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NASA NTRS1976

Reaction of NH2 with NO and O2

Experiments were performed on the photooxidation of NH3 at room temperature and the photolysis of NH3-NO mixtures in order to determine the reaction paths of NH2 with O2. NH3 was photolyzed (NH3 + E yields NH2 + H) in the presence of O2 above 0.6 torr at 213.9 nm and 25 C, producing N2 and N2O. Only N2 and N2O were produced with any significant quantum yield, and their quantum yield was invariant with reaction conditions, which imposes a great number of constraints reducing the number of possible reactions greatly. It is argued that the N2 must be produced from the NH2O2 radical which was produced by the reaction between NH2 and O2. Subsequent reactions leading to N2 and N2O are speculative. In the photolysis of NH3 in the presence of NO and NO-O2 mixtures, the products identified were N2, H2, and N2O. Without the presence of O2, the reaction scheme after photolysis is (2) NH2 + NO yields N2 + H2O, (3) H + NO + M yields HNO + M, (4) H + HNO yields H2 + NO, and (5) 2HNO yields N2O + H2O. The average value for the ratio k3 times the square root of k5 divided by k4 was computed to be (1.6 plus or minus 0.6) times 10 to the minus 28th cm to the exponent 9/2 per square root sec. In addition, the presence of 113 mtorr of O2 had no effect on the quantum yields of N2 or H2, so it appears that it does not deactivate electronically excited NH3.

Jayanty, R. K. M.↗

NASA NTRS1976

A new estimate of volatile outgassing on Mars

The presence of 28% argon on Mars, as calculated by Levine and Riegler (1974) and indirectly inferred from Soviet Mars-6 lander data, has important implications for the outgassing history of H2O, CO2, and N2 on Mars. Even if the terrestrial volatile outgassing ratio is only approximately valid for Mars, then large quantities of H2O (of the order of 100,000 g/sq cm), about 10,000 g/sq cm of CO2 (about 1000 times more CO2 than found at present in the Martian atmosphere), and some 450 g/sq cm of N2 may have outgassed over the history of Mars.

Levine, J. S.↗

NASA NTRS1976

Effect of water vapor on the destruction of ozone in the stratosphere perturbed by ClX or NOx pollutants

Results are presented for a self-consistent one-dimensional coupled flow calculation for Ox, NOx, HOx, ClX, H2O, H2, CH4, H2O2, and N2O densities between 10 and 120 km. The results agree well with observations for the normal midlatitude atmosphere over this altitude range. ClX, NOx, and H2O are varied independently in the model considered. It is shown that the effect of depletion of ozone by ClX is to remove ozone preferentially above 30 km and to lower the altitude of maximum ozone density. This leads to enhanced solar heating of the lower stratosphere and tropopause and suggests the possibility of an increased flux of water into the stratosphere. Increasing water vapor in the stratosphere greatly enhances the rate of destruction of O3 by ClX and also causes an increase in the rate of destruction of O3 in the NOx-perturbed atmosphere.

Liu, S. C.↗

NASA NTRS1976

Vibrational and rotational relaxation in mixtures of water vapor and oxygen

Experimental measurements of sound absorption in air, measurements of ultrasonic absorption in H2O/O2 mixtures at 500 K, and experimental measurements in mixtures of H2O with other impurities have been analyzed to determine the energy transfer rates in mixtures of O2 and H2O as a function of temperature. A set of energy transfer rate coefficients was found that give results consistent with all the experimental data examined and with vibrational energy transfer theory. The rotational relaxation time for H2O/O2 mixtures was determined from the 500 K ultrasonic measurements.

Bass, H. E.↗

NASA NTRS1977

Gaseous sodium sulfate formation in flames and flowing gas environments

Formation of Na2SO4(g) in flames and hot flowing gas systems was studied by high pressure, free-jet expansion, modulated molecular beam mass spectrometric sampling. Fuel-lean CH4-O2 flames doped with SO2, H2O and NaCl yielded the gaseous Na2SO4 molecule in residence times of less than one millisecond. Intermediate species NaSO2(g) and NaSO3(g) were also observed and measured. Composition profiles were obtained for all reaction products. Nonflame flowing gas experiments showed that Na2SO4 and NaSO3 gaseous molecules were formed at 1140 C in mixtures of O2, H2O(g), SO2 and NaCl(g). Experimental results are compared with calculated equilibrium thermodynamic predictions.

