The fluorocarbon and nitrous oxide content of the stratosphere have been studied as a function of altitude, latitude, and time. Whole air samples have been gathered from a balloon platform, primarily through use of a cryogenic sampler. Twenty‐two flights were conducted between 1975 and 1980, and gas chromatography was utilized to determine species mixing ratios in the retrieved samples. Results are evaluated in terms of various stratosphere models.

Chemiluminescence and resonance fluorescence of FeO has been observed upon release of iron carbonyl into the atomic oxygen-rich region of the upper atmosphere. The FeO molecules are formed in a fast reaction between IC and atomic oxygen in the mixing zone surrounding the rocket. FeO does not persist to form a long-lasting wake, apparently since it reacts with another O to give Fe and O•. The upper atmosphere can be a convenient environment to study the formation, destruction, and radiation characteristics of some unstable molecular species that in the laboratory would suffer from the presence of walls, higher collision rates, or insufficient optical path. The molecule Fe0 is a case in point. Its emission spectrum has been observed in a flame of an iron arc in air, or when iron carbonyl is introduced into a flame [see, e.g., Pearse and Gaydon, 1950; Mavrodineanu and Boiteux, 1965]. However, little is known on the reaction of Fe0 with atomic oxygen or the resonance fluorescence emission when the molecule is irradiated. The irradiation effects particularly can be studied in the upper atmosphere.

A cryogenic whole air sampler and a filter sampler were used, simultaneously, on a balloon platform to capture and preserve all significant stratospheric chlorine species with the exception of Cl and ClO at altitudes of 15, 20, 25, and 30 km. The whole air samples were analyzed by gas chromatography to determine mixing ratios of CF2Cl2, CFCl3, CH3Cl, CH3CCl3, and CCl4. Liquid extractions of the filter samples were analyzed for acidic and particulate chlorine content using neutron activation and wet chemistry techniques. Summation of the contributions from the major species produced total chlorine mixing ratios that decreased from 2.6 ppbv at 15 km to 2.2–2.5 ppbv for the higher altitudes. Omission of Cl and ClO introduced about a 3–7% error at 25–30 km and negligible error at 15 and 20 km. The combined contributions of all other omitted species introduced 1–2% error to the total chlorine values for all altitudes investigated. The increase in total acidic species content with increasing altitude correlates with the decrease in the mixing ratios of the chlorine species of tropospheric origin.

Whole air samples were obtained in the stratosphere using a liquid helium‐cooled cryosampler mounted on a balloon platform. Approximately 1 g mol of sample was obtained at each of three altitudes per balloon flight and was maintained at 4 K until desorption just prior to analysis. Samples were obtained at six altitudes ranging from 12 to 30 km and at five latitudes from 9° to 64°N. Nitric oxide and the sum of nitric oxide and nitrogen dioxide content of the samples were determined using two chemiluminescence analyzers. Results from flights conducted between 1977 and 1981 are correlated with atmospheric motions and other significant variables and evaluated in terms of both one‐ and two‐dimensional models of the stratosphere.