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NASA NTRS1989

Direct determination of the morphology, structure and composition of cometary and interstellar ice analogs in the laboratory

Ices of various kinds (H2O, CO, CO2, CH4, NH3, CH3OH, etc.) comprise a volumetrically significant proportion of objects in the solar system (comets, outer planets, planetary rings, satellites) as well as in interstellar space (astrophysical ices). The refinement of analytical electron microscopy (AEM) procedures for storing, preparing and analyzing ices and other materials at cryogenic temperatures is discussed. These procedures will be essential to the successful analysis of returned comet nucleus samples.

Blake, D. F.↗

NASA NTRS1989

Modifications of comet materials by the sublimation process: Results from simulation experiments

An active comet like comet Halley loses by sublimation a surface layer of the order of 1 m thickness per perihelion passage. In situ measurements show that water ice is the main constituent which contributes to the gas emission although even more volatile species (CO, NH3, CH4, CO2 etc.) have been identified. Dust particles which were embedded in the ices are carried by the sublimating gases. Measurements of the chemical composition of cometary grains indicate that they are composed of silicates of approximate chondritic composition and refractory carbonaceous material. Comet simulation experiments show that significant modifications of cometary materials occur due to sublimation process in near surface layers which have to be taken into account in order to derive the original state of the material.

Gruen, E.↗

NASA NTRS1989

Electron Spin Resonance (ESR) studies of returned comet nucleus samples

The most important objective of the Comet Nucleus Sample Returm Mission is to return samples which could reflect formation conditions and evolutionary processes in the early solar nebula. It is expected that the returned samples will consist of fine-grained silicate materials mixed with ices composed of simple molecules such as H2O, NH3, CH4 as well as organics and/or more complex compounds. Because of the exposure to ionizing radiation from cosmic-ray, gamma-ray, and solar wind protons at low temperature, free radicals are expected to be formed and trapped in the solid ice matrices. The kind of trapped radical species together with their concentration and thermal stability can be used as a dosimeter as well as a geothermometer to determine thermal and radiation histories as well as outgassing and other possible alternation effects since the nucleus material was formed. Since free radicals that are known to contain unpaired electrons are all paramagnetic in nature, they can be readily detected and characterized in their native form by the Electron Spin Resonance (ESR) method. In fact, ESR has been shown to be a non-destructive, highly sensitive tool for the detection and characterization of paramagnetic, ferromagnetic, and radiation damage centers in terrestrial and extraterrestrial geological samples. The potential use of ESR as an effective method in the study of returned comet nucleus samples, in particular, in the analysis of fine-grained solid state icy samples is discussed.

Tsay, Fun-Dow↗

NASA NTRS1990

New parameter-free polarization potentials in low-energy positron collisions

The polarization potential plays a decisive role in shaping up the cross sections in low energy positron collisions with atoms and molecules. However, its inclusion without involving any adjustable parameter, is still a challenge. Various other techniques employed so far for positron collisions are summarized, and a new, nonadjustable and very simple form of the polarization potential for positron-atom (molecule) collisions below the threshold of positronium formation is discussed. This new recently proposed potential is based on the correlation energy of a single positron in a homogeneous electron gas. The correlation energy was calculated by solving the Schrodinger equation of the positron-electron system and fitted to an analytical form in various ranges of the density parameter. In the outside region, the correlation energy is joined smoothly with the correct asymptotic form. This new positron correlation polarization (PCOP) potential was tested on several atomic and molecular targets such as the Ar, CO, and CH4. The results on the total and differential cross sections on these targets are shown along with the experimental data where available.

Jain, Ashok↗

NASA NTRS1989

Measurements of the D/H ratio in planetary atmospheres by ground based infrared spectroscopy

A systematic study of deuterium in the solar system using the molecules CH3D and HDO as tracers is carried out. For the outer solar system, ground-based spectra of Saturn, Uranus, Neptune and Titan in the region of CH3D absorptions near, 1.6 microns are obtained. The analyses of these spectra required extensive high-resolution laboratory studies of both CH4 and CH3D. For the terrestrial planets, the spectrum of Mars in the region of HDO absorption near 3.7 microns, is recorded. A similar study of Venus is underway. The values of D/H derived from these investigations are used to constrain models for the origin and evolution of the various atmospheres.

Debergh, C.↗

NASA NTRS1990

High resolution, low temperature photoabsorption cross-section of C2H2 with application to Saturn's atmosphere

New laboratory observations of the VUV absorption cross-section of C2H2, obtained under physical conditions approximating stratospheres of the giant planets, were combined with IUE observations of the albedo of Saturn, for which improved data reduction techniques have been used, to produce new models for that atmosphere. When the effects of C2H2 absorption are accounted for, additional absorption by other molecules is required. The best-fitting model also includes absorption by PH3, H2O, C2H6 and CH4. A small residual disagreement near 1600 A suggests that an additional trace species may be required to complete the model.

