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2007-09-18
Global distribution of mean age of stratospheric air from MIPAS SF<sub>6</sub> measurements
G. P. Stiller
gabriele.stiller@imk.fzk.de
T. von Clarmann
M. Höpfner
N. Glatthor
U. Grabowski
S. Kellmann
A. Kleinert
A. Linden
M. Milz
T. Reddmann
T. Steck
H. Fischer
B. Funke
M. López-Puertas
A. Engel
Forschungszentrum Karlsruhe and University of Karlsruhe, Institut für Meteorologie und Klimaforschung, Karlsruhe, Germany
Instituto de Astrofísica de Andalucía CSIC, Granada, Spain
Institut für Atmosphäre und Umwelt, J.~W.~Goethe Universität Frankfurt am Main, Frankfurt, Germany
now at: Institutionen för Rymdvetenskap, Luleå Tekniska Universitet, Kiruna, Sweden
Global distributions of profiles of sulphur hexafluoride (SF<sub>6</sub>) have been retrieved
from limb emission spectra recorded by the Michelson Interferometer
for Passive Atmospheric Sounding (MIPAS) on Envisat covering the period September 2002
to March 2004. Individual SF<sub>6</sub> profiles have a precision of 0.5 pptv below 25 km altitude and a vertical
resolution of 4–6 km up to 35 km altitude. These data have been validated versus
in situ observations obtained during balloon flights of a cryogenic whole-air sampler.
For the tropical troposphere a trend of 0.227±0.008 pptv/yr has been
derived from the MIPAS data, which is in excellent agreement with the trend from ground-based flask and in situ
measurements from the National Oceanic and Atmospheric Administration Earth System Research Laboratory, Global Monitoring Division.
For the data set currently available, based on at least three days of data per
month, monthly 5° latitude mean values have a 1σ standard error of 1%. From the global
SF<sub>6</sub> distributions, global daily and monthly distributions of the apparent mean age of air
are inferred by application of the tropical tropospheric trend derived from MIPAS data. The inferred
mean ages are provided for the full globe up to 90° N/S, and have a 1σ standard error of 0.25 yr.
They range between 0 (near the tropical tropopause) and 7 years (except for situations
of mesospheric intrusions) and agree well with earlier observations. The seasonal
variation of the mean age of stratospheric air indicates episodes of severe intrusion
of mesospheric air during each Northern and Southern polar winter observed,
long-lasting remnants of old, subsided polar winter air over the spring and
summer poles, and a rather short period of mixing with midlatitude air and/or
upward transport during fall in October/November (NH) and April/May (SH),
respectively, with small latitudinal gradients, immediately before the new polar
vortex starts to form. The mean age distributions further confirm that SF<sub>6</sub>
is destroyed in the mesosphere to a considerable amount. Model calculations
with the Karlsruhe simulation model of the middle atmosphere (KASIMA) chemical transport
model agree well with observed global distributions of the mean
age only if the SF<sub>6</sub> sink reactions in the mesosphere are included in the model.
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 CO<sub>2</sub>, CH<sub>4</sub>, and N<sub>2</sub>O, J. Geophys. Res., 106, 32 295–32 314, \doi10.1029/2001JD000465, 2001.
Austin, J. and Li, F.: On the relationship between the strength of the Brewer-Dobson circulation and the age of stratospheric air, Geophys. Res. Lett., 33, L17807, \doi10.1029/2006GL026867, 2006.
Boering, K A., Wofsy, S C., Daube, B C., Schneider, H R., Loewenstein, M., Podolske, J R., and Conway, T J.: Stratospheric Mean Ages and Transport Rates from Observations of Carbon Dioxide and Nitrous Oxide, Science, 274, 1340–1343, \doi10.1126/science.274.5291.1340, 1996.
Burgess, A B., Grainger, R G., Dudhia, A., Payne, V H., and Jay, V L.: MIPAS measurement of sulphur hexafluoride (SF$_6$), Geophys. Res. Lett., 31, L05112, \doi10.1029/2003GL019143, 2004.
Burgess, A B., Grainger, R G., and Dudhia, A.: Zonal mean atmospheric distribution of sulphur hexafluoride (SF$_6$), Geophys. Res. Lett., 33, L07809, \doi10.1029/2005GL025410, 2006.
