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All sourcesNASA NTRSDOE OSTI
NASA NTRS1984

The evolution of the prebiotic atmosphere

One-dimensional radiative-convective and photochemical models are used to estimate the vertical temperature structure and composition of the earth's prebiotic atmosphere. Greatly enhanced CO2 levels (100-1000 times present) are required to keep the mean surface temperature above freezing in the face of decreased solar luminosity during the earth's early history. Such high CO2 partial pressures would have affected the atmospheric oxidation state by facilitating the photochemical production of soluble species including H2O2 and H2CO. Oxidation of ferrous iron in the oceans by H2O2 dissolved in rainwater should have kept the atmospheric H2 mixing ratio above 0.0002, and the ground-level O2 mixing ratio below 10 to the -11th, regardless of the magnitude of the rate of volcanic release of reduced gases.

Kasting, J. F.↗
NASA NTRS1984

Energetics of the protonation of CO - Implications for the observation of HOC(+) in dense interstellar clouds

A number of molecular species on the H3CO(+) energy hypersurface is examined. Ab initio molecular orbital theory is used to determine the structures and relative energetics of the two isomers of HCO(+) and HOC(+) together with the affinity of CO for protonation at either end. The proton affinities of H2 and H2CO are also examined. The calculations are performed using large basis sets and include the effects of electron correlation. The calculated vibrational frequencies are used to correct for zero point energy differences. The results show that the proton affinities of H2 and CO to form HOC(+) are within 1 kcal of each other. The calculations demonstrate that there is no thermodynamic driving force to form HOC(+) in collisions of H3(+) with CO, and that the formation of HCO(+) in such collisions is very exoergic. A plausible mechanism is suggested to explain the differences observed between the laboratory and the interstellar medium.

Dixon, D.↗
NASA NTRS1985

Chemistry in dynamically evolving clouds

A unified model of chemical and dynamical evolution of isolated, initially diffuse and quiescent interstellar clouds is presented. The model uses a semiempirically derived dependence of the observed cloud temperatures on the visual extinction and density. Even low-mass, low-density, diffuse clouds can collapse in this model, because the inward pressure gradient force assists gravitational contraction. In contrast, previous isothermal collapse models required the low-mass diffuse clouds to be unrealistically cold before gravitational contraction could start. Theoretically predicted dependences of the column densities of various atoms and molecules, such as C and CO, on visual extinction in diffuse clouds are in accord with observations. Similarly, the predicted dependences of the fractional abundances of various chemical species (e.g., CO, H2CO, HCN, HCO(+)) on the total hydrogen density in the core of the dense clouds also agree with observations reported to date in the literature. Compared with previous models of interstellar chemistry, the present model has the potential to explain the wide spectrum of chemical and physical properties of both diffuse and dense clouds with a common formalism employing only a few simple initial conditions.

Tarafdar, S. P.↗
NASA NTRS1986

Interstellar grain mantles

Interstellar molecular grain mantles are an important component of the interstellar dust inside dense molecular clouds as evidenced by the detection of absorption bands at 2.97, 3.08, 4.61, 6.0 and 6.8 microns. Mantles may also be the precursors of more complex grain mantles in the diffuse interstellar medium. The molecular composition of these icy grain mantles were calculated employing gas phase as well as grain surface reactions. The calculated mixtures consist mainly of the molecules H2O, H2CO, N2, CO, O2, H2O2, NH2, and their deuterated counterparts in varying ratios. The exact compositions depend strongly on the physical conditions in the gas phase. The absorption spectra of H2O with other molecules was studied in the laboratory. Optical constants were determined for a few selected mixtures. Extinction and polarization cross sections across the 3 micron ice band were calculated. A comparison with the observations towards BN shows that the low frequency wing observed on this feature is due to absorption by a mixture of H2O and other molecules rather than scattering by large, pure H2O ice grains.

Bregman, J.↗
NASA NTRS1986

Photoabsorption and photodissociation of molecules important in the interstellar medium

In the period from May 15, 1985 to May 14, 1986, the photoabsorption and photodissociation cross sections of the interstellar radical of SO and the interstellar molecules of HCl, H2CO, and CH3CN were measured and the results were reported in scientific papers. In the meantime, a windowless apparatus is used to measure the photoabsorption and photodissociation cross sections of CO in the 90-105 nm region. The optical data obtained in this research program are needed for the determination of the formation and destruction rates of molecules and radicals in the interstellar medium. Accomplishments in this research period are summarized below.

