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At least 1,261 records · Page 70

Far-infrared measurement of stratospheric carbon monoxide

The stratospheric vertical distribution of CO is obtained from balloon-based FIR limb thermal emission spectra by analyzing several limb sequences of the R8 and R1 spectral lines at 34.588 and 49.932/cm, respectively. This constitutes the first determination of the stratospheric CO profile from IR thermal emission spectra. The results, indicating 24.6 + or - 7.6 ppbv at 21 km and 34.4 + or - 10.1 ppbv at 37 km, are compared with the remote-sensing and in situ measurements by other groups and with photochemical-dynamical model calculations.

Abbas, M. M.↗

Chemistry of OClO in the Antarctic stratosphere - Implications for bromine

Previous observations of OClO over the Antarctic obtained in 1986 are used to constrain the stratospheric abundance of bromine. The observed diurnal variation is consistent with the production of OClO via the reaction of ClO with BrO if the branching ratio to the BrCl channel is between 3.5 and 14 percent. Otherwise, an additional source in twilight is indicated. The present results suggest a stratospheric bromine concentration of 16 + or - 4 pptv, a value which is consistent with independent measurements.

Salawitch, Ross J.↗

Simultaneous measurement of minor stratospheric constituents with emission far-infrared spectroscopy

The vertical mixing ratio profiles of H2O, HDO, O3, heavy ozone, HF, HCl, HCN, and OH in the stratosphere are retrieved from high-resolution far-infrared emission spectra. These spectra were obtained with a balloon-borne Fourier transform spectrometer in the spring of 1979 at 32 deg N. The nonlinear least squares fit method is used in the analysis. The results are obtained relative to the O2 mixing ratio, whose emission features can be found in the same spectra. The retrieval of OH together with other species should be particularly significant for the study of upper stratospheric photochemistry, although the errors are relatively large: 28 percent for OH and 16-19 percent for other species.

Carli, Bruno↗

Characterization of the Nimbus-7 SBUV radiometer for the long-term monitoring of stratospheric ozone

Precise knowledge of in-orbit sensitivity change is critical for the successful monitoring of stratospheric ozone by satellite-based remote sensors. This paper evaluates those aspects of the in-flight operation that influence the long-term stability of the upper stratospheric ozone measurements made by the Nimbus-7 SBUV spectroradiometer and chronicles methods used to maintain the long-term albedo calibration of this UV sensor. It is shown that the instrument's calibration for the ozone measurement, the albedo calibration, has been maintained over the first 6 yr of operation to an accuracy of approximately + or - 2 percent. The instrument's wavelength calibration is shown to drift linearly with time. The knowledge of the SBUV wavelength assignment is maintained to a 0.02-nm precision.

Cebula, Richard P.↗

Submillimeter measurement of stratospheric chlorine monoxide

The measurement of the ClO concentration in the stratosphere provides crucial information on the mechanism for ozone depletion by catalytic reactions involving chlorine. Two rotational transitions of ClO, J = 35/2 - 33/2 and J = 37/2 - 35/2 have been identified in balloon-borne high-resolution spectra of the stratospheric emission in the submillimeter region. The measurements provide information on the ClO concentration at altitudes around 28 km. In the case of afternoon measurements obtained in April 1979, a scaling factor of 0.85 (+0.67, -0.64) is observed, and in the case of afternoon and early morning measurements obtained in October 1982, a scaling factor of 0.88 (+0.18, -0.08) is observed.

Carli, B.↗

Effects of stratospheric lapse rate on thunderstorm cloud-top structure in a three-dimensional numerical simulation. I - Some basic results of comparative experiments

The effects of stratospheric temperature lapse rate on cloud top height/temperature structure for strongly sheared, mature, isolated midlatitude thunderstorms are investigated by performing three different experiments with an anelastic, three-dimensional model: (1) with an assumed stratospheric lapse rate of 0 K/km (i.e., the isothermal case), (2) with 3 K/km, and (3) with -3 K/km (i.e., the case of inversion). Kinematic storm structure is very similar in all three cases, especially in the troposphere; a strong quasi-steady updraft evolves and splits into a dominant cyclonic overshooting right-mover and a weaker, anticyclonic left-mover that does not reach the tropopause.

