Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 9 3 2009 10.5194/acpd-9-11551-2009 http://www.atmos-chem-phys-discuss.net/9/11551/2009/ http://www.atmos-chem-phys-discuss.net/9/11551/2009/acpd-9-11551-2009.html http://www.atmos-chem-phys-discuss.net/9/11551/2009/acpd-9-11551-2009.pdf 11551 11587 2009-05-11 First multi-year occultation observations of CO₂ in the MLT by ACE satellite: observations and analysis using the extended CMAM S. R. Beagley beagley@nimbus.yorku.ca C. D. Boone V. I. Fomichev J. J. Jin K. Semeniuk J. C. McConnell P. F. Bernath Department of Earth and Space Science and Engineering, York University, Toronto, Ontario, Canada Department of Chemistry, University of Waterloo, Waterloo, Ontario, Canada Department of Chemistry, University of York, Heslington, York, UK This paper presents the first multi-year global set of observations of CO₂ in the mesosphere and lower thermosphere (MLT) obtained by the ACE-FTS instrument on SCISAT-I, a small Canadian satellite launched in 2003. The observations use the solar occultation technique and document the fall-off in the mixing ratio of CO₂ in the MLT region. The beginning of the fall-off of the CO₂, or "knee" occurs at about 78 km and lies higher than in the CRISTA measurements (~70 km) but lower than in the SABER 1.06 (~82 km) and much lower than in rocket measurements. We also present the measurements of CO obtained concurrently which provide important constraints for analysis. We have compared the ACE measurements with simulations of the CO₂ and CO distributions in the vertically extended version of the Canadian Middle Atmosphere Model (CMAM). Applying standard chemistry we find that we cannot get agreement between the model and ACE CO₂ observations although the CO observations are adequately reproduced. There appears to be about a 10 km offset compared to the observed ACE CO₂, with the model knee occurring too high. In analysing the disagreement, we have investigated the variation of several parameters of interest, photolysis rates, formation rate for CO₂, and the impact of uncertainty in eddy diffusion, in order to explore parameter space for this problem. Our conclusions are that there must be a loss process for CO₂, about 2–4 times faster than photolysis that will sequester the carbon in some form other than CO and we have speculated on the role of meteoritic dust as a possible candidate. In addition, from this study we have highlighted a possible important role for vertical eddy diffusion in 3-D models in determining the distribution of candidate species in the mesosphere which requires further study. Beagley, S. R., McLandress, C., Fomichev, V. I., and Ward, W. E.: The Extended Canadian Middle Atmosphere Model, Geophys. Res. Lett., 27(16), 2529–2532, 2000. Beagley, S. R., McConnell, J. C., Fomichev, V. I., Semeniuk, K., Jonsson, A. I., Garcia Munoz, A., McLandress, C., and Shepherd, T. G.: Extended CMAM: Impacts of thermospheric neutral and ion chemistry on the middle atmosphere, AGU, fall, 2007. Bernath, P. F., McElroy, C. T., Abrahams, M. C., Boone, C. D., Butler, M., Camy-Peyret, C., Carleer, M., Clerbaux, C., Coheur, P.F., Colin, R., DeCola, P., DeMazire, M., Drummond, J. R., Dufour, D., Evans, W. F. J., Fast, H., Fussen, D., Gilbert, K., Jennings, D. E., Llewellyn, E. J., Lowe, R. P., Mahieu, E., McConnell, J. C., McHugh, M., McLeod, S. D., Michaud, R., Midwinter, C., Nassar, R., Nichitiu, F., Nowlan, C., Rinsland, C. P., Rochon, Y. J., Rowlands, N., Semeniuk, K., Simon, P., Skelton, R., Sloan, J. J., Soucy, M.