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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.

Attention is given to total vertical column abundances of carbonyl sulfide (OCS) derived from time series of high-resolution IR solar absorption spectra recorded near Tucson, Arizona, and in the Swiss Alps. The analysis of both data sets is based on nonlinear least squares spectral fittings of narrow intervals centered on lines of the intense nu3 band of OCS, the P(37) transition at 2045.5788/cm, and the P(15) transition at 2055.8609/cm, with a consistent set of spectroscopic line parameters. The Arizona measurements, recorded on 20 different days between May 1977 and March 1991, show a 10-percent peak-to-peak seasonal cycle with a summer maximum and a winter minimum and a trend in the total column abundance equal to (0.1 +/-0.2) percent/yr, 2sigma. The Alpine total columns exhibit a more complex seasonal variation than noted in the Arizona data. The results from the two sites indicate that there has been no significant change in the OCS total column abundance at northern midlatitudes over the last decade.

The secular trend and the seasonal cycle of the total and the tropospheric column abundances of C2H6 over the Jungfraujoch Station (Switzerland) were deduced from infrared solar spectra recorded in 1951 and from 1984 to 1988. Results show a definite seasonal variation in the total vertical column abundance of C2H6, with a maximum of (1.43 + or - 0.03) x 10 to the 16th molecules/sq cm during March and April and a minimum in the fall; the ratio between the maximum and the minimum column abundances was found to be 1.62 + or - 0.11. The secular trend in the tropospheric burden above the Jungfraujoch was found to be (0.85 + or - 0.3) percent/yr.

The secular increase of the total vertical column abundance of carbon monoxide has been derived from sets of infrared solar spectra recorded from an altitude of 3.58 km at the Jungfraujoch Station, Switzerland, in 1950-1951 and in 1985-1987. The results are based on equivalent width measurements of the R3 line of the 1-0 vibration-rotation band of (C-12)(0-16) at 2159.30/cm. The set of 1985-1987 observations indicates a strong seasonal cycle in the total column abundance of CO, with a + or - 25 percent modulation between minimum values in late summer and the maximum values in late winter. Variability on shorter time scales is also present in both the old and recent data sets. The mean cumulative rate of increase of the total column abundance of CO above the Jungfraujoch is found to be (0.85 + or - 0.20) percent/yr between 1950-1951 and 1985-1987. The present findings are compared with trends reported in earlier studies.

It is argued from the central limit theorem that the uncertainty in model predicted changes of the ozone column density is best represented by a normal probability density distribution. This conclusion is validated by comparison with a probability distribution generated by a Monte Carlo technique. In the case of the CFM-induced ozone depletion, and based on the estimated uncertainties in the reaction rate coefficients alone the relative mean standard deviation of this normal distribution is estimated to be 0.29.

The methane concentration of an air sample collected near the stratopause was measured by gas chromatography and determined to be 0.25 plus or minus 0.02 ppm by volume. The integrity of the air sample with respect to its methane content, the method of analysis, and the result are briefly discussed.