Schlesinger, Robert E.↗

ClO and O3 stratospheric profiles - Balloon microwave measurements

Stratospheric ClO and O3 vertical profiles were measured at 32-deg N in May 1985 and October 1986. The ClO profiles and diurnal variation are in general agreement with theory, but have somewhat less midday ClO near 34 km. Measured 35-45 km O3 is larger than theoretical, and no stratospheric O3 diurnal variation was observed, as expected. HNO3 was detected, and an H2O2 upper limit was obtained.

Waters, J. W.↗

Laboratory studies of the nitric acid trihydrate - Implications for the south polar stratosphere

Vapor pressures of HNO3 and H2O have been measured over the trihydrate crystal, formed by vapor deposit on a glass surface. In the temperature range 190 to 205 K the two phase-equilibrium trihydrate/vapor was studied by adding and removing H2O. Coexistence equilibria vapor pressures of trihydrate/solid solutions of HNO3 in ice and of mono-/trihydrate were also measured. Results show that for typical mixing ratios of H2O and HNO3 found in the lower stratosphere (3 ppm H2O, 5 ppb HNO3) the trihydrate would start to form at temperatures about 7 K higher than the ice point. The pressure of atmospheric HNO3 would rapidly decrease as the atmosphere cools without large changes in partial pressures of H2O. These laboratory results provide information on the formation of polar stratospheric clouds containing H2O and HNO3.

Hanson, David↗

Influence of polar stratospheric clouds on the depletion of Antarctic ozone

Precipitation of nitrate in polar stratospheric clouds (PSCs) can provide a significant sink for Antarctic stratospheric odd nitrogen. It is argued that the depth of the Ozone Hole is sensitive to the occurrence of temperatures below about 196 K. An increase in the prevalence of temperatures below 196 K would enhance ozone loss by increasing the spatial extent and persistence of PSCs, and by decreasing the level of HNO3 that remains following PSC evaporation. Concentrations of halogen gases in the 1960s and earlier were insufficient to support major ozone loss, even if thermal conditions were favorable.

Salawitch, Ross J.↗

Backscatter laser depolarization studies of simulated stratospheric aerosols: Crystallized sulfuric acid droplets

The optical depolarizing properties of simulated stratospheric aerosols were studied in laboratory laser (0.633 micrometer) backscattering experiments for application to polarization lidar observations. Clouds composed of sulfuric acid solution droplets, some treated with ammonia gas, were observed during evaporation. The results indicate that the formation of minute ammonium sulfate particles from the evaporation of acid droplets produces linear depolarization ratios of beta equivalent to 0.02, but beta equivalent to 0.10 to 0.15 are generated from aged acid cloud aerosols and acid droplet crystallization effects following the introduction of ammonia gas into the chamber. It is concluded that partially crystallized sulfuric acid droplets are a likely candidate for explaining the lidar beta equivalent to 0.10 values that have been observed in the lower stratosphere in the absence of the relatively strong backscattering from homogeneous sulfuric acid droplet (beta equivalent to 0) or ice crystal (beta equivalent to 0.5) clouds.

Sassen, Kenneth↗

Persistence of Antarctic polar stratospheric clouds

The persistence of Polar Stratospheric Clouds (PSCs) observed by the Stratospheric Aerosol Measurement (SAM) 2 satellite sensor over a 9-year period is compared and contrasted. Histograms of the SAM 2 1.0 micron extinction ratio data (aerosol extinction normalized by the molecular extinction) at an altitude of 18 km in the Antarctic have been generated for three 10-day periods in the month of September. Statistics for eight different years (1979 to 1982 and 1984 to 1987) are shown in separate panels for each figure. Since the SAM 2 system is a solar occultation experiment, observations are limited to the edge of the polar night and no measurements are made deep within the vortex where temperatures could be colder. For this reason, use is made of the NMC global gridded fields and the known temperature-extinction relationship to infer additional information on the occurrence and areal coverage of PSCs. Calculations of the daily areal coverage of the 195 K isotherm will be presented for this same period of data. This contour level lies in the range of the predicted temperature for onset of the Type 1 particle enhancement mode at 50 mb (Poole and McCormick, 1988b) and should indicate approximately when formation of the binary HNO3-H2O particles begins.