Stearns, C. A.↗

NASA NTRS1976

Calculations of molecular ionization energies using a self-consistent-charge Hartree-Fock-Slater method

A numerical-variational method for performing self-consistent molecular calculations in the Hartree-Fock-Slater (HFS) model is presented. Molecular wavefunctions are expanded in terms of basis sets constructed from numerical HFS solutions of selected one-center atomlike problems. Binding energies and wavefunctions for the molecules are generated using a discrete variational method for a given molecular potential. In the self-consistent-charge (SCC) approximation to the complete self-consistent-field (SCF) method, results of a Mulliken population analysis of the molecular eigenfunctions are used in each iteration to produce 'atomic' occupation numbers. The simplest SCC potential is then obtained from overlapping spherical atomlike charge distributions. Molecular ionization energies are calculated using the transition-state procedure; results are given for CO, H2O, H2S, AlCl, InCl, and the Ni5O surface complex. Agreement between experimental and theoretical ionization energies for the free-molecule valence levels is generally within 1 eV. The simple SCC procedure gives a reasonably good approximation to the molecular potential, as shown by comparison with experiment, and with complete SCF calculations for CO, H2O, and H2S.

Rosen, A.↗

NASA NTRS1976

Ultraviolet stellar occultation measurement of the H2 and O2 densities near 100 km in the earth's atmosphere

Results are presented for an experimental study designed to measure the density of H2 near 100 km in the earth's atmosphere from occultation of a star, Gamma Vel, by the earth's atmosphere at several wavelengths near the H2 absorption line at 1108.128 A by a spectrometer on an orbiting astronomical observatory. Measurement of the O2 density between 95 and 123 km is also reported. Attention is focused on testing the predictions of a model of the distribution of hydrogen constituents, H, H2, H2O, CH4, OH, and H2O in the upper atmosphere related to a theory of hydrogen escape developed by Hunten and Strobel (1974) and by Liu and Donahue (1974). The measured H2 densities are found to be in good agreement with recent theoretical predictions, whereas the measured O2 density profile generally agrees with the models except for a wavelike structure in the range 104-114 km.

Atreya, S. K.↗

NASA NTRS1976

Cosmic ray interactions with lunar materials - Nature and composition of species formed

The paper discusses the effect of cosmic-ray proton interactions with lunar material, the nature and composition of the species resulting from these interactions, and the contribution of these species to the lunar atmosphere. It is shown that hydrogen atoms resulting from cosmic-ray proton neutralization escape into the atmosphere mostly as H2, that only a small fraction of the very small amount of OH and H2O produced by cosmic-ray protons escapes into the atmosphere, and that cosmic-ray protons play a very minor role, as compared with solar-wind protons, in producing lunar atmospheric hydrogen and hydrogenated species. It is concluded that the atmospheric contributions of H2, H, OH, and H2O produced by cosmic-ray protons are about three orders of magnitude less than those due to solar-wind protons.

Mukherjee, N. R.↗

NASA NTRS1977

Photometric imaging of Mars during the 1973 opposition

The paper discusses imaging of Mars at 20 wavelengths in the spectral region from 0.35 to 1.10 microns performed during the 1973 opposition with a photometric imaging system that uses a silicon vidicon tube as the detector. The imaging system and data-reduction procedures are described in detail, and relative reflectance spectra for several small areas in the images are presented along with vidicon images obtained during early phases in the development of the 1973 dust storms. Several anomalous blue brightenings are examined and attributed to ground fog and H2O frost. It is suggested that anomalously large amounts of H2O were pulsed into the atmosphere from the regolith by the storm system. An apparent fading and recession of the north polar hood is noted, surface units revealed in contrast-enhanced ratio images are identified, and the need for higher-spatial-resolution orbital spectroscopy of dark areas is emphasized.

