BUDGETS OF CHLORINE AND FLUORINE; HALOGENATED GASES; SPECTROSCOPIC OBSERVATIONS; atmospheric composition; remote sensing; Montreal Protocol; ATMOS; stratosphere
Abstract :
[en] The set of high-resolution infrared solar observations made with the Atmospheric Trace Molecule Spectroscopy (ATMOS) - Fourier transform spectrometer from onboard Spacelab 3 (30 April-1 May 1985) has been used to evaluate the total budgets of the odd chlorine and fluorine chemical families in the stratosphere. These budgets are based on volume mixing ratio profiles measured for HCl, HF, CH3Cl, ClONO2, CCl4, CCl2F2, CCl3F, CHClF2, CF4, COF2, and SF6, near 30-degrees north latitude. When including realistic concentrations for species not measured by ATMOS, i.e., the source gases CH3CCl3, and C2F3Cl3 below 25 km, and the reservoirs ClO, HOCl and COFCl between 15 and 40 km (five gases actually measured by other techniques), the 30-degrees-N zonal 1985 mean total mixing ratio of chlorine, Cl, was found to be equal to (2.58 +/- 0.10) ppbv (parts per billion by volume) throughout the stratosphere, with no significant decrease near the stratopause. The results for total fluorine indicate a slight, but steady, decrease of its volume mixing ratio with increasing altitude, around a mean stratospheric value of (1.15 +/- 0.12) ppbv. Both uncertainties correspond to one standard deviation. These mean springtime 1985 stratospheric budgets are commensurate with values reported for the tropospheric Cl and F concentrations in the early 1980s, when allowance is made for the growth rates of their source gases at the ground and the time required for tropospheric air to be transported into the stratosphere. The results are discussed with emphasis on conservation of fluorine and chlorine and the partitioning among source, sink, and reservoir gases throughout the stratosphere.
Zander, Rodolphe ; Université de Liège - ULiège > Services généraux (Faculté des sciences) > Relations académiques et scientifiques (Sciences)
Gunson, Michael R.; California Institute of Technology (Pasadena, U.S.A.) > Jet Propulsion Laboratory
Farmer, Crofton B.; California Institute of Technology (Pasadena, U.S.A.) > Jet Propulsion Laboratory
Rinsland, Curtis P.; NASA Langley Research Center (Virginia, USA)
Irion, F. W.; California Institute of Technology( Pasadena, U.S.A.) > Department of Chemical Engineering
Mahieu, Emmanuel ; Université de Liège - ULiège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Language :
English
Title :
The 1985 chlorine and fluorine inventories in the stratosphere based on atmos observations at 30-degrees north latitude
Anderson J.G., Margitan J.J., Stedman D.H. (1977) Atomic chlorine and the chlorine monoxide radical in the stratosphere: three in-situ observations. Science 198:501-503.
Anderson J.G., Grassl H.J., Shetter R.E., Margitan J.J. (1980) Stratospheric free chlorine measured by balloon-borne in situ resonance fluorescence. Journal of Geophysical Research 85:2869-2887.
Berg W.W., Crutzen P.J., Grahek F.E., Gitlen S.N., Sedlacek W.A. (1980) First measurements of total chlorine and bromine in the lower stratosphere. Geophysical Research Letters 7:937-940.
Bischof W., Borchers R., Fabian P., Küger B.C. (1985) Increased concentration and vertical distribution of carbon dioxide in the stratosphere. Nature 316:708-710.
Brown A., McKean D.C., Duncan J.L. (1988) Vibrational anharmonicity and Fermi resonances in CHF2Cl. Spectrochim. Acta 44:553-565.
Brown L.R., Farmer C.B., Rinsland C.P., Toth R.A. (1987) Molecular line parameters for the atmospheric trace molecule spectroscopy experiment. Appl. Opt. 26:5154-5182.
Brown L.R., Cohen E.A..
Chance K.V., Johnson D.G., Traub W.A. (1989) Measurement of stratospheric HOCl: concentration profiles, including diurnal variation. Journal of Geophysical Research 94:11059-11069.
Cicerone R.J., Stolarski R.S., Walters S. (1974) Stratospheric ozone destruction by man-made chlorofluoromethanes. Science 185:1165-1167.
Cicerone R.J. (1981) Halogens in the atmosphere. Rev. Geophys. Space Phys. 19:123-139.
