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NASA NTRS1975

Ultraviolet-gas phase and -photocatalytic synthesis from CO and NH3

Ammonium cyanate is identified as the major product of the photolysis of gaseous NH3-CO mixtures at 206.2 or 184.9 nm. Lesser amounts of urea, biurea, biuret semicarbazide, formamide and cyanide are observed. A series of 18 reactions underlying the formation of photolysis products is presented and discussed. Photocatalytic syntheses of C-14-urea, -formamide, and -formaldehyde are carried out through irradiation of (C-14)O and NH3 in the presence of Vycor, silica gel, or volcanic ash shale surfaces. The possible contributions of the relevant reactions to the abiotic synthesis of organic nitrogen compounds on Mars, the primitive earth, and in interstellar space are examined.

Hubbard, J. S.↗

NASA NTRS1978

NH3 in IRC plus 10216

Ammonia was detected in the circumstellar envelope of IRC +10216 by means of three infrared absorption lines in the nu sup 2 band around 950/cm. The lines are fully resolved at a resolution of 0.22 km/sec and indicate that most of the circumstellar gas is accelerated to expansion velocities around 14 km/sec within a few stellar radii. The NH3 profiles indicate a rotational temperature between 400 and 700 K, and H2 density between 10 to the 8th power/cu cm and 10 to the 10th power/cu cm, and NH3 column density of 10 to the 17th power/sq cm. The H2 density indicates that the mass of the circumstellar envelope within a 1 arcsec radius is approximately 0.1 solar masses.

Betz, A. L.↗

NASA NTRS1980

Energy transfer in NH3-He collisions

The paper presents a new electron gas intermolecular NH3-He potential determined by the Hartree-Fock results of Davis, Boggs, and Mehrotra (1979) with semiempirical long-range induction and dispersion terms. The resulting potential agrees with beam scattering and pressure broadening measurements; it was also found that the quadrupole induced dipole interaction is not as effective as the short range anisotropy. It was concluded that discrepancies remain in the quantitative description of energy transfer in the NH3-He system; discrepancies result from improper consideration of the dependence of cross-sections on degenerate magnetic quantum levels in the experimental investigation.

Green, S.↗

NASA NTRS1982

The tropospheric gas composition of Jupiter's north equatorial belt (NH3, PH3, CH3D, GeH4, H2O) and the Jovian D/H isotropic ratio

The gas composition of the troposphere of Jupiter in the clearest regions of the North Equatorial Belt (NEB) was derived from the Voyager 1 IRIS data. The infrared spectrum for this homogeneous cloud free region was modeled to infer altitude profiles for NH3, PH3, GeH4 and H2O. The Profiles for NH3 and PH3 were found to be depleted in the upper troposphere but otherwise in agreement with their solar values at the 1 bar level. The mole fraction for CH3D was determined to be 3.5(+1.0 or -1.3) x 10 to the minus 7th power. The GeH4 mole fraction of 7+ or -2 x 10 to the minus 10th power at the 2 to 3 bar level is a factor of 10 lower than the solar value. The H2O mole fraction is approximately 1 x 0.00001 at the 2.5 bar level and is increasing to approximately 3 x 0.00001 at 4 bars where it is a factor of 30 lower than solar. Using IRIS infrared values for the mole fractions of CH3D and CH4 a value of D/H = 3.6(+1.0 or -1.4)x 0.00001 is derived. Assuming this Jovian D/H ratio is representative of the protosolar nebula, and correcting for chemical galactic evolution, yields a value of 5.5 - 9.0 x 0.00001 for the primordial D/H ratio and an upper limit of 1.8 to 2.4 x 10 to the minus 31st power cu cm for the present day baryon density.

