ALBERT

Description: Vertical mixing ratio profiles of four relatively long-lives gases, HCN, C2H2, CO, and C2H6, have been retrieved from 0.01/cm resolution infrared solar occultation spectra recorded between latitudes of 5.3degN and 31.4degN. The observations were obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the Atmospheric Laboratory for Applications and Science (ATLAS) 3 shuttle flight, 3-12 November 1994. Elevated mixing ratios below the tropopause were measured for these gases during several of the occultations. The positive correlations obtained between the simultaneously measured mixing ratios suggest that the enhancements are likely the result of surface emissions, most likely biomass burning and/or urban industrial activities, followed by common injection via deep convective transport of the gases to the upper troposphere. The elevated levels of HCN may account for at least part of the "missing NO," in the upper troposphere. Comparisons of the observations with values measured during a recent aircraft campaign are presented.

Description: Infrared solar spectra recorded at the International Scientific Station of the Jungfraujoch (3580 m altitude), Switzerland, in 1950-1951 and from 1984 to 1992 have been analyzed to determine vertical column abundances of nitrous oxide (N2O) above the station. The best fit to the relatively dense set of measurements made between 1984 and 1992 indicates a mean exponential rate of increase equal to 0.36 +/- 0.06%/yr (1 sigma) and a seasonal modulation of 7.2% peak to peak, the minimum occurring at the end of the winter and the maximum in early September. The column abundances for April of the years 1951, 1984, and 1992 were found equal to 3.49 x 10(exp 18), 3.76 x 10(exp 18), and 3.87 x 10(exp 18) molecules/sq cm, respectively; they translate into N2O concentrations at the altitude of the Jungfraujoch equal to 275, 296, and 305 parts per billion by volume. These results indicate that the exponential rate of increase for 1951-1984 was equal to 0.23 +/- 0.04%/yr (1 sigma), thus substantially lower than for the 1984-1992 time interval and that the so-called preindustrial levels of N2O pertained until 1951 with most of the increase in atmospheric N2O occurring thereafter.

Description: Volume mixing ratio profiles of COF2 have been derived through most of the stratosphere between 30 deg N and 54 deg S from series of 0.01-/cm resolution infrared solar spectra recorded in the occultation mode by the atmospheric trace molecule spectroscopy (ATMOS) instrument during the ATLAS 1 space shuttle mission of March-April 1992. When compared with similar results obtained from the ATMOS/Spacelab 3 mission of April-May 1985, the cumulative increase in the burden of COF2 in the middle and upper stratosphere was found to be 67% for that 7-year time interval. By combining a subset of these COF2 results with upper stratospheric concentrations of HF also derived from the ATMOS observations, it was further found that the budget of inorganic fluorine above 35 km altitude increased by (60 +/- 10)% over the 1985-1992 time interval, which corresponds to an average exponential rate of increase of (6.7 +/- 1/1)%/yr, or a linear rate of increase reference to 1985 of (8.5 +/- 1.3)%/yr at the 1 sigma confidence level. The total inorganic F atom volume mixing ratio found in the upper stratosphere for 1985 and 1992 and the increase during this perid mirror the rise in man-made fluorine-bearing compounds at the ground during the early to mid 1980s. This demonstrates the negligible impact of natural sources of fluorine, in particular volcanic activity, on the observed change in F in the upper stratosphere. Implications of the present findings and comparison with model results are discussed.

Description: Vertical profiles of sulfur hexafluoride (SF6) in the lower stratosphere and upper troposphere have been retrieved from 0.01/cm resolution infrared solar occultation spectra recorded by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the ATLAS (Atmospheric Laboratory for Applications and Science) 1 shuttle mission of March 24 to April 2, 1992. Based on measurements of the unresolved absorption by the SF6 mu(sub 3) band Q branch at 947.9/cm, average SF6 volume mixing ratios and 1-sigma uncertainties of 3.20 +/- 0.54 parts per trillion by volume (pptv; 10(exp -12) ppv) at 200 mbar (approximately 11.8 km) declining to 2.86 +/- 0.29 pptv at 100 mbar (approximately 16.2 km) and 1.95 +/- 0.50 pptv at 30 mbar (approximately 23.9 km) have been retrieved. The profiles show no obvious dependence with latitude over the range of the measurements (eight occultations spanning 28 deg S to 54 deg S). Assuming an exponential growth model and applying a correction for the interhemispheric concentration difference, an average SF6 rate of increase of 8.7 +/- 2.2% per year, 2 sigma, between 12 and 18 km has been derived by fitting the present measurements, ATMOS measurements from the April-May 1985 Spacelab 3 mission, and balloon-borne IR measurements obtained in March 1981 and June 1988.

