NATO Science Series~IV: Earth and Environment Science, Kluwer Academic Publishers, 26, 177–187, 2003. Hairer, E. and Wanner, G.: Solving ordinary differential equations~2 – Stiff and differential-algebraic problems, Springer series in computational mathematics, Springer, Second edition, Vol 14, 1996. Hollingsworth, A. and Lönnberg, P.: The statistical structure of short-range forecast errors as determined from radiosonde data, Part~I The wind field, Tellus, 38A, 111–136, 1986. Jackman, C. H., McPeters, R. D., Labow, G. J., Fleming, E. L., Praderas, C. J., and Russell, J. M.: Northern hemisphere atmospheric effects due to the July~2000 Solar Proton Event, Geophys. Res. Lett., 28(1), 2883–2886, 2001. Jackman, C. H. and McPeters, R. D.: The Effect of Solar Proton Events on Ozone and Other Constituents, in: Solar Variability and its Effects on Climate, edited by: Pap, J. M., Fox, P., Frohlich, C., Hudson, H. S., Kuhn, J., McCormack, J., North, G., Sprigg, W., and Wu, S. T., AGU, Washington, D.C., Geoph. Monog. Series, 141, 305–319, 2004. Jackman, C. H., DeLand, M. T., Labow, G. J., Fleming, E. L., Weisenstein, D. K., Ko, M. K. W., Sinnhuber, M., and Russell, J. M.: Neutral atmospheric influences of the solar proton events in October-November~2003, J. Geophys. Res., 110, A09S27, doi:10.1029/2004JA010888, 2005. Jackman, C. H., Marsh, D. R., Vitt, F. M., Garcia, R. R., Fleming, E. L., Labow, G. J., Randall, C. E., López-Puertas, M., Funke, B., von Clarmann, T., and Stiller, G. P.: Short- and medium-term atmospheric constituent effects of very large solar proton events, Atmos. Chem. Phys., 8, 765–785, 2008. Kalnay, E.: Atmospheric Modeling, Data Assimilation and Predictability, Cambridge University Press, 2003. Kawa, S. R., Kumer, J. B., Douglass, A. R., Roche, A. E., Smith, S. E., Taylor, F. W., and Allen, D. J.: Missing chemistry of reactive nitrogen in the upper stratospheric polar winter, Geophys. Res. Let., 22, 2629–2632, 1995. López-Puertas, M., Funke, B., Gil-López, S., von Clarmann, T., Stiller, G. P., Höpfner, M., Kellmann, S., Fischer, H., and Jackman, C. H.: Observation of NO<sub>x</sub> enhancement and ozone depletion in the Northern and Southern Hemispheres after the October–November~2003 solar proton events, J. Geophys. Res., 110, A09S43, doi:10.1029/2005JA011050, 2005. Manney, G. L., Zurek, R. W., O'Neill, A., and Swinbank, R.: On the motion of air through the stratospheric polar vortex, J. Atmos. Sci., 51, 2973–2994, 1994. Manney, G. L., Krüger, K., Sabutis, J. L., Sena, S. A., and Pawson, S.: The remarkable 2003-2004 winter and other recent warm winters in the Arctic stratosphere since the late 1990s, J. Geophys. Res., 110, D04107, doi:10.10129/2004JD005367, 2005. McDonald, M. R. L., de Zafra, R., and Muscari, G.: Millimiter wave spectroscopic measurements over the South Pole, 5, Morphology and evolution of HNO<sub>3</sub> vertical distribution, 1993 versus 1995, J. Geophys. Res., 105, 17739–17750, 2000. Ménard, R., Gauthier, P., de Grandpré, J., Robichaud, A., Rochon, Y., Chabrillat, S., Fonteyn, D., von Clarmann, T., Yang, Y., Charron, M., McConnell, J., Kaminski, J., Vaillancourt, P., Charrette, C., and Kallaur, A.: Coupled chemical-dynamical data assimilation, executive summary available at