Crutzen P.J., Isaksen I.S.A., McAfee J.R. (1978) The impact of chlorocarbon industry on the ozone layer. J. Geophys. Res. 83:345-363.
Fabian P., Borchers R., Flentje G., Matthews W.A., Seiler W., Giehl H., Bunse K., Müller F., Schmidt U., Volz A., Khedim A., Johnen F.J. (1981) The vertical distribution of stable trace gases at mid-latitudes. J. Geophys. Res. 86:5179-5184.
Fabian P. (1986) Halogenated hydrocarbons in the atmosphere. Handbook of Environmental Chemistry , O., Hutzinger, Springer-Verlag, New York; 23-51.
Fabian P., Borchers R., Krüger B.C., Lal S. (1987) CF4 and C2F6 in the atmosphere. Journal of Geophysical Research 92:9831-9835.
Farmer C.B. (1987) High resolution infrared spectroscopy of the sun and the earth's atmosphere from space. Mikrochim. Acta [Wien] 3:189-214.
Farmer C.B., Raper O.F., O'Callaghan F.G. Final report on the first flight of the ATMOS instrument during the Spacelab 3 mission, 29 April through 6 May 1985, JPL Publication 87-32, Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California; 1987.
Gallagher C.C., Forsberg C.A., Mason A.S., Gandrud B.W., Janhorbani M. (1985) Total chlorine content in the lower stratosphere. J. Geophys. Res. 90:10747-10752.
Gunson M.R., Farmer C.B., Norton R.H., Zander R., Rinsland C.P., Shaw J.H., Gao B.-C. (1990) Measurements of CH4, N2O, CO, H2O, and O3 in the middle atmosphere by the Atmospheric Trace Molecule Spectroscopy Experiment on Spacelab 3. Journal of Geophysical Research 95:13867-13882.
Heidt L.E., Vedder J.F., Pollock W.H., Lueb R.A., Henry B.E. (1989) Trace gases in the Antarctic atmosphere. Journal of Geophysical Research 94:11599-11611.
Kaye J.A., Douglas A.R., Jackman C.H., Stolarski R.S., Zander R., Roland G. (1991) Two-dimensional model calculation of fluorine-containing reservoir species in the stratosphere. Journal of Geophysical Research 96:12865-12881.
Ko M.K.W., Sze N.D. (1984) Diurnal variation of ClO: implications for the stratospheric chemistries of ClONO2, HOCl, and HCl. J. Geophys. Res. 89:11619-11632.
Lazrus A.L., Gandrud B.W., Greenberg J., Bonelli J., oz E., Sedlacek W.A. (1977) Midlatitude seasonal measurements of stratospheric acidic chlorine vapor. Geophysical Research Letters 4:587-589.
Mankin W.G., Coffey M.T. (1983) Latitudinal distributions and temporal changes of stratospheric HCl and HF. J. Geophys. Res. 88:10776-10784.
McDaniel A.H., Cantrell C.A., Davidson J.A., Shetter R.E., Calvert J.A. (1991) The temperature dependent absorption cross sections for the chlorofluorocarbons: CFC-11, CFC-12, CFC-13, CFC-14, CFC-22, CFC-113, CFC-114, and CFC-115. J. Atmos. Chem. 12:211-227.
Molina M.J., Rowland F.S. (1974) Stratospheric sink for chlorofluoromethanes: chlorine atomcatalysed destruction of ozone. Nature 249:810-812.
oz E.J., Lazrus A.L., Bonelli J.E. (1977) Direct measurements of stratospheric fluoride. Geophys. Res. Lett. 4:149-150.
Norton R.H., Rinsland C.P. (1991) ATMOS data processing and science analysis methods. Applied Optics 30:389-400.
Park J.H., Zander R., Farmer C.B., Rinsland C.P., Russell J.M., Norton R.H., Raper O.F. (1986) Spectroscopic detection of CH3Cl in the upper troposphere and lower stratosphere. Geophysical Research Letters 13:765-768.
Prather M.J., Watson R.T. (1990) Stratospheric ozone depletion and future levels of atmospheric chlorine and bromine. Nature 344:729-734.
Prinn R.G. (1988) How have the atmospheric concentrations of the halocarbons changed?. The Changing Atmosphere , F. S., Rowland, I. S. A., Isaksen, Wiley, New York; 33-48.