Butchart, N., Scaife, A A., Bourqui, M., de~Grandpre, J., Hare, S. H E., Kettleborough, J., Langematz, U., Manzini, E., Sassi, F., Shibata, K., Shindell, D., and Sigmond, M.: Simulations of anthropogenic change in the strength of the Brewer-Dobson circulation, Clim. Dyn., 27, 727–741, \doi10.1007/s00382-006-0162-4, 2006.
Elkins, J W., Fahey, D W., Gilligan, J M., Dutton, G S., Baring, T J., Volk, C M., Dunn, R E., Myers, R C., Montzka, S A., Wamsley, P R., Hayden, A H., Butler, J H., Thompson, T M., Swanson, T H., Dlugokencky, E J., Novelli, P C., Hurst, D F., Lobert, J M., Ciciora, S J., McLaughlin, R J., Thompson, T L., Winkler, R H., Fraser, P J., Steele, L P., and Lucarelli, M P.: Airborne gas chromatograph for in situ measurements of long-lived species in the upper troposphere and lower stratosphere, Geophys. Res. Lett., 23, 347–350, \doi10.1029/96GL00244, 1996.
Engel, A., Bönisch, H., Brunner, D., Fischer, H., Franke, H., Günther, G., Gurk, C., Hegglin, M., Hoor, P., Königstedt, R., Krebsbach, M., Maser, R., Parchatka, U., Peter, T., Schell, D., Schiller, C., Schmidt, U., Spelten, N., Szabo, T., Weers, U., Wernli, H., Wetter, T., and Wirth, V.: Highly resolved observations of trace gases in the lowermost stratosphere and upper troposphere from the Spurt project: an overview, Atmos. Chem. Phys., 6, 283–301, 2006a.
Engel, A., Möbius, T., Haase, H.-P., Bönisch, H., Wetter, T., Schmidt, U., Levin, I., Reddmann, T., Oelhaf, H., Wetzel, G., Grunow, K., Huret, N., and Pirre, M.: Observation of mesospheric air inside the arctic stratospheric polar vortex in early 2003, Atmos. Chem. Phys., 6, 267–282, 2006b.
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., Koopmann, 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. Discuss., 7, 8795–8893, 2007.
Flaud, J.-M., Piccolo, C., Carli, B., Perrin, A., Coudert, L H., Teffo, J.-L., and Brown, L R.: Molecular line parameters for the MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) experiment, Atmos. Oceanic Opt., 16, 172–182, 2003.
Funke, B., López-Puertas, M., Stiller, G P., von Clarmann, T., and Höpfner, M.: A new non–LTE Retrieval Method for Atmospheric Parameters From MIPAS–ENVISAT Emission Spectra, Adv. Space Res., 27, 1099–1104, 2001.
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$\rm_x$ into the polar stratosphere and lower mesosphere during the Antarctic 2003 and Arctic 2002/2003 winters, J. Geophys. Res., 110, D24308, \doi10.1029/2005JD006463, 2005.
Funke, B., López-Puertas, M., , Bermejo-Pantaleón, D., von Clarmann, T., Stiller, G P., Höpfner, M., Grabowski, U., and Kaufmann, M.: Analysis of nonlocal thermodynamic equilibrium CO 4.7 μm fundamental, isotopic and hot band emissions measured by the Michelson Interferometer for Passive Atmospheric Sounding on Envisat, J. Geophys. Res., 112, D11305, \doi10.1029/2006JD007933, 2007.
Geller, L S., Elkins, J W., Lobert, J M., Clarke, A D., Hurst, D F., Butler, J H., and Myers, R C.: Tropospheric SF$_6$: Observed latitudinal distribution and trends, derived emissions and interhemispheric exchange time, Geophys. Res. Lett., 24, 675–678, \doi10.1029/97GL00523, 1997.
Glatthor, N., von Clarmann, T., Fischer, H., Funke, B., Gil-López, S., Grabowski, U., Höpfner, M., Kellmann, S., Linden, A., López-Puertas, M., Mengistu Tsidu, G., Milz, M., Steck, T., Stiller, G P., and Wang, D.-Y.: Retrieval of stratospheric ozone profiles from MIPAS/ENVISAT limb emission spectra: a sensitivity study, Atmos. Chem. Phys., 6, 2767–2781, 2006.
