Atmos. Chem. Phys. Discuss., 13, 4221-4287, 2013
www.atmos-chem-phys-discuss.net/13/4221/2013/
doi:10.5194/acpd-13-4221-2013
© Author(s) 2013. This work is distributed
under the Creative Commons Attribution 3.0 License.
Review Status
This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O from measurements made by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS)
A. T. Brown1, C. M. Volk2, M. R. Schoeberl3, C. D. Boone4, and P. F. Bernath5,6
1Department of Physics, University of York, Heslington, YO10 5DD, UK
2Department of Physics, University of Wuppertal, 42119 Wuppertal, Germany
3Science and Technology Corporation, Lanham, MD 20706, USA
4Department of Chemistry, University of Waterloo, Ontario, Canada
5Department of Chemistry and Biochemistry, Old Dominion University, VA, USA
6Department of Chemistry, University of York, Heslington, YO10 5DD, UK

Abstract. Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer-tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the VMR from tropical ground-based AGAGE sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 195 + (−) 75 (42) yr (CH4), 69 + (−) 65 (23) yr (CH3Cl) and 123 + (−) 53 (28) yr (N2O). The errors on these values are the weighted 1-σ non-systematic errors. The stratospheric lifetime of CH3Cl represents the first calculations of the stratospheric lifetime of CH3Cl using data from a space based instrument.

Citation: Brown, A. T., Volk, C. M., Schoeberl, M. R., Boone, C. D., and Bernath, P. F.: Stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O from measurements made by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), Atmos. Chem. Phys. Discuss., 13, 4221-4287, doi:10.5194/acpd-13-4221-2013, 2013.
 
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