Mccormick, M. Patrick↗

Balloon borne Antarctic frost point measurements and their impact on polar stratospheric cloud theories

The first balloon-borne frost point measurements over Antarctica were made during September and October, 1987 as part of the NOZE 2 effort at McMurdo. The results indicate water vapor mixing ratios on the order of 2 ppmv in the 15 to 20 km region which is somewhat smaller than the typical values currently being used significantly smaller than the typical values currently being used in polar stratospheric cloud (PSC) theories. The observed water vapor mixing ratio would correspond to saturated conditions for what is thought to be the lowest stratospheric temperatures encountered over the Antarctic. Through the use of available lidar observations there appears to be significant evidence that some PSCs form at temperatures higher than the local frost point (with respect to water) in the 10 to 20 km region thus supporting the nitric acid theory of PSC composition. Clouds near 15 km and below appear to form in regions saturated with respect to water and thus are probably mostly ice water clouds although they could contain relatively small amounts of other constituents. Photographic evidence suggests that the clouds forming above the frost point probably have an appearance quite different from the lower altitude iridescent, colored nacreous clouds.

Rosen, James M.↗

Formation of polar stratospheric clouds simulated in a two dimensional model of the atmosphere

A microphysics code has been implemented in a two dimensional model of the atmosphere to study formation of polar stratospheric clouds containing HCl or HNO3. The model range is from pole to pole in latitude and from the ground to about 20 km in altitude. Resolution in latitude is 10 deg and about 0.8 km in altitude. This is an Eulerian model with prescribed eddy diffusion coefficients and the circulation obtained from observations. The chemistry of the model follows the family approach for NO(x), Cl(x) and HO(x) while the ozone is fixed and changed seasonally. The aerosol code is based on an assigned population of condensation, coagulation and sedimentation. Aerosol growth is simulated in nine different size bins ranging between 0.01u and 2.56u. The model has been built to study aerosol layers formation in the upper troposphere and lower stratosphere and has been validated for sulfate aerosol resulting from a rather complex sulfur chemistry.

Visconti, Guido↗

Ice in the Antarctic polar stratosphere

On six occasions during the 1987 Airborne Antarctic Ozone Experiment, the Polar Stratospheric Cloud (PSC) ice crystals were replicated over the Palmer Peninsula at approximately 70 deg South. The sampling altitude was approximately 60 to 65 thousand feet, the temperature range was -83.5 to -72C and the atmosphere was subsaturated in all cases. The collected crystals were predominantly complete and hollow prismatic columns with maximum dimensions up to 217 microns. Evidence of scavenging of submicron particles was detected on several crystals. While the replicated crystal sizes were larger than anticipated, their relatively low concentration results in a total surface area less than one tenth that of the sampled aerosol particles. The presence of large crystals suggest that PSC ice crystals can play a very important role in stratospheric dehydration processes.

Goodman, J. K.↗

Heterogeneous physicochemistry of the winter polar stratosphere

Present chemical theories of the Antarctic ozone hole assume that heterogeneous reactions involving polar stratospheric clouds (PSCs) are the precursor of springtime ozone depletions. However, none of the theories quantify the rates of proposed heterogeneous processed, and none utilize the extensive data base on PSC's. Thus, all of the theories must be considered incomplete until the heterogeneous mechanisms are properly defined. A unified treatment developed of the cloud related processes, both physical and chemical, and the importance of these processes using observation data is calibrated. The rates are compared competitive heterogeneous processes to place reasonable limits on critical mechanisms such as the denitrification and dechlorination of the polar winter stratosphere. Among the subjects addressed here are the physical/chemical properties of PSC's including their relevant microphysical, optical and compositional characteristics, mass transfer rates of gaseous constituents to cloud particles, adsorption, accommodation and sticking coefficients on cloud particles, time constants for condensation, absorption and other microphysical processes, effects of solubility and vapor pressure on cloud composition, the statistics of cloud processing of chemically active condensible species, rate limiting steps in heterogeneous chemical reactions, and the nonlinear dependence of ozone loss on physical and chemical parameters.