Kunde, V.↗

NASA NTRS1983

The ground state far infrared spectrum of NH3

The NH3 far infrared spectrum is particularly useful for the study of planetary composition and atmospheric dynamics. Studies of this spectrum were conducted by Dowling (1969), Helminger et al. (1971), and Urban et al. (1981). Sattler et al. (1981) have reported measurements of a few nu2 lines with tunable diode lasers. By using simple sum rules, these lines and accurate ground state inversion lines considered by Poynter and Kakar (1975) have been employed in the present investigation to deduce a few of the far infrared ground state transitions. An extensive set of high signal/noise, high resolution (0.0048 per cm) scans of the nu2 bands of NH3 from about 600 per cm through about 1300 per cm ait a series of low pressures have been made in order to accurately determine both the line positions and strengths. The obtained data provide line positions with an absolute accuracy of about 0.0001 per cm in the more favorable cases.

Poynter, R. L.↗

NASA NTRS1983

Detection of interstellar NH3 in the far-infrared - Warm and dense gas in Orion-KL

Results of an investigation are presented which show the detection of the (J,K) = a(4,3)-s(3,3) rotation-inversion transition of ammonia at 124.6 microns toward the center of the Orion-KL region. The line is found to be in emission and has a FWHM greater than or equal to 30 km/s, while the far-IR ammonia line emission probably comes mainly from the 'hot core', a compact region of warm, very dense gas previously identified by the radio inversion lines of NH3. The a(4,3)-s(3,3) line is very optically thick and it is determined that radiative excitation of the (4,3) NH3 level by far-IR emission from dust within the source can be ruled out. It is concluded that the (4,3) level is probably collisionally excited and the gas in the hot core region is warmer than the dust. Densities of approximately 10 to the 7th/cu cm are high enough to explain the observations, while shock heating by the mass outflow from IRc2 may account for the high gas temperatures in the hot core region.

Townes, C. H.↗

NASA NTRS1984

Partial phase diagram for the system NH3-H2O - The water-rich region

Phase boundaries of the H2O-NH3 system for (NH3)/x/(H2O)/1-x/ have been determined with diamond-anvil cells for mixtures in two composition ranges: (1) for x in the range from 0 to 0.3, at pressures up to 4 GPa at 21 C, and (2) for x in the range from 0.46 to 0.50, at pressures up to 5 GPa from 150 to 400 K. Phases were identified visually with a microscope and polarized optics. The NH3.2(H2O) phase is strongly anisotropic with a much smaller refractive index than that of ice VII and cracks in two nonperpendicular networks. NH3.H2O has a refractive index closer to that of Ice VII and does not appear to form cracks. Both phases are colorless. Phase boundaries were determined on both increasing and decreasing pressures, and compositions of the ammonia ices were determined by estimating relative amounts of water and ammonia ices at known overall compositions. For low-ammonia compositions (x equal to or less than 0.15), the following assemblages succedd one another as pressure increases: liquid; liquid and Ice VI (at 1.0 + GPa); liquid and Ice VII (at 2.1 GPa); Ice VII and NH3.H2O (at 3.5 GPa). For x in the range from 0.15 to 0.30, the water ice and liquid fields are replaced by the NH3.2(H2O) and liquid field at pressures down to 1.0 GPa and lower.

Johnson, M. L.↗

NASA NTRS1983

Deposition of silicon nitride from SiCl4 and NH3 in a low pressure RF plasma

Silicon nitride coatings were deposited in a low-pressure (1-10 Torr) RF plasma from SiCl4 and NH3 in the presence of argon onto stainless martensitic steel grounded and floating substrates at 300 C and 440 C respectively. The heating of the substrates depends mainly on the position and the induced RF power. The coatings were identified as silicon nitride by X-ray investigation and were found to contain chlorine by energy-dispersive analysis of X-rays. The growth rate, the microhardness and the chlorine concentration of the coatings were determined as a function of the total gas pressure, the RF power input and the NH3-to-SiCl4 ratio. It was observed that the coatings on the floating substrates have higher deposition rates and are of superior quality.