Hall, T M. and Waugh, D W.: Influence of nonlocal chemistry on tracer distributions: Inferring the mean age of air from SF$_6$, J. Geophys. Res., 103, 13,327–13,336, \doi10.1029/98JD00170, 1998.
Hauchecorne, A., Bertaux, J.-L., Dalaudier, F., Russell III, J M., Mlynczak, M G., Kyrölä, E., and Fussen, D.: Large increase of NO<sub>2</sub> in the north polar mesosphere in January-February 2004: Evidence of a dynamical origin from GOMOS/ENVISAT and SABER/TIMED data, Geophys. Res. Lett., 34, L03810, \doi10.1029/2006GL027628, 2007.
Höpfner, M., Oelhaf, H., Wetzel, G., Friedl-Vallon, F., Kleinert, A., Lengel, A., Maucher, G., Nordmeyer, H., Glatthor, N., Stiller, G P., von Clarmann, T., Fischer, H., Kröger, C., and Deshler, T.: Evidence of scattering of tropospheric radiation by PSCs in mid–IR limb emission spectra: MIPAS–B observations and KOPRA simulations, Geophys. Res. Lett., 29, 1278, \doi10.1029/2001GL014443, 2002.
Kida, H.: General circulation of air parcels and transport characteristics derived from a hemispheric GCM, Part 2, Very long-term motions of air parcels in the troposphere and stratosphere, J. Meteorol. Soc. Jpn., 61, 510–522, 1983.
Ko, M. K W., Sze, N D., Wang, W.-C., Shia, G., Goldman, A., Murcray, F J., Murcray, D G., and Rinsland, C P.: Atmospheric sulfur hexafluoride: Sources, sinks and greenhouse warming, J. Geophys. Res., 98, 10,499–10,507, \doi10.1029/93JD00228, 1993.
Konopka, P., Engel, A., Funke, B., Müller, R., Grooß, J.-U., Günther, G., Wetter, T., Stiller, G P., von Clarmann, T., Glatthor, N., Oelhaf, H., Wetzel, G., López-Puertas, M., Pirre, M., Huret, N., and Riese, M.: Ozone loss driven by nitrogen oxides and triggered by stratospheric warmings can outweigh the effect of halogens, J. Geophys. Res., 112, D05105, \doi10.1029/2006JD007064, 2007.
López-Puertas, M. and Taylor, F W.: Non-LTE radiative transfer in the Atmosphere, World Scientific Pub., Singapore, 2001.
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, \doi10.1029/2004JD005367, 2005a.
Manney, G L., Sabutis, J L., Allen, D R., Lahoz, W A., Scaife, A A., Randall, C E., Pawson, S., Naujokat, B., and Swinbank, R.: Simulations of Dynamics and Transport During the September 2002 Antarctic Major Warming, J. Atmos. Sci., 62, 690–707, 2005b.
Morris, R A., Miller, T M., Viggiano, A., and Paulson, J F.: Effects of electron and ion reactions on atmospheric lifetimes of fully fluorinated compounds, J. Geophys. Res., 100, 1287–1294, \doi10.1029/94JD02399, 1995.
Nemtchinov, V. and Varanasi, P.: Thermal infrared absorption cross-sections of CF<sub>4</sub> for atmospheric applications, J. Quant. Spectrosc. Radiat. Transfer, 82, 461–471, \doi10.1016/S0022-4073(03)00170-5, 2003.
Nett, H., Carli, B., Carlotti, M., Dudhia, A., Fischer, H., Flaud, J.-M., Perron, G., Raspollini, P., and Ridolfi, M.: MIPAS Ground Processor and Data Products, in: Proc. IEEE 1999 International Geoscience and Remote Sensing Symposium, 28 June – 2 July 1999, Hamburg, Germany, pp. 1692–1696, 1999.
Norton, H. and Beer, R.: New apodizing functions for Fourier spectrometry, J. Opt. Soc. Am, 66, 259–264, (Errata J. Opt. Soc. Am., 67, 419,1977), 1976.
