[en] BUDGETS OF CHLORINE AND FLUORINE ; HALOGENATED GASES ; SPECTROSCOPIC OBSERVATIONS ; atmospheric composition ; remote sensing ; Montreal Protocol ; ATMOS ; stratosphere
[en] The set of high-resolution infrared solar observations made with the Atmospheric Trace Molecule Spectroscopy (ATMOS) - Fourier transform spectrometer from onboard Spacelab 3 (30 April-1 May 1985) has been used to evaluate the total budgets of the odd chlorine and fluorine chemical families in the stratosphere. These budgets are based on volume mixing ratio profiles measured for HCl, HF, CH3Cl, ClONO2, CCl4, CCl2F2, CCl3F, CHClF2, CF4, COF2, and SF6, near 30-degrees north latitude. When including realistic concentrations for species not measured by ATMOS, i.e., the source gases CH3CCl3, and C2F3Cl3 below 25 km, and the reservoirs ClO, HOCl and COFCl between 15 and 40 km (five gases actually measured by other techniques), the 30-degrees-N zonal 1985 mean total mixing ratio of chlorine, Cl, was found to be equal to (2.58 +/- 0.10) ppbv (parts per billion by volume) throughout the stratosphere, with no significant decrease near the stratopause. The results for total fluorine indicate a slight, but steady, decrease of its volume mixing ratio with increasing altitude, around a mean stratospheric value of (1.15 +/- 0.12) ppbv. Both uncertainties correspond to one standard deviation. These mean springtime 1985 stratospheric budgets are commensurate with values reported for the tropospheric Cl and F concentrations in the early 1980s, when allowance is made for the growth rates of their source gases at the ground and the time required for tropospheric air to be transported into the stratosphere. The results are discussed with emphasis on conservation of fluorine and chlorine and the partitioning among source, sink, and reservoir gases throughout the stratosphere.