-A., Strong, K., Tremblay, P., Turnbull, D., Walker, K. A., Walkty, I., Wardle, D. A., Wehrle, V., Zander, R., and Zou, J.: Atmospheric Chemistry Experiment(ACE): Mission overview, Geophys. Res. Lett., 32, L15S01, doi:10.1029/2005GL022386, 2005. Boone, C. D., Nassar, R., Walker, K. A., Rochon, Y., McLeod, S. D., Rinsland, C. P., and Bernath, P. F.: Retrievals for the atmospheric chemistry experiment Fourier-transform spectrometer, Appl. Opt., 44(33), 7218–7231, 2005. Brasseur, G. and Solomon, S.: Aeronomy of the Middle Atmosphere, D. Reidel, 441 pp., 1984. Chabrillat, S. and Kockarts, G.: Simple parameterization of the absorption of the solar Lyman-alpha line, Geophys. Res. Lett., 24, 2659–2662, 1997. Chabrillat, S., Kockarts, G., Fonteyn, D., and Brasseur, G.: Impact of molecular diffusion on the CO₂ distribution and the temperature in the mesosphere, Geophys. Res. Lett., 29, 1729, doi:10.1029/2002GL015309 2002. de Grandpré, J., Beagley, S. R., Fomichev, V. I., Griffioen, E., McConnell, J. C., Medvedev, A. S., and Shepherd, T. G.: Ozone climatology using interactive chemistry: Results from the Canadian Middle Atmosphere Model, J. Geophys. Res., 105(D21), 26475–26492, doi:10.1029/2000JD900427, 2000. Fomichev, V. I., Blanchet, J.-P., and Turner, D. S.: Matrix parameterization of the 15 μm CO₂ band cooling in the middle and upper atmosphere for variable CO₂ concentration, J. Geophys. Res., 103, 11505–11528, 1998. Fomichev, V. I., Ward, W. E., Beagley, S. R., McLandress, C., McConnell, J. C., McFarlane, N. A., and Shepherd, T. G.: Extended Canadian Middle Atmosphere Model: Zonal-mean climatology and physical parameterizations, J. Geophys. Res., 107(D10), 4087, doi:10.1029/2001JD000479, 2002. Girard, A., Besson, J., Brard, D., Laurent, J., Lemaitre, M. P., Lippens, C., Muller, C., Vercheval, J., and, Ackerman, M.: Global results of grille spectrometer experiment on board Spacelab 1, Planet. Space Sci., 36, 291–300, 1988. Hines, C. O.: Doppler-spread parameterization of gravity-wave momentum deposition in the middle atmosphere. Part 1: Basic formulation, J. Atmos. Sol.-Terr. Phys., 59, 371–386, 1997a. Hines, C. O.: Doppler-spread parameterization of gravity-wave momentum deposition in the middle atmosphere. Part 2: Broad and quasi-monochromatic spectra, and implementation, J. Atmos. Sol.-Terr. Phys., 59, 387–400, 1997b. Jin, J. J., Semeniuk, K., Beagley, S. R., Fomichev,V. I., Jonsson A. I., McConnell, J. C., Urban, J., Murtagh, D., Manney, G. L., Boone, C. D., Bernath, P. F., Walker, K. A., Barret, B., Ricaud, P., and Dupuy, E.: Comparison of CMAM simulations of CO (CO), nitrous oxide (N₂O), and methane (CH₄) with observations from Odin/SMR, ACE-FTS, and Aura/MLS, Atmos. Chem. Phys. Discuss., 8, 13063–13123, 2008. Jin, J. J., Semeniuk, K., Jonsson, A. I., Beagley, S. R., McConnell, J. C., Boone, C. D.,Walker, K. A., Bernath, P. F., Rinsland, C. P., Dupuy, E., Ricaud, P., De la Noe, J., Urban, J., and Murtagh, D.: A comparison of co-located ACE-FTS and SMR stratospheric-mesospheric CO measurements during 2004 and comparison with a GCM, Geophys. Res. Letts, 32, L15S03, doi:10.1029/2005GL022433, 2005. Karaiskou, A., Vallance, C., Papadakis, V., Vardavas, I. M., and Rakitzis, T. P.: Absolute absorption cross-section