Description: Simultaneous stratospheric volume mixing ration (VMR) profiles of dinitrogen pentoxide (N2O5) and nitric acid (HNO3) at sunrise between 25 deg N and 15 deg S latitude and profiles of HNO3 at sunset between 42 deg S and 53 deg S latitude have been derived from 0.01/cm resolution infrared solar occultation spectra recorded 9.5 months after the massive eruption of the Mount Pinatubo volcano in the Philippine Islands. The measurements were obtained by the atmospheric trace molecule spectroscopy (ATMOS) Fourier transform spectrometer during the ATLAS 1 shuttle mission (March 24 to April 2, 1992). The measured HNO3 VMRs are higher at all altitudes and latitudes than corresponding values measured by the limb infrared monitor of the stratosphere (LIMS) instrument during the same season in 1979, when the aerosol loading was near background levels. The largest relative increase in the HNO3 VMR occurred near the equator at 30-km altitude, where the ATMOS/ATLAS 1 values are about a factor of 2 higher than the LIMS measurements. Two-dimensional model calculations show that the increase in HNO3 and the ATMOS/ATLAS 1 measurement of a steep decrease in the N2O5 VMR below 30 km can be explained by the enhanced conversion of N2O5 to HNO3 on the surfaces of the Mount Pinatubo sulfate aerosols. Our profile results demonstrate the global impact of the N2O5 + H2O yields 2HNO3 heterogeneous reaction in altering the partitioning of stratospheric odd nitrogen after a major volcanic eruption.

Description: Series of high-resolution infrared solar spectra recorded at the International Scientific Station of the Jungfraujoch, Switzerland, between 06/1986 and 11/1992, and at Kitt Peak National Observatory, Tucson, Arizona (U.S.A.), from 12/1980 to 04/1992, have been analyzed to provide a comprehensive ensemble of vertical column abundances of CHClF2 (HCFC-22; Freon-22) above the European and the North American continents. The columns were derived from nonlinear least-squares curve fittings between synthetic spectra and the observations containing the unresolved 2 nu(sub 6) Q-branch absorption of CHClF2 at 829.05/cm. The changes versus time observed in these columns were modeled assuming both an exponential and a linear increase with time. The exponential rates of increase at one-sigma uncertainties were found equal to (7.0 +/- 0.35)%/yr for the Junfraujoch data and (7.0 +/- 0.23)%/yr for the Kitt Peak data. The exponential trend of 7.0%/yr found at both stations widely separated in location can be considered as representative of the global increase of the CHClF2 burden in the Earth's atmosphere during the period 1980 to 1992. When assuming two realistic vertical volume mixing ratio profiles for CHClF2 in the troposphere, one quasi constant and the other decreasing by about 13% from the ground to the tropopause, the concentrations for mid-1990 were found to lie between 97 and 111 pptv (parts per trillion by volume) at the 3.58 km altitude of the Jungfraujoch and between 97 and 103 pptv at Kitt Peak, 2.09 km above sea level. Corresponding values derived from calculations using a high vertical resolution-2D model and recently compiled HCFC-22 releases to the atmosphere, were equal to 107 and 105 pptv, respectively, in excellent agreement with the measurements. The model calculated lifetime of CHClF2 was found equal to 15.6 years. The present results are compared critically with similar data found in the literature. On average, the concentrations found here are lower by 15-20% than those derived from in situ investigations; this difference cannot be explained by the absolute uncertainty of +/- 11% assigned presently to the infrared remote measurements.

Description: Results are presented of an investigation of the Cl and F inventories derived from the concentrations of eleven Cl- and F-bearing organic and inorganic species throughout the atmosphere, based on observations with the Atmospheric Trace Molecule Spectroscopy instrument aboard the Space Shuttle during the Spacelab 3 mission of April 29 to May 6, 1985. It was found that, in April-May 1985, near 30 deg N, the mean total stratospheric concentrations of Cl and F were 2.58 +/-0.10 ppbv and 1.15 +/-0.12 ppbv, respectively. Partitioning among the source, sink, and reservoir species was consistent with the conservation of the F and Cl budgets throughout the stratosphere. It is shown that the budgets of Cl and F above about 45 km altitude can be determined accurately by measuring only HCl, HF, and CF4 and provide a straightforward timely reference point for future inventories and trends evaluations.

Description: Vertical profiles of infrared cirrus extinction have been derived from tropical and subtropical upper tropospheric solar occultation spectra. The measurements were recorded by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the Atmospheric Laboratory for Applications and Sciences (ATLAS) 3 shuttle flight in November 1994. The presence of large numbers of small ice crystals is inferred from the appearance of broad extinction features in the 8-12 micron region. These features were observed near the tropopause and at lower altitudes. Vertical profiles of the ice extinction (/km) in microwindows at 831, 957, and 1204/cm have been retrieved from the spectra and analyzed with a model for randomly oriented spheroidal ice crystals. An area-equivalent spherical radius of 6 microns is estimated from the smallest ice crystals observed in the 8-12 gm region. Direct penetration of clouds into the lower stratosphere is inferred from observations of cloud extinction extending from the upper troposphere to 50 mbar (20 km altitude). Cloud extinction between 3 and 5 microns shows very little wavelength dependence, at least for the cases observed by the ATMOS instrument in the tropics and subtropics during ATLAS 3.

Description: Stratospheric volume mixing ration profiles of chlorine nitrate have been retrieved from 0.01-cm(sub -1) resolution infrared solar occutation spectra recorded at latitudes between 14 degrees N and 54 degrees S by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the ATLAS 1 shuttle mission (March 24 to April 2, 1992).