Mccord, T. B.↗

NASA NTRS1977

Gaseous sodium sulfate formation in flames and flowing gas environments

Formation of Na2SO4(g) in flames and hot flowing gas systems was studied by high pressure, free-jet expansion, modulated molecular beam mass spectrometric sampling. Fuel-lean CH4-O2 flames doped with SO2, H2O and NaCl yielded the gaseous Na2SO4 molecule in residence times of less than one millisecond. Intermediate species NaSO2(g) and NaSO3(g) were also observed and measured. Composition profiles were obtained for all reaction products. Non-flame flowing gas experiments showed that Na2SO4 and NaSO3 gaseous molecules were formed at 1140 C in mixtures of O2, H2O(g), SO2 and and NaCl(g). Experimental results are compared with calculated equilibrium thermodynamic predictions.

Stearns, C. A.↗

NASA NTRS1977

Flight IV technical report for experiment 74-37 contained polycrystalline solidification in low-G

Experiments were performed to study the effect of a low-gravity environment on the columnar-to-equiaxed transition (CET) during polycrystalline solidification. Solutions of H2O-30 wt% NH4Cl and H2O-37 wt% NH4Cl were solidified in semicylindrical molds with radial heat extraction. Both solutions were quenched from the same soak temperature (90 C); the respective superheat temperatures were, therefore, approximately 57 and 23 C. The lower superheat resulted in a completely columnar structure, and the higher superheat resulted in a 1/3 columnar - 2/3 equiaxed microstructure; these results were independent of the relationship between heat flow direction and gravity. Grain multiplication mechanisms observed were showering, thermal inversion driven convection cells, and compositionally induced density inversion driven convection cells.

Papazian, J. M.↗

NASA NTRS1977

The energetics of molecular clouds. I - Methods of analysis and application to the S255 molecular cloud

Observations of the S255 molecular cloud in the radio lines of CO, (C-13)O, and H2O as well as in the IR region from 12 to 20 microns are presented. These results show that an extended molecular cloud is associated with the optically visible H II regions S255 - S257, both the kinetic temperature and molecular density are enhanced in an area centered on a compact near-IR source, this source is also coincident with an OH and an H2O maser (within the errors), and the IR source exhibits the silicon absorption feature. First-order techniques which allow physical properties of molecular clouds to be estimated and the energetics of the gas and dust in the clouds to be analyzed are developed and applied to S255. It is concluded that: (1) the gas cooling rate is much less than the dust cooling rate; (2) the primary energy flow is in the IR through dust emission over a range of temperatures; (3) the near-IR source is apparently responsible for the local peak in gas kinetic temperature; and (4) the exciting stars of nearby H II regions appear to be the primary heat sources for the overall molecular cloud.

Evans, N. J., II↗

NASA NTRS1978

Airborne infrared spectrophotometry of Mira variables

Airborne spectrophotometric observations of R Cas near minimum and maximum light, R Leo near minimum, and NML Tau near maximum are reported which were obtained over the wavelength range from 1.2 to 4 microns with 1.5% resolution. The spectral energy distributions of the three stars at the indicated times are presented, and it is shown that the H2O bands at 1.4, 1.9, and 2.7 microns are clearly evident in all the spectra, while the absorption bands of CO at about 1.6 and 2.3 microns are probably present although they are masked by the strong water vapor features. The results indicate that water vapor is the dominant opacity source in the atmospheres of Mira variables, that R Leo and NML Tau may be fitted well over the entire spectrum by respective single temperatures of 2250 and 1800 K, and that R Cas near both minimum and maximum cannot be adequately described by one temperature over the entire wavelength range investigated. The shapes and depths of the absorption bands are determined together with the apparent angular diameter of each star and the equivalent widths of the H2O + CO absorption bands. It is concluded that water vapor absorption is more strongly correlated with color temperature than with spectral type for R Cas and R Leo.