Caldwell, John↗

NASA NTRS1990

Measurements of the methane relaxation times for application to the infrared emission models of the upper atmospheres of outer planets and Titan

The 7.8 micrometer emission from the nu(sub 4) band of methane (CH4) is a regularly observed feature in the stratosphere of all the giant planets and Titan. On Jupiter, enhancements in this emission are associated with the infrared hot spots in the auroral zone. Attempts to model this phenomenon in particular, and to understand the role of methane in general, have been hampered in part by a lack of adequate laboratory measurements of the collisional relaxation times for the nu(sub 3) and nu(sub 4) levels over the appropriate temperature range. To provide this needed data, a series of laboratory experiments were initiated. In the experimental arrangement the nu(sub3) band of methane is pumped at 3.3 micrometers using a pulsed infrared source (Nd:YAG/dye laser system equipped with a wave-length extender). The radiative lifetime of the nu(sub 3) level (approximately 37 ms) is much shorter than the nu(sub 4) lifetime (approximately 390 ms); however, a rapid V-V energy transfer rate ensures that the nu(sub 4) level is substantially populated. The photoacoustic technique is used to acquire relaxation rate information. The experiments are performed using a low-temperature, low-pressure cell. Experimental apparatus and technique are described. In addition some of the experimental difficulties associated with making these measurements are discussed and some preliminary results are presented.

Halthore, Rangasayi N.↗

NASA NTRS1990

Interstellar grain chemistry and organic molecules

The detection of prominant infrared absorption bands at 3250, 2170, 2138, 1670 and 1470 cm(-1) (3.08, 4.61, 4.677, 5.99 and 6.80 micron m) associated with molecular clouds show that mixed molecular (icy) grain mantles are an important component of the interstellar dust in the dense interstellar medium. These ices, which contain many organic molecules, may also be the production site of the more complex organic grain mantles detected in the diffuse interstellar medium. Theoretical calculations employing gas phase as well as grain surface reactions predict that the ices should be dominated only by the simple molecules H2O, H2CO, N2, CO, O2, NH3, CH4, possibly CH3OH, and their deuterated counterparts. However, spectroscopic observations in the 2500 to 1250 cm(-1)(4 to 8 micron m) range show substantial variation from source reactions alone. By comparing these astronomical spectra with the spectra of laboratory-produced analogs of interstellar ices, one can determine the composition and abundance of the materials frozen on the grains in dense clouds. Experiments are described in which the chemical evolution of an interstellar ice analog is determined during irradiation and subsequent warm-up. Particular attention is paid to the types of moderately complex organic materials produced during these experiments which are likely to be present in interstellar grains and cometary ices.

Allamandola, L. J.↗

NASA NTRS1990

Laboratory simulation of interstellar grain chemistry and the production of complex organic molecules

During the past 15 years considerable progress in observational techniques has been achieved in the middle infrared (5000 to 500 cm(-1), 2 to 20 microns m), the spectral region most diagnostic of molecular vibrations. Spectra of many different astronomical infrared sources, some deeply embedded in dark molecular clouds, are now available. These spectra provide a powerful probe, not only for the identification of interstellar molecules in both the gas solid phases, but also of the physical and chemical conditions which prevail in these two very different domains. By comparing these astronomical spectra with the spectra of laboratory ices one can determine the composition and abundance of the icy materials frozen on the cold (10K) dust grains present in the interior of molecular clouds. These grains and their ice mantles may well be the building blocks from which comets are made. As an illustration of the processes which can take place as an ice is irradiated and subsequently warmed, researchers present the infrared spectra of the mixture H2O:CH3OH:CO:NH3:C6H14 (100:50:10:10:10). Apart from the last species, the ratio of these compounds is representative of the simplest ices found in interstellar clouds. The last component was incorporated into this particular experiment as a tracer of the behavior of a non-aromatic hydrocarbon. The change in the composition that results from ultraviolet photolysis of this ice mixture using a UV lamp to simulate the interstellar radiation field is shown. Photolysis produces CO, CO2, CH4, HCO, H2CO, as well as a family of moderately volatile hydrocarbons. Less volatile carbonaceous materials are also produced. The evolution of the infrared spectrum of the ice as the sample is warmed up to room temperature is illustrated. Researchers believe that the changes are similar to those which occur as ice is ejected from a comet and warmed up by solar radiation. The warm-up sequence shows that the nitrile or iso-nitrile bearing compound produced during photolysis evaporates between 200 and 250K, suggesting that it is carried by a small molecular species. These molecules could be similar to the source material in Comet Halley that is ejected in grains into the coma, freed by sublimation, and photolyzed by solar radiation to produce the observed jets.

