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Abstract :
[fr] Fluorine enters the stratosphere principally in the form of CFCs (chlorofluorocarbons, mainly CFC-12 and CFC-11), HCFCs (hydrochlorofluorocarbons, mainly HCFC-22) and HFCs (hydrofluorocarbons, mainly HFC-134a) which have been (or are still) widely emitted at ground level by human activities. In the lower stratosphere, the photolysis of these halogenated source gases leads to the formation of the two fluorine reservoirs COClF and COF2. The subsequent photolysis of these two compounds frees F atoms, which principally react with CH4 and H2O to form the extremely stable HF gas, by far the dominant fluorine reservoir in the middle and upper stratosphere.
Despite the fact that fluorine does not significantly contribute in stratospheric ozone depletion, measurements of the concentrations of individual F-containing species in different altitude ranges of the atmosphere are important as they reflect the amounts of anthropogenic gases transported into the middle atmosphere as well as their decomposition. Such measurements also provide insight into the partitioning between major fluorine source gases (which are potent greenhouse gases) and reservoirs and allows a global inventory of organic (CFy), inorganic (Fy) and total (FTOT) fluorine burdens to be monitored as a function of time. Indeed, regular updates of such inventories are important as the partitioning between F-containing gases in the stratosphere is continually evolving as emissions of anthropogenic gases from the surface change, principally as a consequence of the progressive ban on the production of CFCs and HCFCs adopted by the Montreal Protocol and its subsequent Amendments and Adjustments.
To complement recent studies regarding fluorine species (Duchatelet et al., 2009, 2010, 2011; Mahieu et al., 2011), this communication presents the time series of the inorganic fluorine budget Fy over the last twenty-five years, based on HF and COF2 total column amounts derived from high resolution Fourier transform infrared (FTIR) solar spectra recorded at Jungfraujoch (46.5°N, 8.0°E, 3580m asl). A trend analysis of our HF, COF2 and Fy time series is performed and discussed in the context of past and current emissions of halogenated source gases. Comparisons with model and space data are also included.