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., 22, L18811, \doi10.1029/2006GL027160, 2006.
Randall, C E., Harvey, V L., Singleton, C S., Bailey, S M., Bernath, P F., Codrescu, M., Nakajima, H., and Russell III, J M.: Energetic particle precipitation effects on the Southern Hemisphere stratosphere in 1992-2005, J. Geophys. Res., 112, D08308, \doi10.1029/2006JD007696, 2007.
Ravishankara, A R., Solomon, S., Turnipseed, A A., and Warren, R F.: Atmospheric lifetimes of long-lived halogenated species, Science, 259, 194–199, \doi10.1126/science.259.5092.194, 1993.
Ray, E A., Moore, F L., Elkins, J W., Dutton, G S., Fahey, D W., Vömel, H., Oltmans, S J., and Rosenlof, K H.: Transport into the Northern Hemisphere lowermost stratosphere revealed by in situ tracer measurements, J. Geophys. Res., 104, 26,565–26,580, \doi10.1029/1999JD900323, 1999.
Ray, E A., Moore, F L., Elkins, J W., Hurst, D F., Romashkin, P A., S.Dutton, G., 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.
Reddmann, T., Ruhnke, R., and Kouker, W.: Three–dimensional model simulations of SF$_6$ with mesospheric chemistry, J. Geophys. Res., 106, 14,525–14,537, \doi10.1029/2000JD900700, 2001.
Rinsland, C P., Brown, L R., and Farmer, C B.: Infrared spectroscopic detection of sulfur hexafluoride (SF$_6$) in the lower stratosphere and upper troposphere, J. Geophys. Res., 95, 5577–5585, \doi10.1029/89JD03413, 1990.
Rinsland, C P., Gunson, M R., Abrams, M C., Lowes, L L., Zander, R., and Mahieu, E.: ATMOS/ATLAS1 measurements of sulfur hexafluoride (SF$_6$) in the lower stratosphere and upper troposphere, J. Geophys. Res., 98, 20,491–20,494, \doi10.1029/93JD02258, 1993.
Rinsland, C P., Goldman, A., Stephen, T M., Chiou, L S., Mahieu, E., and Zander, R.: SF$_6$ ground-based infrared solar absorption measurements: long-term trend, pollution events, and a search for SF$_5$CF<sub>3</sub> absorption, J. Quant. Spectrosc. Radiat. Transfer, 78, 41–53, 2003.
Rinsland, C P., Boone, C., Nassar, R., Walker, K., Bernath, P., Mahieu, E., Zander, R., McConnell, J C., and Chiou, L.: Trends of HF, HCl, CCl<sub>2</sub>F<sub>2</sub>, CCl<sub>3</sub>F, CHCLF<sub>2</sub> (HCFC-22), and SF$_6$ in the lower stratosphere from Atmospheric Chemistry Experiment (ACE) and Atmospheric Trace Molecule Spectroscopy (ATMOS) measurements near 30$^o$N latitude, Geophys. Res. Lett., 32, L16S03, \doi10.1029/2005GL022415, 2005.
Rodgers, C D.: Inverse Methods for Atmospheric Sounding: Theory and Practice, vol 2 of Series on Atmospheric, Oceanic and Planetary Physics, edited by: F W Taylor,, World Scientific, 2000.
Rothman, L S., Jacquemart, D., Barbe, A., Benner, D C., Birk, M., Brown, L R., Carleer, M R., Chackerian Jr., C., Chance, K., Coudert, L 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 \itHITRAN 2004 molecular spectroscopic database, J. Quant. Spectrosc. Radiat. Transfer, 96, 139–204, \doi10.1016/j.jqsrt.2004.10.008, 2005.
Schmidt, U. and Khedim, A.: In situ measurements of carbon dioxide in the winter Arctic vortex and at midlatitudes: An indicator of the "age" of stratospheric air, Geophys. Res. Lett., 18, 767–766, 1991.
Seppälä, A., Verronen, P T., Clilverd, M A., Randall, C E., Tamminen, J., Sofieva, V., Backman, L., and Kyrölä, E.: Arctic and Antarctic polar winter NO$_x$ and energetic particle precipitation in 2002-2006, Geophys. Res. Lett., 34, L12810, \doi10.1029/2007GL029733, 2007.