Allamandola, L. J.↗

NASA NTRS1990

Carbon in the outer solar system

The satellites of Uranus, with densities between 1.3 and 1.7 g cm(-3) (from Voyager 2 observations) and the Pluto-Charon system, with a mean density of just above 1.8 g cm(-3) (from terrestrial observations of mutual eclipse events), are too dense to have a significant amount of methane ice in their interiors. However, the observed densities do not preclude contributions from such organic materials as the acid-insoluble residue in carbonaceous chondrites and laboratory-produced tholins, which have densities on the order of approximately 1.5 g cm(-3). These and other considerations have led researchers to investigate the carbon mass budget in the outer solar system, with an emphasis on understanding the contribution of organic materials. Modeling of the interiors of Pluto and Charon (being carried out by R. Reynolds and A. Summers of NASA/Ames), assuming rock and water ice as the only constituents, suggests a silicate mass fraction for this system on the order of 0.65 to 0.70. The present work includes the most recent estimates of the C/H enhancements and high z/low z ratios of the giant planets (Pollack and Bodenheimer, 1987), and involves a more careful estimation of the high z/low z mass ratio expected from solar abundances than was used in Pollack et al. (1986), including the influence of the fraction of C in CO on the amount of condensed water ice. These calculations indicate that for a particular fraction of C in CO and a given fraction of C-bearing planetesimals that dissolve in the envelope (most likely in the range 0.50 to 0.75), (1) Jupiter and Saturn require a larger fraction of C in condensed materials than Uranus and Neptune, but (2) the Jupiter and Saturn results are much less strongly constrained by the error bars on the observed C/H enhancements and high z/low z ratios than is the case for Uranus and Neptune. The clearest result is that in the region of the solar nebula near Uranus and Neptune, the minority of carbon that is not in gaseous CO (1) must include a nonzero amount of condensed material, but (2) is most likely not condensed material alone, i.e., there must be a third carbon-bearing component besides condensed material and gaseous CO. Given the implied dearth of methane ice, the condensed carbon is likely dominated by organic material, and the third component present in addition to CO and organics is assumed to be CH4 gas.

Simonelli, D. P.↗

NASA NTRS1989

Remote sensing of biomass burning in the tropics

A technique for assessing the effects of biomass burning on the climate is described. This method is based on the analysis of remote sensing data for the emitted particulates. The relationship between particulates and trace gases is studied. The assessment technique is applied to the 1987 burning season in Brazil. It is noted that during the dry season there may be up to 5000 fires per day which emit 200 ton/hr CO2, 20 ton/hr CO, and 0.5 ton/hr of CH4 to the atmosphere.

Kaufman, Yoram J.↗

NASA NTRS1989

Cryogenic Limb Array Etalon Spectrometer (CLAES) - Experiment overview

The Cryogenic Limb Array Etalon Spectrometer (CLAES) is one of a complement of instruments on the NASA Upper Atmosphere Research Satellite which is expected to study atmospheric photochemistry, energy input, and dynamics following a 1991 launch. CLAES measures stratospheric altitude profiles of temperature, pressure, O3, H2O, CH4, N2O, NO, NO2, N2O5, HNO3, ClONO2, HCl, CFC-11, and CFC-12. These data are obtained typically between 10 and 60 km, with 2.5-km vertical resolution and 500-km horizontal grid size. Coverage is obtained between latitudes 80 deg north and south, thereby providing substantial coverage of the Antarctic spring polar ozone-hole region. CLAES derives the listed geophysical parameters from measurement of earth-limb spectral emissions between 3.5 and 13 microns. Brief discussions of the measurement concept, instrument design, and performance are presented, followed by a more detailed discussion of scientific capabilities and measurement modes.

Roche, Aidan E.↗

NASA NTRS1989

Production of organic compounds in plasmas - A comparison among electric sparks, laser-induced plasmas, and UV light

In order to ascertain the features of organic compound-production in planetary atmospheres under the effects of plasmas and shocks, various mixtures of N2, CH4, and H2 modeling the atmosphere of Titan were subjected to discrete sparks, laser-induced plasmas, and UV radiation. The experimental results obtained suggest that UV photolysis from the plasma is an important organic compound synthesis process, as confirmed by the photolysis of gas samples that were exposed to the light but not to the shock waves emitted by the sparks. The thermodynamic equilibrium theory is therefore incomplete in the absence of photolysis.

