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NASA NTRS1984

Passive microwave remote sensing of the atmosphere from satellites

Present and future satellite atmospheric sounding is discussed. Although present systems sound principally the temperature profile and the water vapor and precipitation abundances over ocean, future systems will measure other constituents such as O3, H2O2, and ClO, and will provide improved spatial resolution, retrieval accuracy, and altitude coverage for temperature and humidity. Present systems with only a few channels will be replaced by systems with 20 or more, and larger antennas with more sensitive radiometers will permit horizontal resolutions of 15 to 50 km or less, even from geosynchronous orbit. The success of imaging microwave spectrometers in penetrating clouds and in yielding uniquely accurate measurements ensure a growing role in operational and research systems for these remote sensing techniques.

Staelin, D. H.↗

NASA NTRS1985

Measurement of Elements in the Stratosphere

Balloon-borne winch system; stratospheric free radicals; stratospheric sounding; copper vapor lasers; ozone measurement; NO2 analysis; chlorine chemistry; trace elements; and ClO observations are discussed.

Anderson, J. G.↗

NASA NTRS1984

A balloon-borne microwave limb sounder for stratospheric measurements

The balloon-borne microwave limb sounder (BMLS) measures atmospheric thermal emission from millimeter wavelength spectral lines to determine vertical profiles of stratospheric species. The instrument flown to date operates at 205 GHz to measure ClO, O3, and H2O2. A 63 GHz radiometer will be added to test the technique for determining tangent point pressure from the MLS experiment on the upper atmosphere research satellite (UARS). Many additional species could also be measured by the BMLS. A radiometer at 270 GHz would provide measurements of HO2, NO2, HNO3, N2O, O-16O-18O-16, and HCN. With this addition, the BMLS can test the current theory of O3 photochemical balance in the upper stratosphere.

Waters, J. W.↗

NASA NTRS1985

Space telescope observations of the earth's upper atmosphere by stellar occultations

Stellar occultations provide a useful means of measuring the trace gas composition of the earth's mesosphere with a sensitivity of order one part per billion. The operational details will differ from those of other astronomical observations by ST, because of the difficulties in guiding near the earth's limb. Two specific trace gases of interest to atmospheric studies, Cl and ClO, are discussed in this paper.

Caldwell, J.↗

NASA NTRS1985

Tentative identification of the 780/cm nu-4 band Q branch of chlorine nitrate in high-resolution solar absorption spectra of the stratosphere

According to models of the photochemistry of the stratosphere, chlorine nitrate (ClONO2) is an important temporary reservoir of stratospheric chlorine. At night, ClO is believed to combine in a three-body reaction with NO2 to form chlorine nitrate. During daylight, chlorine nitrate is destroyed by photolysis to form free chlorine and NO3. Infrared spectroscopy has the potential to provide a technique for conducting important quantitative measurements of stratospheric chlorine nitrate. The present paper reports a detailed study of spectra in the 780/cm region. This study has led to the tentative identification of the nu-4 band Q branch of ClONO2 as a significant contributor to the observed stratospheric absorption near 780.21 per cm.

Rinsland, C. P.↗

NASA NTRS1985

Microwave limb sounder for stratospheric measurements

The balloon-borne Microwave Limb Sounder (BMLS) measures atmospheric thermal emission from millimeter wavelength spectral lines to determine vertical profiles of stratospheric species. The instrument flown to data operates at 205 BHz to measure ClO, O3, and H2O2. A 63 GHz radiometer is added to test the technique for determining tangent point pressure from the MLS experiment on the Upper Atmosphere Research Satellite (UARS). Many additional species is also measured by the BLMS. A radiometer at 270 GHz would provide measurements of HO2, NO2, HNO3, N2O, 16O18O16O, and HCN. With this addition the BMLS can test the current theory of O3 heavy ozone photochemical balance in the upper stratosphere.

Waters, J. W.↗

NASA NTRS1985

Atmospheric concentrations and behavior of halocarbons and methane

The atmospheric concentrations of halocarbons and methane in the troposphere and stratosphere were precisely measured by grab-sampling followed by gas-chromatographic analysis in the laboratory. Chlorofluorocarbons such as CCl2F2 and CCl3F have received a great deal of attention due to their probable impact on the stratospheric ozone: the chlorofluorocarbons accumulated in the troposphere are eventually decomposed by photolysis in the stratosphere releasing Cl radicals which in turn participate in the ClO sub x-catalytic chain destroying the ozone, especially in the upper stratosphere. Methane reacts with Cl in the stratosphere reducing the ozone depletion, while its source and future trend of concentration in the troposphere are uncertain. The study of their distribution and behavior in the atmosphere are therefore very important. After the extensive survey of the locations for collection of atmospheriic samples representing the midlatitudes Northern Hemisphere (N.H.) without local contamination, we have measured the concentrations of CCl2F2, CCl3F, CH3CCl3, CC1, CHCl=CCl2 and CCl2=CCl2 with plus or minus 1 pptv precision in samples collected in Hokkaido and west coast Tohoku area (the northern part of Japan, 40 deg to 45 deg N) every summer and winter since 1979. The observed concentrations of CCl2F2 and CCl3F are now above 360 and 200 pptv, respectively, and have been steadily increasing by approx. 15 and approx. 8 pptv/year during the last several years.