Spang, R., Remedios, J J., and Barkley, M P.: Colour indices for the detection and differentiation of cloud types in infra–red limb emission spectra, Adv. Space Res., 3, 1041–1047, \doi10.1016/S0273-1177(03)00585-4, 2004.
Steck, T.: Methods for determining regularization for atmospheric retrieval problems, Appl. Opt., 41, 1788–1797, 2002.
Steck, T. and von Clarmann, T.: Constrained profile retrieval applied to the observation mode of the Michelson Interferometer for Passive Atmospheric Sounding, Appl. Opt., 40, 3559–3571, 2001.
Stiller, G P., von Clarmann, T., Funke, B., Glatthor, N., Hase, F., Höpfner, M., and Linden, A.: Sensitivity of trace gas abundances retrievals from infrared limb emission spectra to simplifying approximations in radiative transfer modelling, J. Quant. Spectrosc. Radiat. Transfer, 72, 249–280, 2002.
Strunk, M., Engel, A., Schmidt, U., Volk, C M., Wetter, T., Levin, I., and Glatzel-Mattheier, H.: CO<sub>2</sub> and SF$_6$ as stratospheric age tracers: consistency and the effect of mesospheric SF$_6$–loss, Geophys. Res. Lett., 27, 341–344, \doi10.1029/1999GL011044, 2000.
Tikhonov, A.: On the solution of incorrectly stated problems and method of regularization, Dokl. Akad. Nauk. SSSR, 151, 501–504, 1963.
Varanasi, P., Li, Z., Nemtchinov, V., and Cherukuri, A.: Spectral Absorption–Coefficient Data on HCFC–22 and SF$_6$ for Remote–Sensing Applications, J. Quant. Spectrosc. Radiat. Transfer, 52, 323–332, 1994.
Volk, C M., Elkins, J W., Fahey, D W., Dutton, G S., Gilligan, J M., Loewenstein, M., Podolske, J R., Chan, K R., and Gunson, M R.: Evaluation of source gas lifetimes from stratospheric observations, J. Geophys. Res., 102, 25,543–25,564, \doi10.1029/97JD02215, 1997.
von Clarmann, T., Ceccherini, S., Doicu, A., Dudhia, A., Funke, B., Grabowski, U., Hilgers, S., Jay, V., Linden, A., López-Puertas, M., Mart\'\in-Torres, F.-J., Payne, V., Reburn, J., Ridolfi, M., Schreier, F., Schwarz, G., Siddans, R., and Steck, T.: A blind test retrieval experiment for infrared limb emission spectrometry, J. Geophys. Res., 108, 4746, \doi10.1029/2003JD003835, 2003a.
von Clarmann, T., Glatthor, N., Grabowski, U., Höpfner, M., Kellmann, S., Kiefer, M., Linden, A., Mengistu Tsidu, G., Milz, M., Steck, T., Stiller, G P., Wang, D Y., Fischer, H., Funke, B., Gil-López, S., and López-Puertas, M.: Retrieval of temperature and tangent altitude pointing from limb emission spectra recorded from space by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), J. Geophys. Res., 108, 4736, \doi10.1029/2003JD003602, 2003b.
Waugh, D W. and Hall, T M.: Age of stratospheric air: theory, observations, and models, Rev. Geophys., 40, 1010, \doi10.1029/2000RG000101, 2002.
Waugh, D W., Strahan, S E., and Newman, P A.: Transport and modeling of stratospheric inorganic chlorine, Atmos. Chem. Phys. Discuss., 7, 8597–8616, 2007.
Zander, R., Rinsland, C P., and Demoulin, P.: Infrared spectroscopic measurements of the vertical column abundance of sulfur hexafluoride, SF$_6$, from the ground, J. Geophys. Res., 96, 15 447–15 454, \doi10.1029/91JD01214, 1991.
Zander, R., Gunson, M R., Farmer, C B., Rinsland, C P., Irion, F W., and Mahieu, E.: The 1985 chlorine and fluorine inventories in the stratosphere based on ATMOS observations at 30$^\circ$ North latitude, J. Atm. Chem., 15, 171–186, \doi10.1007/BF00053758, 1992.