Ron, Y.↗

NASA NTRS1986

Constraints on the NH3 and PH3 distributions in the Great Red Spot

Medium resolution (10 A) UV spectra were obtained for the Great Red Spot (GRS) and South Tropical Zone (STZ) of Jupiter using the low dispersion mode of the IUE spectrometers at wavelengths from 1900-2200 A. The scans were carried out to determine the coloring agent for the GRS to improve the database for developing photochemical models of the feature. The wavelengths were selected to cover the absorption features of NH3 and PH3. The resulting data were interpreted using a vertically inhomogeneous Rayleigh scattering radiative transfer model. Various NH3 concentrations were explored in an effort to fit the data, taking into account changes which would occur at different atmospheric pressure levels and due to the projected temperature fields. A forbidden NH3/forbidden H2 mixing ratio that was calculated at the 80-125 mbar pressure level in the GRS was enhanced by 3-10 percent relative to the STZ. An upper limit was obtained for the mixing ratio of PH3 in the GRS that is significantly lower than previously predicted concentrations, implying that vertical transport in the GRS is not much greater than in adjacent regions.

Wagener, R.↗

NASA NTRS1987

The production of NH(A 3Pi i) through photodissociative excitation of NH3

The NH(A-X) emission produced by photodissociation of NH3 is examined using a line emission source in the 600-1340 A region. It is observed that the production of the NH(A 3Pi i) photofragment involves a spin-forbidden transition. Fluorescence spectra of NH3 are derived and analyzed. The relationship between fluorescence cross sections and fluorescence count rates and gas pressure is studied. The fluorescence cross sections of NH(A-X) are calculated as 2.1 x 10 to the -22nd, 3.1 x 10 to the -22nd, 3.0 x 10 to the -21st, 1.5 x 10 to the -20th, and 3.4 x 10 to the -20th sq cm for the primary photon wavelength of 1239, 1184, 1065, 1037, and 976 A, respectively; and the corresponding fluorescence quantum yields are 0.00002, 0.00003, 0.0012, 0.0085, and 0.015.

Wu, C. Y. Robert↗

NASA NTRS1989

NH3 column abundances over Lauder, New Zealand

Gaseous NH3 has been observed in the atmosphere over central New Zealand with infrared absorption spectra. The amount of NH3 shows marked variability, which is strongly correlated with time of day and season. The pattern is similar to data obtained in Denver, Colorado, but is much more variable than data from Hampton, Virginia. The rapid variability indicates a residence time of 8 hours in some cases.

Murcray, Frank J.↗

NASA NTRS1989

NH2 fluorescence efficiencies and the NH3 abundance in Comet Halley

If NH3 is the dominant source of the NH2 observed in comet spectra, then the NH3 abundance can in principle be accurately determined. Fluorescence efficiencies for the (0, v-prime/2/, O) to (0, 0, 0) progression of NH2 bands are calculated for NH2 bands likely to be observed in the 4500-8200-A region of comets. The results differ from previous determinations of the NH2 band fluorescence efficiencies by factors in the range 1.4-5.9, leading t6o significant changes in previously reported NH2 production rates in comets. A recalculation of the NH3/H2O abundance ratio in Comet Halley gives about (0.5 + or - 0.2) percent in better agreement with the Giotto ion-mass-spectrometer results of Allen et al (1987).

Tegler, Stephen↗

NASA NTRS1991

Photoabsorption and photoionization cross sections of NH3, PH3, H2S, C2H2, and C2H4 in the VUV region

Using synchrotron radiation as a continuum light source, the photoabsorption and photoionization cross sections of NH3, PH3, H2S, C2H2, and C2H4 have been measured from their respective ionization thresholds to 1060 A. The vibrational constants associated with the nu(2) totally symmetric, out-of-plane bending vibration of the ground electronic state of PH3(+) have been obtained. The cross sections and quantum yields for producing neutral products through photoexcitation of these molecules in the given spectral regions have also been determined. In the present work, autoionization processes were found to be less important than dissociation and predissociation processes in NH3, PH3, and C2H4. Several experimental techniques have been employed in order to examine the various possible systematic errors critically.

