1Department of Physics, University of York, Heslington, YO10 5DD, UK
2Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
3Department of Chemistry, University of Waterloo, Waterloo, Ontario, Canada
4Department of Chemistry and Biochemistry, Old Dominion University, Virginia, USA
5Department of Chemistry, University of York, Heslington, YO10 5DD, UK
Received: 04 Apr 2013 – Published in Atmos. Chem. Phys. Discuss.: 25 Jun 2013
Abstract. Fluorine-containing species can be extremely effective atmospheric greenhouse gases. We present fluorine budgets using organic and inorganic species retrieved by the ACE-FTS satellite instrument supplemented with output from the SLIMCAT 3-D chemical transport model. The budgets are calculated between 2004 and 2009 for a number of latitude bands: 70–30° N, 30–00° N, 00° N–30° S, and 30–70° S. At lower altitudes total fluorine profiles are dominated by the contribution from CFC-12, up to an altitude of 20 km in the extra-tropics and 29 km in the tropics; above these altitudes the profiles are dominated by hydrogen fluoride (HF). Our data show that total fluorine profiles at all locations have a negative slope with altitude, providing evidence that overall fluorine emissions (measured by their F content) have been increasing with time. Total stratospheric fluorine is increasing at a similar rate in the tropics: 32.5 ± 4.9 ppt yr−1 (1.31 ± 0.20% per year) in the Northern Hemisphere (NH) and 29.8 ± 5.3 ppt yr−1 (1.21 ± 0.22% per year) in the Southern Hemisphere (SH). Extra-tropical total stratospheric fluorine is also increasing at a similar rate in both the NH and SH: 28.3 ± 2.7 ppt per year (1.12 ± 0.11% per year) in the NH and 24.3 ± 3.1 ppt per year (0.96 ± 0.12% per year) in the SH. The calculation of radiative efficiency-weighted total fluorine allows the changes in radiative forcing between 2004 and 2009 to be calculated. These results show an increase in radiative forcing of between 0.23 ± 0.11% per year and 0.45 ± 0.11% per year, due to the increase in fluorine-containing species during this time. The decreasing trends in the mixing ratios of halons and chlorofluorocarbons (CFCs), due to their prohibition under the Montreal Protocol, have suppressed an increase in total fluorine caused by increasing mixing ratios of hydrofluorocarbons (HFCs). This has reduced the impact of fluorine-containing species on global warming.
Revised: 07 Nov 2013 – Accepted: 15 Nov 2013 – Published: 09 Jan 2014
Brown, A. T., Chipperfield, M. P., Richards, N. A. D., Boone, C., and Bernath, P. F.: Global stratospheric fluorine inventory for 2004–2009 from Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements and SLIMCAT model simulations, Atmos. Chem. Phys., 14, 267-282, doi:10.5194/acp-14-267-2014, 2014.