Scattergood, Thomas W.↗

NASA NTRS1988

Optical emission diagnostics of electron cyclotron resonance and glow discharge plasmas for a-Si:H and a-SiC:H film depositions

It is demonstrated that the steady-state and kinetic characteristics of ECR (electron cyclotron resonance) and RF glow discharge plasmas can be readily monitored by OES (optical emission spectroscopy) in real time during a-Si:H and a-SiC:H film depositions using an OMA detection system. The ECR and RF glow discharge plasmas used for a-Si:H and a-SiC:H film depositions were studied by monitoring the emission of SiH(asterisk), H(asterisk), H(asterisk)2, and CH(asterisk) excited states. The OES of the ECR plasma shows a strong emission at 434 nm from H(asterisk), which is not detectable in the glow discharge plasma. Steady-state OES studies have established preliminary correlations between SiH(asterisk) and CH(asterisk) emission intensities and the film deposition rate. Transient OES spectra of SiH4 and CH4 plasmas have shown different kinetics in SiH(asterisk) and CH(asterisk) emission intensities. Transient studies of the SiH(asterisk) emission intensity have indicated that additional mechanisms for producing the SiH(asterisk) species become evident in hydrogen-diluted silane plasmas.

Yang, C. L.↗

NASA NTRS1989

Trace gases in the atmosphere of Mars - An indicator of microbial life

The detection of certain trace gases in the atmosphere of Mars would indicate the presence of microbial life on the surface. Candidate biogenic gases include CH4, NH3, N2O, and several reduced sulfur species. Chemical thermodynamic equilibrium and photochemical calculations preclude the presence of these gases in any measurable concentrations in the atmosphere of Mars in the absence of biogenic production. A search for these gases utilizing either high-resolution (spectral and spatial) spectroscopy from a Mars orbiter, such as the Mars Observer orbiter, and/or in situ measurements from a Mars lander or rover is proposed.

Levine, Joel S.↗

NASA NTRS1989

Transport into the south polar vortex in early spring

The effect of transport on the springtime decline in ozone in the southern polar vortex was investiated using data on long-lived gas tracers (N2O, CH4, CCl4, CH3CCl3, CO, CFC-11, CFC-12, and CFC-113) obtained by the ER-2 aircraft in the period between August 23 and September 22 during the Airborne Antarctic Ozone Experiment. It was found that, while the concentrations of long-lived trace gases remained relatively constant for fixed potential temperature and latitude, the ozone mixing ratio over the same period declined by more than 50 percent inside the polar vortex near 18-km altitude. These data indicate a substantial photochemical sink of ozone. The evidence of the zero or negative time tendencies for long-lived trace gases and the meridional and vertical gradients of ozone imply that transport is supplying ozone to the polar region during springtime.

Hartmann, D. L.↗

NASA NTRS1989

Precision measurements of photoabsorption cross sections of Ar, Kr, Xe, and selected molecules at 58.4, 73.6, and 74.4 nm

Absolute absorption cross sections have been measured for the rare gases at 58.43, 73.59, and 74.37 nm with an accuracy of + or - 0.8 percent. For the molecules H2, N2, O2, CO, N2O, CO2, and CH4, precision measurements were made at 58.43 nm with an accuracy of + or - 0.8 percent. Molecular absorption cross sections are also reported at 73.59 and 74.37 nm. However, in the vicinity of these wavelengths most molecules exhibit considerable structure, and cross sections measured at these wavelengths may depend on the widths and the amounts of self-reversal of these resonance lines. A detailed discussion is given of the systematic errors encountered with the double-ion chamber used in the cross-sectional measurements. Details are also given of precision pressure measurements.

Samson, James A. R.↗

NASA NTRS1990

Upper atmosphere models and research; Proceedings of Workshops X and XI and the Topical Meeting of the 27th COSPAR Plenary Meeting, Espoo, Finland, July 18-29, 1988

Topics are presented on the updating of CIRA, the trace constituents of the middle and upper atmosphere, and the localized response of the lower thermosphere and ionosphere at high latitude. Papers are presented on mean temperature fields in the lower thermosphere, a comparison of the thermosphere total density model TD 88 with CIRA 86, improved reference models for the middle-atmosphere ozone, a reference model for CH4 and N2O and trends, reference models for thermospheric NO, and a simulation of odd nitrogen distribution in the thermosphere. Other papers are on the response of the ionosphere-thermosphere system to magnetospheric forcing, microinstabilities driven by nonthermal plasma in the high-latitude F-region, the characteristics of the high-latitude trough, the lower thermospheric coupling study of the CEDAR and WITS programs, and numerical simulations of the seasonal response of the thermosphere to propagating tides.

Rycroft, M. J.↗