measurements of CO₂ in the ultraviolet from 200 to 206 nm at 295 and 373 K , Chem. Phys. Lett., 400, 30–34, 2004. Kaufmann, M., Gusev, O. A., Grossmann K. U., Roble, R. G., Hagan, M. E., Hartsough, C., and Kutepov, A. A.: The vertical and horizontal distribution of CO₂ densities in the upper mesosphere and lower thermosphere as measured by CRISTA, J. Geophys. Res., 107(D23), 8182, doi:10.1029/2001JD000704, 2002. Kaye, J. A. and Miller, T. L.: The ATLAS series of shuttle missions, Geophys. Res. Lett., 23, 2285–2288, 1996. Kumer, J. B., Stair Jr., A. T., Wheeler, N., Baker, K. D., and Baker, D. J.: Evidence for an OH$^\ne\buildrel vv\over\longrightarrow $ N$_2^\ne\buildrelvv\over\longrightarrow$CO₂ ($\nu_3) \buildrel\over\longrightarrow$ O₂+hν (4.3 μm) mechanism for 4.3-μm airglow, J. Geophys. Res., 83, 4743–4747, 1978. Lewis, B. R. and Carver, J. H.: Temperature dependence of the carbon dioxide photoabsorption cross section between 1200 and 1970 A, J. Quant. Spectrosc. Radiat. Trans., 30, 297–309, 1983. Lindzen R. S.: Turbulence and stress owing to gravity wave and tidal breakdown. J. Geophys. Res., 86, 9704–9714, 1981. López-Puertas, M. and Taylor, F. W.: Non-LTE Radiative Transfer in the Atmosphere. World Scientific, Singapore/New Jersey/London/Hong Kong, 487 pp., 2001. López-Puertas, M. and Taylor, F. W.: Carbon dioxide 4.3 μm emission in the Earth's atmosphere: A comparison between NIMBUS 7 SAMS measurements and non-local thermodynamic equilibrium radiative transfer calculations, J. Geophys. Res., 94, 13045–13068, 1989. López-Puertas, M., Zaragoza, G., López-Valverde, M. Á., and Taylor, F. W.: Non local thermodynamic equilibrium (LTE) atmospheric limb emission at 4.6 μm 2, An analysis of the daytime wideband radiances as measured by UARS improved stratospheric and mesospheric sounder, J. Geophys. Res., 103, 8515–8530, 1998. McLandress, C., Ward, W. E., Fomichev, V. I., Semeniuk, K., Beagley, S. R., McFarlane, N. A., and Shepherd, T. G.: Large-scale dynamics of the mesosphere and lower thermosphere: An analysis using the extended Canadian Middle Atmosphere Model, J. Geophys. Res., 111, D17111, doi:10.1029/2005JD006776, 2006. Megner, L., Siskind, D. E., Rapp, M., and Gumbel, J.: Global and temporal distribution of meteoric smoke: A two-dimensional simulation study, J. Geophys. Res., 113, D03202, doi:10.1029/2007JD009054, 2008. Mertens, C. J., Winick, J. R., Picard, R. H., Evans, D. S., López-Puertas, M., Wintersteiner, P. P., Xu, X., Mlynczak, M. G., and Russell III, J. M.: Influence of solar-geomagnetic disturbances on SABER measurements of 4.3 μm emission and the retrieval of kinetic temperature and carbon dioxide, Adv. Space Res., 43, 1325–1336, 2009. Mertens, C. J., Russell, J. M., Mlynczak, M. Y., She, C.-Y., Schmidlin, F. J., Goldberg, R. A., López-Puertas, M., Wintersteiner, P. P., Picard, R. H., Winick, J. R., and Xu, X.: Kinetic temperature and carbon dioxide from broadband infrared limb emission measurements taken from the TIMED/SABER instrument, Adv. Space Res., 43, 15–27, 2009. Nebel, H., Wintersteiner, P. P., Picard, R. H., Winick, J. R., Sharma, and R. D.: CO₂ non-local thermodynamic equilibrium radiative excitation and infrared dayglow at 4.3 μm: Application to spectral infrared rocket experiment data, J. Geophys. Res., 99, 10409–10419, 1994. Offermann, D. and Grossmann, K. U.: Thermospheric density and compositions as determined by