[en] Total fluorine (FTOT) in the stratosphere has been determined using Atmospheric
Chemistry Experiment Fourier transform spectrometer (ACE-FTS) measurements of HF,
COF2, COClF, CF4, CCl3F (CFC-11), CCl2F2 (CFC-12), CHClF2 (HCFC-22),
CCl2FCClF2 (CFC-113), CH3CClF2 (HCFC-142b), CH2FCF3 (HFC-134a), and SF6. The
retrieval of HFC-134a (CH2FCF3) from spaceborne measurements had not been carried
out prior to this work. Measurements of these species have been supplemented by data
from models to extend the altitude range of the profiles and have also been complemented
by estimates of 15 minor fluorine species. Using these data, separate fluorine budgets were
determined in five latitude zones (60°–82°N, 30°–60°N, 30°S–30°N, 30°–60°S, and
60°–82°S) by averaging over the period of February 2004 to January 2005 inclusive,
when possible. Stratospheric FTOT profiles in each latitude zone are nearly linear, with
mean stratospheric FTOT values ranging from 2.50 to 2.59 ppbv (with a 1sig precision of
0.04–0.07 ppbv and an estimated accuracy of 0.15 ppbv) for each zone. The highest mean
FTOT value occurred in the tropics, which is qualitatively consistent with increasing levels
of stratospheric fluorine and the mean stratospheric circulation pattern.
Disciplines :
Earth sciences & physical geography
Author, co-author :
Nassar, Ray; University of Waterloo > Department of Chemistry
Bernath, Peter F.; University of Waterloo (Ontario, Canada) > Department of Chemistry
Boone, Christopher D.; University of Waterloo (Ontario, Canada) > Department of Chemistry
Mc Leod, Sean; University of Waterloo (Ontario, Canada) > Department of Chemistry
Skelton, Randall; University of Waterloo (Ontario, Canada) > Department of Chemistry
Walker, Kaley; University of Waterloo (Ontario, Canada > Department of Chemistry
Rinsland, Curtis P.; NASA Langley Research Center (Virginia, USA)
Duchatelet, Pierre ; Université de Liège - ULiège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Language :
English
Title :
A global inventory of stratospheric fluorine in 2004 based on Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements
Publication date :
30 November 2006
Journal title :
Journal of Geophysical Research
ISSN :
0148-0227
eISSN :
2156-2202
Publisher :
American Geophysical Union, Washington, United States - District of Columbia
Anderson, J., and J. M. Russell III (2004), Long term changes of HCl and HF as observed by HALOE, in Ozone, vol. II, Proceedings of the XX Quadrennial Ozone Symposium, Kos, Greece, 1-8 June 2004, edited by C. S. Zerefos, pp. 223-224, Univ. of Athens, Athens.
Anderson, J., J. M. Russell III, S. Solomon, and L. E. Deaver (2000), Halogen Occultation Experiment confirmation of stratospheric chlorine decreases in accordance with the Montreal Protocol, J. Geophys. Res., 105, 4483-4490.
Bernath, P. F., et al. (2005), Atmospheric Chemistry Experiment (ACE): Mission overview, Geophys. Res. Lett., 32, L15S01, doi:10.1029/ 2005GL022386.
Boone, C. D., R. Nassar, K. A. Walker, Y. Rochon, S. D. McLeod, C. P. Rinsland, and P. F. Bernath (2005), Retrievals for the Atmospheric Chemistry Experiment Fourier transform spectrometer, Appl. Opt., 44, 7218-7231.
Brown, L. R., et al. (1987), Molecular line parameters for the atmospheric trace molecule spectroscopy experiment, Appl. Opt., 26, 5154-5182.
Brown, L. R., et al. (1996), The 1995 Atmospheric Trace Molecule Spectroscopy (ATMOS) linelist, Appl. Opt., 35, 2828-2848.
Burgess, A. B., R. G. Grainger, A. Dudhia, V. H. Payne, and V. L. Jay (2004), MIPAS measurement of sulfur hexafluoride (SF6), Geophys. Res. Lett., 31, L05112, doi:10.1029/2003GL019143.
Burgess, A. B., R. G. Grainger, and A. Dudhia (2006), Zonal mean atmospheric distribution of sulfur hexafluoride (SF6), Geophys. Res. Lett., 33, L07809, doi:10.1029/2005GL025410.
Clerbaux, C., R. Colin, P. C. Simon, and C. Granier (1993), Infrared cross sections and global warming potentials of 10 alternative hydrohalocarbons, J. Geophys. Res., 98(D6), 10,491-10,497.
Coheur, P. F., C. Clerbaux, and R. Colin (2003), Spectroscopic measurements of halocarbons and hydrohalocarbons by satellite-borne remote sensors, J. Geophys. Res., 108(D4), 4130, doi:10.1029/ 2002JD002649.
Dufour, G., C. D. Boone, and P. F. Bernath (2005), First measurements of CFC-113 and HCFC-142b from space using ACE-FTS infrared spectra, Geophys. Res. Lett., 32, L15S09, doi:10.1029/2005GL022422.