Makide, Y.↗

NASA NTRS1985

Halogentated species

Stratospheric measurements of halogen containing species are reviewed and compared with model predictions. Halocarbons, HCl, HF, ClONO2, and ClO are discussed.

Molina, M. J.↗

NASA NTRS1985

Far-infrared spectroscopy of the earth's stratosphere

This paper discusses the spectrum of the earth's stratosphere in the far-infrared, from 5 to 250/cm. Many of the trace gases that are important in stratospheric photochemistry have been measured, or are potentially measurable in the far-infrared. The spectral features of these gases are discussed with application to spacecraft measurements. In particular, the suitability of the spectrum for measurements of the HO(x) and ClO(x) families and of O3 are compared for different classes of instruments: Fourier transform spectrometers, filter radiometers, and scanning high-resolution Fabry-Perot instruments. It is found that these types of instruments have complementary capabilities that would best be used in combination in a comprehensive multispecies measurement scheme.

Chance, K. V.↗

NASA NTRS1985

The Imaging Spectrometric Observatory

Design and performance features of the Imaging Spectrometric Observatory (ISO) first flown on Spacelab 1 for atmospheric, earth surface and stellar monitoring are outlined. The ISO has five grating spectrometers fitted with CCD arrays for simultaneously gathering spectral and spatial data. The instrument covered the 300-12,700 A range on the Spacelab 1 flight, when it was mounted on a pallet and used for atmospheric scans at high solar zenith angles. A future mission is planned which will include limb-viewing of OH, NO, ClO and NO2 radicals in the middle atmosphere to complement the data collected in the Upper Atmosphere Research Satellite program. Technical details are presented of the instrument components and ground- and balloon-borne test results.

Torr, D. G.↗

NASA NTRS1986

Sensitivity of an atmospheric photochemistry model to chlorine perturbations including consideration of uncertainty propagation

Models of stratospheric photochemistry are generally tested by comparing their predictions for the composition of the present atmosphere with measurements of species concentrations. These models are then used to make predictions of the atmospheric sensitivity to perturbations. Here the problem of the sensitivity of such a model to chlorine perturbations ranging from the present influx of chlorine-containing compounds to several times that influx is addressed. The effects of uncertainties in input parameters, including reaction rate coefficients, cross sections, solar fluxes, and boundary conditions, are evaluated using a Monte Carlo method in which the values of the input parameters are randomly selected. The results are probability distributions for present atmosheric concentrations and for calculated perturbations due to chlorine from fluorocarbons. For more than 300 Monte Carlo runs the calculated ozone perturbation for continued emission of fluorocarbons at today's rates had a mean value of -6.2 percent, with a 1-sigma width of 5.5 percent. Using the same runs but only allowing the cases in which the calculated present atmosphere values of NO, NO2, and ClO at 25 km altitude fell within the range of measurements yielded a mean ozone depletion of -3 percent, with a 1-sigma deviation of 2.2 percent. The model showed a nonlinear behavior as a function of added fluorocarbons. The mean of the Monte Carlo runs was less nonlinear than the model run using mean value of the input parameters.

Stolarski, R. S.↗

NASA NTRS1985

LIMS data - Inferred stratospheric distribution of NOx and HOx trace constituents and the calculated odd nitrogen budget

LIMS, SAMS, SBUV and in-situ data have been used to infer species not measured but which are of photochemical interest, e.g., O(3P), O(1D), NO, N2O5, OH, HO2, ClO and HCl. (LIMS = limb infrared monitor of the stratosphere; SAMS = stratospheric and mesospheric sounder; and SBUV = solar backscattered ultraviolet instrument.) Production and loss of odd nitrogen have been calculated and estimates have been made of the odd nitrogen transport due to adiabatically driven circulation derived from LIMS data. Data used from LIMS include O3, NO2, HNO3, H2O and T. CH4 and N2O were taken from SAMS and the UV solar flux from the SBUV instrument. Species were inferred for periods in October, December, March and May. Results for December are discussed. Results indicate: (1) maximum stratospheric odd nitrogen levels of 25 ppbv; (2) evidence of odd nitrogen transport from the mesosphere appearing at 25 km in the wintertime polar latitudes; (3) the polar night build-up of high levels of N2O5 beginning after the autumnal equinox; and (4) the possibility of large downward fluxes of odd nitrogen into the troposphere during the winter at latitudes poleward of 60 degrees.