Turco, R. P.↗

Lidar observations of polar stratospheric clouds at McMurdo, Antarctica, during NOZE-2

SRI International operated a dual wavelength (1.064 micrometer and .532 micrometer) aerosol lidar at McMurdo Station, Antarctica, as part of the National Ozone Expedition-2 (NOZE-2). The objective of the project was to map the vertical distributions of polar stratospheric clouds (PSCs), which are believed to play an important role in the destruction of ozone in the Antarctic spring. Altitude, thickness, homogeneity, and duration of PSC events as well as information on particle shape, size or number density will be very useful in determining the exact role of PSCs in ozone destructions, and when combined with measurements of other investigators, additional properties of PSCs can be estimated. The results are currently being analyzed in terms of PSC properties which are useful for modeling the stratospheric ozone depletion mechanism.

Morley, Bruce M.↗

Infrared measurements of column amounts of stratospheric constituents in the Antarctic winter, 1987

The discovery of Farman et al. of recent large depletions of ozone in the Antarctic stratosphere in the austral spring has aroused great interest because of its serious potential consequences, as well as its surprising nature. An airborne expedition, including 21 experiments on two aircraft, was mounted for Punta Arenas, Chile, in August and September, 1987, to gather a wide range of data to understand the origins and implications of this phenomenon, known as the ozone hole. As a part of this expedition, a high resolution Fourier transform spectrometer was flown on the DC-8, measuring the column amount of a number of trace gases above the flight altitude. Column results are presented only from the flight of September 21; results from other flights are included in an accompanying paper. The deduced column for ozone HCl, and NO2 deduced from the spectra, plotted as a function of latitude are shown. It should be noted that there are many other factors varying as well as the latitude, but latitude seems to be the variable which most clearly provides a passage across the vortex boundary. It can be seen that south 76 degrees S., the column of ozone, HCl, and NO2, all decreas markedly, The ratio of HCl to Hf, normally about 5:1 in midlatitudes, approaches unity. Clearly the chemistry of chlorine and nitrogen are disturbed in the region of low ozone. While dynamical theories could perhaps explain a reduction of these three gases in the same region, since all are of stratospheric origin, it is difficult to see how any purely dynamical mechanism could produce the observed HCl:HF ratio, since the two gases have similar origins. A close look at other species to be reported as well as the correlation with other measurements, such as ClO supports the conclusion that the ozone depletion is a result of chemical processes which deplete HCl and NOx relative to the midlatitude situation.

Mankin, William G.↗

Photochemical modeling of the Antarctic stratosphere: Observational constraints from the airborne Antarctic ozone experiment and implications for ozone behavior

The rapid decrease in O3 column densities observed during Antarctic spring has been attributed to several chemical mechanisms involving nitrogen, bromine, or chlorine species, to dynamical mechanisms, or to a combination of the above. Chlorine-related theories, in particular, predict greatly elevated concentrations of ClO and OClO and suppressed abundances of NO2 below 22 km. The heterogeneous reactions and phase transitions proposed by these theories could also impact the concentrations of HCl, ClNO3 and HNO3 in this region. Observations of the above species have been carried out from the ground by the National Ozone Expedition (NOZE-I, 1986, and NOZE-II, 1987), and from aircrafts by the Airborne Antarctic Ozone Experiment (AAOE) during the austral spring of 1987. Observations of aerosol concentrations, size distribution and backscattering ratio from AAOE, and of aerosol extinction coefficients from the SAM-II satellite can also be used to deduce the altitude and temporal behavior of surfaces which catalyze heterogeneous mechanisms. All these observations provide important constraints on the photochemical processes suggested for the spring Antarctic stratosphere. Results are presented for the concentrations and time development of key trace gases in the Antarctic stratosphere, utilizing the AER photochemical model. This model includes complete gas-phase photochemistry, as well as heterogeneous reactions. Heterogeneous chemistry is parameterized in terms of surface concentrations of aerosols, collision frequencies between gas molecules and aerosol surfaces, concentrations of HCl/H2O in the frozen particles, and probability of reaction per collision (gamma). Values of gamma are taken from the latest laboratory measurements. The heterogeneous chemistry and phase transitions are assumed to occur between 12 and 22 km. The behavior of trace species at higher altitudes is calculated by the AER 2-D model without heterogeneous chemistry. Calculations are performed for solar illumination conditions typical of 60, 70, and 80 S, from July 15 to October 31.

Rodriguez, Jose M.↗