Raper O.F., Farmer C.B., Zander R., Park J.H. (1987) Infrared spectroscopic measurements of halogenated sink and reservoir gases in the stratosphere with the ATMOS instrument. Journal of Geophysical Research 92:9851-9858.
Rinsland C.P., Zander R., Brown L.R., Farmer C.B., Park J.H., Norton R.H., Russell J.M., Raper O.F. (1986) Detection of carbonyl fluoride in the stratosphere. Geophysical Research Letters 13:769-772.
Rinsland C.P., Brown L.R., Farmer C.B. (1990) Infrared spectroscopic detection of sulfur hexafluoride (SF6) in the lower stratosphere and upper troposphere. J. Geophys. Res. 95:5577-5585.
Rinsland C.P., Levine J.S., Goldman A., Sze N.D., Ko M.K.W., Johnson D.W. (1991) Infrared measurements of HF and HCl total column abundances above Kitt Peak, 1977–1990: seasonal cycles, long-term increases, and comparison with model calculations. Journal of Geophysical Research 96:15523-15540.
Russell J.M., Farmer C.B., Rinsland C.P., Zander R., Froidevaux L., Toon G.C., Gao B., Shaw J., Gunson M. (1988) Measurements of odd nitrogen compounds in the stratosphere by the ATMOS experiment on Spacelab 3. J. Geophys. Res. 93:1718-1736.
.
.
Schmidt U., Khedim A. (1991) In situ measurements of carbon dioxide in the winter Arctic vortex and at midlatitudes: an indicator of the ‘age’ of the stratosphere. Geophys. Res. Lett. 18:763-766.
Stolarski R.S., Rundel R.D. (1975) Fluorine photochemistry in the stratosphere. Geophysical Research Letters 2:443-444.
Symonds R.B., Rose W.I., Reed M.H. (1978) Contribution of Cl- and F-bearing gases to the atmosphere by volcanoes. Nature 344:415-418.
Sze N.D. (1978) Stratospheric fluorine: a comparison. Geophysical Research Letters 5:781-783.
Toon G.C., Farmer C.B. (1989) Detection of HOCl in the Antarctic stratosphere. Geophys. Res. Lett. 16:1375-1377.
Wallace L., Livingston W. (1991) Spectroscopic observations of atmospheric trace gases over Kitt Peak. 3. The long-term trends of hydrogen chloride and hydrogen fluoride from 1978 to 1990. Journal of Geophysical Research 96:15513-15521.
Waters J.W., Stachnik R.A., Hardy J.C., Jarnot R.F. (1988) ClO and O3 stratospheric pro balloon microwave measurements. Geophys. Res. Lett. 15:780-783.
Watson R.T., Smokler P.E., DeMore W.B. An assessment of an F2 or N2O4 atmospheric injection from an aborted space shuttle mission, JPL Publication 77-81, Jet Propulsion Laboratory, California Institute of Technology, Pasadena, Calif.; 1978.
Wilson S..
.
Report No. 18, Report of the International Ozone Trends Panel 1988, WMO, World Meteorological Organization, Geneva, Switzerland; 1990.
Report No. 20, Scientific Assessment of Stratospheric Ozone: 1989, WMO, World Meteorological Organization, Geneva, Switzerland; 1990.
Zander R., Rinsland C.P., Farmer C.B., Brown L.R., Norton R.H. (1986) Observation of several chlorine nitrate (ClONO2) bands in stratospheric infrared spectra. Geophysical Research Letters 13:757-761.
Zander R., Rinsland C.P., Farmer C.B., Norton R.H. (1987) Infrared spectroscopic measurements of halogenated source gases in the stratosphere with the ATMOS instrument. J. Geophys. Res. 92:9836-9850.
Zander R., Roland G., Delbouille L., Sauval A., Farmer C.B., Norton R.H. (1987) Monitoring of the integrated column of hydrogen fluoride above the Jungfraujoch station since 1977 — the HF/HCl column ratio. J. Atmos. Chem. 5:385-394.
Zander R., Gunson M.R., Foster J.C., Rinsland C.P., Namkung J. (1990) Stratospheric ClONO2, HCl, and HF concentration profiles derived from ATMOS/Spacelab 3 observations — An update. Journal of Geophysical Research 95:20519-20525.
