H2SO4 photolysis: A source of sulfur dioxide in the upper stratosphere

Numerous absorption lines of stratospheric sulfur dioxide (SO{sub 2}) have been identified in solar occultation spectra recorded by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the Atmospheric Laboratory for Applications and Science (ATLAS)-1 shuttle mission (March 24-April 2, 1992). Based on their analysis, a volume mixing ratio profile of SO{sub 2} increasing from (13 {plus_minus}4) p.p.t.v. (parts per 10{sup {minus}12} by volume) at 16 mbar ({approximately} 28 km) to 455 {plus_minus}90 p.p.t.v. at 0.63 mbar ({approximately} 52 km) has been measured with no significant profile differences between 20{degrees}N and 60{degrees}S latitude. The increase in the SO{sub 2} mixing ratios with altitude indicates the presence of a source of SO{sub 2} in the upper stratosphere. Profiles retrieved from ATMOS spectra recorded during shuttle flights in April-May 1985 and April 1993 show similar vertical distributions but lower concentrations. Two-dimensional model calculations with SO{sub 2} assumed as the end product of H{sub 2}SO{sub 4} photolysis produce SO{sub 2} profiles consistent with the ATMOS measurements to within about a factor of 2. 27 refs., 2 figs.

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