Xia, T. J.↗

NASA NTRS1991

Calculations on the rate of the ion-molecule reaction between NH3(+) and H2

The rate coefficient for the ion-molecule reaction NH3(+) + H2 yields NH4(+) + H has been calculated as a function of temperature with the use of the statistical phase space approach. The potential surface and reaction complex and transition state parameters used in the calculation have been taken from ab initio quantum chemical calculations. The calculated rate coefficient has been found to mimic the unusual temperature dependence measured in the laboratory, in which the rate coefficient decreases with decreasing temperature until 50-100 K and then increases at still lower temperatures. Quantitative agreement between experimental and theoretical rate coefficients is satisfactory given the uncertainties in the ab initio results and in the dynamics calculations. The rate coefficient for the unusual three-body process NH3(+) + H2 + He yields NH4(+) + H + He has also been calculated as a function of temperature and the result found to agree well with a previous laboratory determination.

Herbst, Eric↗

NASA NTRS1991

Modeling of Jupiter's millimeter wave emission utilizing laboratory measurements of ammonia (NH3) opacity

The techniques used to make laboratory measurements of the millimeter wave opacity from gaseous ammonia under simulated Jovian conditions are described. The results are applied to a radiative transfer model, which is used to compute Jupiter's millimeter wavelength emission. The absorptivity of gaseous NH3 is measured to reduce one of the largest uncertainties in modeling Jupiter's millimeter wave emission. Several other millimeter wave opacity sources are examined. New expressions are given for computing the absorptivity of NH3, H2O, cloud condensates, and pressure-induced absorption. Jupiter's reliable millimeter wavelength observations are compared with synthetic emission spectra which utilize these new absorption expressions.

Joiner, Joanna↗

NASA NTRS1992

NH3 and NH2 in the coma of Comet Brorsen-Metcalf

Evidence consistent with NH3 ice in the nucleus of Comet Brorsen-Metcalf as the source of the NH2 observed in the comet coma is presented. The distribution of NH2 is symmetric and shows no evidence for jet structure at the 3-sigma significance level above background emission. An azimuthal average of the NH2 image produces an NH2 surface brightness profile for Comet Brorsen-Metcalf which yields a factor of about-10 improvement in the signal-to-noise ratio over previous 1D long-slit NH2 observations, and provides a significant constraint on the NH2 photodissociation time scale in comets. A Monte Carlo simulation of the comet coma, assuming that NH2 is the primary source of NH2, is described and compared with the observations. For an observed production rate, Q(H2O) is approximately equal to 7 x 10 exp 28 molecules/s, collisional effects on the NH3 and NH2 outflow had at most an approximately 10-percent effect on the NH2 surface brightness profile. Because Comet Brorsen-Metcalf showed no significant dust or gas production rate variability, it is argued that steady state conditions best match the comet at the time of the observations.

Tegler, Stephen C.↗

NASA NTRS1992

The photolysis of NH3 in the presence of substituted acetylenes - A possible source of oligomers and HCN on Jupiter

An NMR spectral study is presently conducted of NH3 photolysis in the presence of substituted acetylenes with NMR spectra and gas chromatography. Quantum yields and percentage conversions to products are reported. It is shown that acetylenic hydrocarbons generated during methane photolysis in Jupiter's stratosphere can react with radicals formed by NH3 photolysis to yield nonvolatile, yellow-brown polymers, alkylnitriles, and in due course, HCN, as observed on Jupiter.

Ferris, James P.↗

NASA NTRS2000

On the reaction CH2O + NH3 Yields CH2NH + H2O

We study the energetics of CH2O + NH3-Yields CH2NH + H2O in the gas phase at the B3LYP and CCSD(T)levels. This reaction is shown to have a sizeable barrier. Ionization of NH3 reduces the barrier to about 5 kcal/mol. We also show that in water, a proton catalyzed mechanism yields no barriers in excess of the reaction endothermicity. Since this reaction has been proposed as one of the steps in interstellar synthesis of glycine, the simplest amino acid, this work suggests that the formation of amino acids is occurring in and/or on interstellar water ice grains, and not in the gas phase.

Walch, Stephen P.↗