Kaye, J. A., A. R. Douglass, C. H. Jackman, R. S. Stolarski, R. Zander, and G. Roland (1991), Two-dimensional model calculation of fluorine-containing reservoir species in the stratosphere, J. Geophys. Res., 96, 12,865-12,881.
McHugh, M., B. Magill, K. A. Walker, C. D. Boone, P. F. Bernath, and J. M. Russell III (2005), Comparison of atmospheric retrievals from ACE and HALOE, Geophys. Res. Lett., 32, L15S10, doi:10.1029/2005GL022403.
Morris, R. A., et al. (1995), Effects of electron and ion reactions on atmospheric lifetimes of fully fluorinated compounds, J. Geophys. Res., 100(D1), 1287-1294.
Nassar, R., P. F. Bernath, C. D. Boone, G. L. Manney, S. D. McLeod, C. P. Rinsland, R. Skelton, and K. A. Walker (2005), ACE-FTS measurements across the edge of the winter 2004 Arctic vortex, Geophys. Res. Lett., 32, L15S05, doi:10.1029/2005GL022671.
Nassar, R., et al. (2006), A global inventory of stratospheric chlorine in 2004, J. Geophys. Res., doi:10.1029/2006JD007073, in press.
Nemtchinov, V., and P. Varanasi (2004), Absorption cross-sections of HFC-134a in the spectral region between 7 and 12 μm, J. Quant. Spectros. Radiat. Transfer, 83, 285-294, doi:10.1016/ S0022-4073(02)00356-4.
Neu, J. L., and R. A. Plumb (1999), Age of air in a "leaky pipe" model of stratospheric transport, J. Geophys. Res., 104, 19,243-19,255.
Patra, K. P., S. Lal, B. H. Subbaraya, C. H. Jackman, and P. Rajaratnam (1997), Observed vertical profile of sulphur hexafluoride (SF6) and its atmospheric applications, J. Geophys. Res., 102, 8855-8859.
Ravishankara, A. R., S. Solomon, A. A. Turnipseed, and R. F. Warren (1993), Atmospheric lifetimes of long-lived halogenated species, Science, 259, 194-199.
Rinsland, C. P., C. Boone, R. Nassar, K. Walker, P. Bernath, E. Mahieu, R. Zander, J. C. McConnell, and L. Chiou (2005), Trends of HF, HCl, CCl2F2, CCl3F, CHClF2,(HCFC-22), and SF6 in the lower stratosphere from Atmospheric Chemistry Experiment (ACE) and Atmospheric Trace Molecule Spectroscopy (ATMOS) measurements near 30°N latitude, Geophys. Res. Lett., 32, L16S03, doi:10.1029/2005GL022415.
Rinsland, C. P., E. Mahieu, R. Zander, R. Nassar, P. Bernath, C. Boone, and L. S. Chiou (2006a), Long-term stratospheric carbon tetrafluoride (CF4) increase inferred from 1985-2004 infrared space-based solar occultation measurements, Geophys. Res. Lett., 33, L02808, doi:10.1029/2005GL024709.
Rinsland, C. P., et al. (2006b), Spectroscopic detection of COCIF in the tropical and mid-latitude lower stratospere, J. Quant. Spectrosc. Radiat Transfer, in press.
Rothman, L. S., et al. (2005), The HITRAN 2004 molecular spectroscopic database, J. Quant. Spectros. Radiat. Transfer, 96, 139-204.
Rummukainen, M. (1996), Modeling stratospheric chemistry in a global three- dimensional chemical transport model, SCTM-1: Model development, Finn. Meteorol. Inst. Contrib., 19, 206 pp.
Russell, J. M., III, et al. (1996), Validation of hydrogen fluoride measurements made by the Halogen Occultation Experiment from the UARS platform, J. Geophys. Res., 101, 10,163-10,174.
Sen, B., G. C. Toon, J-F. Blavier, E. L. Fleming, and C. H. Jackman (1996), Balloon-borne observations of midlatitude fluorine abundance, J. Geophys. Res., 101, 9045-9054.
Stolarski, R. S., and R. D. Rundel (1975), Fluorine photochemistry in the stratosphere, Geophys. Res. Lett., 22, 385-388.
Tuazon, E. C., and R. Atkinson (1993), Tropospheric transformation products of a series of hydroflurocarbons and hydrochlorofluorocarbons, J. Atmos. Chem., 17, 179-199.
Weisenstein, D. K., M. K. W. Ko, and N.-D. Sze (1992), The chlorine budget of the present-day atmosphere: A modeling study, J. Geophys. Res., 97, 2547-2559.
World Meteorological Organization (2003), Scientific assessment of ozone depletion: 2002, Global Ozone Res. Monitor. Proj. Rep. 47, Geneva, Switzerland.
Zander, R., M. R. Gunson, C. B. Farmer, C. P. Rinsland, F. W. Irion, and E. Mahieu (1992), The 1985 chlorine and fluorine inventories in the stratosphere based on ATMOS observations at 30° north latitude, J. Atmos. Chem., 15, 171-186.
Zander, R., et al. (1996), The 1994 northern mid-latitude budget of stratospheric chlorine derived from ATMOS/ATLAS-3 observations, Geophys. Res. Lett., 23, 2357-2360.