http://esamultimedia.esa.int/docs/gsp/completed/C18560ExS.pdf, last access: 10~February~2010, ESA/ESTEC Contract No 18560/04/NL/FF, 2007. Ménard, R.: Bias estimation, in: Data assimilation, edited by: Lahoz, W., Khattatov, B., and Ménard, R., Springer, 2009. Orsolini, Y. J., Manney, G. L., Santee, M., Randall, C. E.: An upper stratospheric layer of enhanced HNO<sub>3</sub> following exceptional solar storms, Geophys. Res. Lett., 32(12), L12S01, doi:10.129/2004GL021588, 2005. Orsolini, Y. J.: Arctic ozone loss inferred from assimilation of MLS and SBUV observations, 37th~COSPAR Scientific Assembly, Montreal, Canada, 13–20~July~2008, A11-0078-08, 2008. Parrish, D. F. and Derber, J. C.: The National Meteorological Center's Spectral Statistical-Interpolation Analysis System, Mon. Weather Rev., 120, 1747–1763, 1992. Polavarapu, S., Ren, S., Rochon, Y., Sankey, D., Ek, N., Koshyk, J., and Tarasick, D.: Data assimilation with the Canadian Middle Atmosphere Model, Atmos. Ocean, 43(1), 77–100, 2005. Randall, C. E., Harvey, V. L., Singleton, C. S., Bernath, P. F., Boone, C. D., and Kozyra, J. U.: Enhanced NO<sub>x</sub> in 2006 linked to strong upper stratospheric Arctic vortex, Geophys. Res. Lett., 33, L18811, doi:10.1029/2006GL027160, 2006. Randall, C. E., Harvey, V. L., Singleton, C. S., Bailey, S. M., Bernath, P. F., Codrescu, M., Nakajima, H., and Russell, J. M.: Energetic particle precipitation effects on the Southern Hemisphere stratosphere in 1992–2005, J. Geophys. Res., 112, D08308, doi:10.1029/2006JD007696, 2007. Ridolfi, M., Blum, U., Carli, B., Catoire, V., Ceccherini, S., Claude, H., De Clercq, C., Fricke, K. H., Friedl-Vallon, F., Iarlori, M., Keckhut, P., Kerridge, B., Lambert, J.-C., Meijer, Y. J., Mona, L., Oelhaf, H., Pappalardo, G., Pirre, M., Rizi, V., Robert, C., Swart, D., von Clarmann, T., Waterfall, A., and Wetzel, G.: Geophysical validation of temperature retrieved by the ESA processor from MIPAS/ENVISAT atmospheric limb-emission measurements, Atmos. Chem. Phys., 7, 4459–4487, 2007. Rinsland, C. P., Boone, C., Nassar, R., Walker, K., Bernath, P., McConnell, J. C., and Chiou, L.: Atmospheric Chemistry Experiment (ACE), Arctic stratospheric measurements of NO<sub>x</sub> during February and March~2004: Impact of intense solar flares, Geophys. Res. Lett., 32, L16S05, doi:10.1029/2005GL022425, 2005. Rozanov, E., Callis, L., Schlesinger, M., Yang, F., Andronova, N., and Zubov, V.: Atmospheric response to NO<sub>y</sub> source due to energetic electron precipitation, Geophys. Res. Lett., 32, L14811, doi:1029/2005GL023041, 2005. 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., Molina, M. J., and Finlayson-Pitts, B. J.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies, Evaluation Number~14, Publication~02-25, JPL, 2003. Semeniuk, K., McConnell, J. C., and Jackman, C. H.: Simulation of the October-November 2003 solar proton events in the CMAM~GCM: Comparison with observations, Geophys. Res. Lett., 32, L15S02, doi:10.1029/2005GL022392, 2005. Seppälä, A., Verronen, P. T., Kyrölä, E., Hassinen, S., Backman, L., Hauchecorne, A., Bertaux, J. L., and Fussen, D.: Solar proton events of October–November~2003: Ozone depletion in the Northern Hemisphere polar winter as seen by GOMOS/Envisat, Geophys. Res. Lett., 31(19), L19107, doi:10.1029/2004GL021042, 2004. Seppälä, A., Verronen, P. T., Cliverd, M. A., et al.: Arctic and Antarctic polar vortex NO<sub>x</sub> and energetic particle precipitation in 2002–2006, Geophys. Res. Lett., 34, L12810, doi:10.1029/2007GL029733, 2007. Sinnhuber, B.