Callis, L. B.↗

NASA NTRS1986

Laser heterodyne system for obtaining height profiles of minor species in the atmosphere

An infrared laser heterodyne system for obtaining height profiles of minor constituents of the atmosphere was developed and erected. A brief discription of the system is given. The system consists of a tunable CO2 waveguide laser in the 9 to 11 micrometer band, that is used as a local oscillator and a heliostat that follows the sun and brings in solar radiation, that is mixed with the laser beam in a high speed liquid nitrogen cooled mercury cadmium telluride detector. The detected signal is analysed in a RF spectrum analyser that allows tracing absorption line profiles. Absorption lines of a number of minor constituents in the troposphere and stratosphere, such as O3, NH3, H2O, SO2, ClO, N2O, are in the 9 to 11 micrometer band and overlap with that of CO2 laser range. The experimental system has been made operational and trial observations taken. Current measurements are limited to ozone height profiles. Results are presented.

Jain, S. L.↗

NASA NTRS1985

Stratospheric chemistry

Recent improvements in the data base for the currently identified reactions describing the chemistry of the major families of trace gas species, HO(x), NO(x), ClO(x), and hydrocarbons are assessed. The important coupling reactions between the families are introduced progressively. Chemical aspects such as heterogeneous reactions and reactions of sodium species, the importance of which are not yet completely established, are discussed. Recent attempts to reconcile some of the more unexpected kinetic behavior which has emerged from the extensive experimental studies of key reactions with current reaction rate theory are also examined. The uncertainties in the current kinetic and photochemical data base is given. The prospects for improvement of data for known reactions of atmospheric importance as well as for the identification of gaps in the chemical description of the atmosphere.

Cox, R. A.↗

NASA NTRS1986

Photochemical production of H2SO4 aerosols on Venus

The quantum yields for producing O2(a (1 delta g)) and O2(b(1 sigma g +)) for the reaction, O + ClO yields Cl + O2, are summarized. Also included are results for other simple reactions capable of producing the singlet oxygen states. An episodic injection of SO2 into the upper atmosphere of Venus is considered as a possible explanation for the airglow values.

Yuk, L. Yung↗

NASA NTRS1987

Atlas of Absorption Lines from 0 to 17900 Cm (sup)-1

Plots of logarithm (base 10) of absorption line strength versus wavenumber from 0 to 17900/cm(sup)-1 are shown for the 28 atmospheric gases (H2O, CO2, O3, N2O, CO, CH4, O2, NO, SO2, NO2, NH3, HNO3, OH, HF, HCl, HBr, HI, ClO, OCS, H2CO, HOCl, N2, HCN, CH3Cl, H2O2, C2H2, C2H6, PH3), which appear in the 1986 Air Force Geophysics Laboratory high-resolution transmission molecular absorption data base (HITRAN) compilation, and for O(P-3), O-18 isotopic ozone, and HO2 from the 1984 JPL compilation in the 0- to 200/cm(sup)-1 region, and infrared solar CO lines at 4500 K. Also shown are plots of logarithm (base 10) of approximate infrared absorption cross sections of 11 heavy molecules versus wavenumber. The cross-section data cover 700 to 1800/cm(sup)-1 and are included as a separate data file in the 1986 HITRAN database.

Park, J. H.↗

NASA NTRS1986

Are Antarctic ozone variations a manifestation of dynamics or chemistry?

The existence of a reverse circulation cell with rising motion in the polar lower stratosphere is suggested as an explanation for the temporal behavior of the ozone column density in the Antarctic region. The upwelling brings ozone-poor air from below 100 mbar to the stratosphere, possibly contributing to the observed ozone decline in early spring. At the same time, the Antarctic stratosphere might contain a very low concentration of NO(x), a condition that could favor a greatly enhanced catalytic removal of O3 by halogen species. It is argued that heterogeneous processes and formation of OClO by the reaction BrO+ClO - OClO+Br before and after the polar night might help to suppress the NO(x) levels during the early spring period.

Tung, K.-K.↗

NASA NTRS1986

Condensation of HNO3 and HCl in the winter polar stratospheres

Nitric acid and hydrochloric acid vapors may condense in the winter polar stratospheres. Nitric acid clouds, unlike water ice clouds, would form at the temperatures at which polar stratospheric clouds (PSCs) are observed and would have optical depths of the magnitude observed suggesting that HNO3 is a dominant component of PSCs. ClO, N2O5 and ClNO3 may react on cloud particle surfaces yielding additional HNO3, HCl, and HOCL. In the vicinity of PSCs these reactions could deplete the stratosphere of photochemically active NO(x) species. The sedimentation of PSCs may remove these materials from the stratosphere. The loss of vapor phase NO(x) might allow halogen-based chemistry to create the ozone hole.

Toon, Owen B.↗