a mass spectrometer with cryo ion source, J. Geophys. Res., 78, 8296–8304, 1973. Offermann, D., Friedrich, V., Ross, P., and Von Zahn, U.: Neutral gas composition measurements between 80 and 120 km, Planet. Space Sci., 29, 747–764, 1981. Ogibalov V. P. and Fomichev, V. I.: Parameterization of solar heating by the near IR CO₂ bands in the mesosphere, Adv. Space Res., 32, 759–764, 2003. Parkinson, W. H., Rufus, J., and Yoshino, K.: Absolute absorption cross section measurements of CO₂ in the wavelength region 163–200 nm and the temperature dependence, Chem. Phys., 290, 251–256, 2003. Philbrick, C. R., Faucher, G. A., and Trzcinski, E.: Rocket measurements of mesospheric and lower thermospheric composition, Space Res., 13, 255–260, Akademie, Berlin, Germany, 1973. Remsberg, E. E., Marshall, B. T., Garcia-Comas, M., Krueger, D., Lingenfelser, G. S., Martin-Torres, J., Mlynczak, M. G., Russell III, J. M., Smith, A. K., Zhao, Y., Brown, C., Gordley, L. L., López-Gonzalez, M. J., López-Puertas, M., She, C.-Y., Taylor, M. J., and Thompson, R. E.: Assessment of the quality of the Version 1.07 temperature-versus-pressure profiles of the middle atmosphere from TIMED/SABER, J. Geophys. Res., 113, D17101, doi:10.1029/2008JD010013, 2008. Rinsland, C., Gunson, M. R., Zander, R., and López-Puertas, M.: Middle and upper atmosphere pressure-temperature profiles and the abundances of CO₂ and CO in the upper atmosphere from ATMOS/Spacelab 3 observations, J. Geophys. Res., 97, 20479–20495, 1992. Roble, R. G.: Energetics of the mesosphere and thermosphere, the upper mesosphere and lower thermosphere: A review of experiment and theory, AGU Monograph, 87, 1995. Rothman, L. S., Jacquemart, D., Barbe, A., Benner, C. C., Birk, M., Brown, L. R., Carleer, M. R., Chackerian Jr., C., Chance, K., Coudert, K. H., Dana, V., Devi, V. M., Flaud, J.-M., Gamache, R. R., Goldman, A., Hartmann, J. -M., Jucks, K. W., Maki, A. G., Mandin, J. -Y., Massie, S. T., Orphal, J., Perrin, A., Rinsland, C. P., Smith, M. A. H., Tennyson, J, Tolchenov, R. N., Toth, R. A., Vander Auwera, J., Varanasi, P., and Wagner, G.: The HITRAN 2004 molecular spectroscopic database, J. Quant. Spectr. Radiat. Trans., 96, 139–204, 2005. Schmidt, H., Brasseur, G. P., Charron, M., Manzini, E., Giorgetta, M. A., Diehl, T., Fomichev, V. I., Kinnison, D., Marsh, D., and Walters, S.: The HAMMONIA chemistry climate model: Sensitivity of the mesopause region to the 11-year solar cycle and CO₂ doubling, J. Climate, 19, 3903–3931, 2006. Schulz, C., Koch, J. D., Davidson, D. F., Jeffries, J. B., and Hanson, R. K.: Ultraviolet absorption spectra of shock-heated carbon dioxide and water between 900 and 3050 K, Chem. Phys. Lett., 355, 82–88, 2002. Shemansky, D. E.: CO₂ Extinction Coefficient 1700–3000 Å, J. Chem. Phys., 56, 1582–1587, 1972. Trinks, H. and Fricke, K. H.: Carbon dioxide concentrations in the lower thermosphere, J. Geophys. Res., 83, 3883–3886, 1978. Yoshino, K., Esmond, J. R., Sun, Y., Parkinson, W. H., Ito, K., and Matsui, T.: Absorption cross section measurements of carbon dioxide in the wavelength region 118.7–175.5 nm and the temperature dependence. J. Quant. Spectrosc. Radiat. Transfer, 55, 53–60, 1991. Zaragoza, G., López-Puertas, M., López-Valverde, M. A., and Taylor, F. W.: Global distribution of CO₂ in the upper mesosphere as derived from UARS/ISAMS measurements, J. Geophys. Res., 105, 19829–19839, 2000.