-M., von der Gathen, P., Sinnhuber, M., Rex, M., König-Langlo, G., and Oltmans, S. J.: Large decadal scale changes of polar ozone suggest solar influence, Atmos. Chem. Phys., 6, 1835–1841, 2006. Siskind, D. E., Nedoluha, G. E., Randall, C. E., Fromm, M., and Russell~III, J. M.: An assessment of Southern Hemisphere stratospheric NO<sub>x</sub> enhancements due to transport from the upper atmosphere, Geophys. Res. Lett., 27, 329–332, 2000. Siskind, D. E., Eckermann, S. D., Coy, L., McCormack, J. P., and Randall, C. E.: On recent interannual variability of the Arctic winter mesosphere: Implications for tracer descent, Geophys. Res. Lett., 34, L09806, doi:10.1029/2007GL029293, 2007. Solomon, S. and Crutzen, P. J.: Analysis of the August~1972 solar proton event including chlorine chemistry, J. Geophys. Res., 86, 1140–1151, 1981. Stiller, G. P., Gizaw, M. T., von Clarmann, T., Glatthor, N., Höpfner, M., Kellmann, S., Linden, A., Ruhnke, R., Fischer, H., López-Puertas, M., Funke, B., and Gil-López, S.: An enhanced HNO<sub>3</sub> second maximum in the Antarctic midwinter upper stratosphere 2003, J. Geophys. Res., 110, D20303, doi:10.1029/2005JD006011, 2005. Turunen, E., Verronen, P. T., Seppälä, A., Rodger, C. J., Clilverd, M. A., Tamminen, J., Enell, C. F., and Ulich, T.: Impact of different energies of precipitating particles on NO<sub>x</sub> generation in the middle and upper atmosphere during geomagnetic storms, J. Atmos. Sol.-Terr. Phy., 71, 1176–1189, doi:10,1016/j.jastp.2008.07.05, 2009. Verronen, P. T., Funke, B., López-Puertas, M., Stiller, G. P., von Clarmann, T., Glatthor, N., Enell, C.-F., Turunen, E., and Tamminen, J.: About the increase of HNO<sub>3</sub> in the stratopause region during the Halloween~2003 solar proton event, Geophys. Res. Lett., 35, L20809, doi:10,1029/2008GL035312, 2008. Vogel, B., Konopka, P., Grooß, J.-U., Müller, R., Funke, B., López-Puertas, M., Reddmann, T., Stiller, G., von Clarmann, T., and Riese, M.: Model simulations of stratospheric ozone loss caused by enhanced mesospheric NO<sub>x</sub> during Arctic Winter 2003/2004, Atmos. Chem. Phys., 8, 5279–5293, 2008. von Clarmann, T.: Personal discussion at ESTEC, The Netherlands, 2007. Wang, D. Y., von Clarmann, T., Fischer, H., et al.: Validation of stratospheric temperatures measured by Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat, J. Geophys. Res., 110, D08301, doi:10.1029/2004JD005342, 2005. Wetzel, G., Bracher, A., Funke, B., Goutail, F., Hendrick, F., Lambert, J.-C., Mikuteit, S., Piccolo, C., Pirre, M., Bazureau, A., Belotti, C., Blumenstock, T., De Mazière, M., Fischer, H., Huret, N., Ionov, D., López-Puertas, M., Maucher, G., Oelhaf, H., Pommereau, J.-P., Ruhnke, R., Sinnhuber, M., Stiller, G., Van Roozendael, M., and Zhang, G.: Validation of MIPAS-ENVISAT NO<sub>2</sub> operational data, Atmos. Chem. Phys., 7, 3261–3284, 2007. WMO: Scientific Assessment of Ozone Depletion: 2006, Global Ozone Research and Monitoring, Project – Report No 50, World Meteorological Organization, Geneva, 2007.