Articles | Volume 14, issue 21
Atmos. Chem. Phys., 14, 11915–11933, 2014
Atmos. Chem. Phys., 14, 11915–11933, 2014

Research article 13 Nov 2014

Research article | 13 Nov 2014

Satellite observations of stratospheric carbonyl fluoride

J. J. Harrison*,1, M. P. Chipperfield2, A. Dudhia3, S. Cai3, S. Dhomse2, C. D. Boone4, and P. F. Bernath5,1 J. J. Harrison et al.
  • 1Department of Chemistry, University of York, Heslington, York, YO10 5DD, UK
  • 2Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
  • 3Atmospheric, Oceanic and Planetary Physics, Clarendon Laboratory, University of Oxford, Parks Road, Oxford, OX1 3PU, UK
  • 4Department of Chemistry, University of Waterloo, 200 University Avenue West, Ontario N2L 3G1, Canada
  • 5Department of Chemistry and Biochemistry, Old Dominion University, Norfolk, Virginia 23529, USA
  • *now at: Space Research Centre, Michael Atiyah Building, Department of Physics and Astronomy, University of Leicester, University Road, Leicester, LE1 7RH, UK

Abstract. The vast majority of emissions of fluorine-containing molecules are anthropogenic in nature, e.g. chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs). These molecules slowly degrade in the atmosphere, leading to the formation of HF, COF2, and COClF, which are the main fluorine-containing species in the stratosphere. Ultimately both COF2 and COClF further degrade to form HF, an almost permanent reservoir of stratospheric fluorine due to its extreme stability. Carbonyl fluoride (COF2) is the second-most abundant stratospheric "inorganic" fluorine reservoir, with main sources being the atmospheric degradation of CFC-12 (CCl2F2), HCFC-22 (CHF2Cl), and CFC-113 (CF2ClCFCl2).

This work reports the first global distributions of carbonyl fluoride in the Earth's atmosphere using infrared satellite remote-sensing measurements by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS), which has been recording atmospheric spectra since 2004, and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, which recorded thermal emission atmospheric spectra between 2002 and 2012. The observations reveal a high degree of seasonal and latitudinal variability over the course of a year. These have been compared with the output of SLIMCAT, a state-of-the-art three-dimensional chemical transport model. In general the observations agree well with each other, although MIPAS is biased high by as much as ~30%, and compare well with SLIMCAT.

Between January 2004 and September 2010 COF2 grew most rapidly at altitudes above ~25 km in the southern latitudes and at altitudes below ~25 km in the northern latitudes, whereas it declined most rapidly in the tropics. These variations are attributed to changes in stratospheric dynamics over the observation period. The overall COF2 global trend over this period is calculated as 0.85 ± 0.34 (MIPAS), 0.30 ± 0.44 (ACE), and 0.88% year−1 (SLIMCAT).

Final-revised paper