Strecker, D. W.↗

NASA NTRS1978

Artificially created holes in the ionosphere

The artificial creation of ionospheric holes by the release of highly reactive molecules into the F region is investigated. Through ion-atom interchange or charge transfer reactions, H2 or H2O reacts with O(+) to form OH(+) or H2O(+), respectively, which subsequently dissociatively recombines with electrons at a very rapid rate. The diffusion of H2 is also modified by chemical loss to the ambient atomic oxygen atmosphere. The limited spatial and temporal extent of the hole-making process allows several approximations to be made which permit three-dimensional analytic solutions of the continuity equations for the released particles, the O(+) and e(-) densities, and the intermediary molecular ions. A versatile formalism is developed whereby the hole-making capability of virtually any spatial-temporal configuration of released particles can be determined by convolving a set of destruction operators which can be viewed as Green's functions for the problem. As a specific application of the techniques developed, the modification of a winter nighttime ionosphere is described by simulating the release of 1000 kg of water vapor near a height of 300 km.

Mendillo, M.↗

NASA NTRS1977

Interaction of NaCl/g/ and HCl/g/ with condensed Na2SO4

Na2SO4(l)-NaCl(g) interactions were studied at a total pressure of one atmosphere of air or oxygen for various temperatures of Na2SO4(l) and for various partial pressures of NaCl(g) and H2O(g). Mass spectrometric sampling techniques were used to identify and monitor gas phase species. Continuous recording thermomicrogravimetric measurements were conducted to determine condensed phase weight change rates. Experimental measurements were supplemented with thermodynamic calculations. Numerous experiments were performed at sample temperatures of 900 and 1000 C with 300 ppm NaCl(g). In these experiments, the reproducibility of the Na2SO4 vaporization weight loss rate and initial weight gain upon addition of NaCl(g) were found to be satisfactory. It was found that the addition of NaCl(g) to air flowing over Na2SO4(l) at 900 and 1000 C enhances the rate of weight loss of the Na2SO4(l). This enhancement increases when H2O(g) is also added to the air flow.

Stearns, C. A.↗

NASA NTRS1978

O/S-1/ interactions - The product channels

The first measurements are reported of the reaction pathways for the interaction between oxygen atoms in the 4.19 eV S-1 state, and four molecules, N2O, CO2, H2O, and NO. Distinction is made between three possible paths - quenching to O(D-1), quenching to O(P-3), and chemical reaction. With N2O, the most reasonable interpretation of the data indicates that there no reaction, in sharp contrast with the interaction between O(D-1) and N2O, which proceeds entirely by reaction. Similarly, there is no reaction with CO2. With H2O, the reactive pathway is the dominant one, although electronic quenching is not negligible. With NO, O(D-1) is the preferred product.

Slanger, T. G.↗

NASA NTRS1978

Airglow from the inner comas of comets

The intensities of radiation from the inner comas of comets which are composed primarily of water and carbon monoxide have been calculated. Only 'airglow' emissions initiated by the absorption of EUV radiation have been considered. The photoionizations of H2O, CO, CO2, and N2 are the most important emission sources, although photoelectron excitation is also considered. Among the emission features for which intensities were calculated are H2O(+), CO(+) (first negative), CO (fourth positive), CO (Cameron), CO2(+), N2 (Vegard-Kaplan), N2(+) (first negative), and O I (1304 A). In the inner coma (collision region) these airglow mechanisms are shown to be possible competitors with the usually assumed resonance-scattering and fluorescence-excitation mechanisms appropriate for the outer coma and tail.

Cravens, T. E.↗

NASA NTRS1978

Oxygen fugacity of basaltic magmas and the role of gas-forming elements

It is suggested that major variations in the relative oxygen fugacity of a basaltic magma are caused primarily by gas-forming elements, especially carbon and hydrogen. According to this theory, carbon, present in the source region of a basaltic magma, reduces the host magma during ascent, as isothermally carbon becomes more reducing with decreasing pressure. For an anhydrous magma such as lunar basalts, this reduction continues through the extrusive phase and the relative oxygen fugacity decreases rapidly until buffered by the precipitation of a metallic phase. For hydrous magmas such as terrestrial basalts, reduction by carbon is eventually superceded by oxidation due to loss of H2 generated by the reaction of C with H2O and by thermal dissociation of H2O. The relative oxygen fugacity of a hydrous magma initially decreases as a magma ascends from the source region and then increases until magnetite crystallization curbs the rising trend of the relative oxygen fugacity.

Sato, M.↗