Lee, L. C.↗
NASA NTRS1985

The hydrocarbon ring C3H2 is ubiquitous in the Galaxy

The discovery of a strong microwave (1.6 cm-wavelength) spectral line, the carrier of which is common and widespread throughout the Galaxy is reported. A survey of a large number of sources shows that the line appears in emission in cold dust clouds, in absorption in the direction of the Galactic center, and exhibits complex profiles toward H II regions. Toward Cas A and distant H II regions, intervening 'spiral arm' clouds produce absorption. For almost all cases, the absorption features show a striking 1:1 radial velocity correspondence with those seen, e.g., in H2CO spectra of the same objects. The data indicate that the line arises between low-lying energy states of a rather polar molecule. Recent work by Thaddeus, Vrtilek, and Gottlieb (1985) incorporating the present data, shows that the line in question is the 1(10)-1(01) transition of the small hydrocarbon ring C3H2.

Matthews, H. E.↗
NASA NTRS1986

Pervasive small-scale structure in molecular clouds

An unbiased CO survey of molecular cloud cores was completed, and the profiles were analyzed within the context of a model for emission from clumpy clouds. It was found that all sources observed contain a significant amount of structure that is not resolved with our 2.3-arcmin beam, and that the parameters which describe the degree of clumping span a remarkably narrow range of the possible values. We studied two separate samples of cloud cores: a large sample of warm cores from the Massachusetts-Stony Brook 12CO survey of the first galactic quadrant, and a sample of cool cores in the Taurus dark clouds chosen primarily on the basis of H2CO emission. We observed all sources in the 1-0 transition of 12CO and 13CO with the 5-m telescope of the Millimeter Wave Observatory. The 12CO/13CO ratios can be explained if there is unresolved structure giving rise to significant variations of opacity across the beam. Our model cloud consists of a large number of identical clumps distributed randomly in the beam. These clumps have velocity widths v small compared to the width of the observed profile, which is determined by the relative motion of the clumps. The entire cloud is isothermal and in local thermodynamic equilibrium. With these assumptions the intensity and linewidth ratios depend on three parameters: the abundance ratio; the peak 13CO opacity through a single clump, tau(0); and the average number of clumps on a line of sight N. Small tau(0) and large N correspond to the microturbulent limit, which is indistinguishable from a uniform gas distribution. In the other extreme, large tau(0) and snall N, at a given velocity at most one clump contributes to the profile on each line of sight. A figure is presented which shows the model parameters which reproduce the measured intensity and linewidth ratios for the sample of warm cores, assuming an abundance ratio of 75.

Martin, B.↗
NASA NTRS1986

Spiral arms and massive star formation: Analysis of the CO face-on pictures of the galaxy

The face-on distribution of molecular gas in the first Galactic quadrant, derived from the Massachusetts-Stony Brook Galactic Plane CO Survey, was compared to the Galactic distribution of giant radio HII regions. The HII regions were found to preferentially select gas regions of higher than average density (more than twice the mean) and showed a strong correlation with the second power of the gas density. Systematic effects were tested with a Monte Carlo simulated HII region distribution and found to be negligible. The 135 HII regions were selected from the radio catalogs of Downes et at. (1980) and Wink et al. (1982). The HII regions were required to be within the CO survey 1 and b limits, within the solar circle, and not part of the 3 kpc expanding arm. The velocities of the HII regions were tabulated by the catalog authors and obvious associations with known objects and H2CO absorptions were used by them to assign distances. The distance assignments were here grouped into two categories; (1) those HII regions with definite distance assignments (85 objects); and (2) those HII regions with less secure distance assignments and those for which no near-far assignment was possible (50 objects).

Clemens, D. P.↗
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

Elemental, isotopic and molecular abundances in comets

The chemical composition of comet nuclei and the factors affecting it are discussed, summarizing the results of recent theoretical, experimental, and observational investigations. Consideration is given to the evidence supporting the view that the nucleus is radially differentiation (except for a thin outer layer), surface differentiation by heat processing and outgassing, and mantle buildup on an undifferentiated core. The nature of the refractory and volatile components is examined, and the elemental and isotopic compositions are given in tables and characterized. The uncertain (except for H2O) molecular composition of the volatile fraction is considered, and it is suggested that some oxides or aldehydes (such as CO, CO2, and H2CO), but no large amounts of fully hydrogenated compounds (such as CH4 and NH3) are included.

Delsemme, A. H.↗
NASA NTRS1986

Fluorescence from VUV excitation of formaldehyde

The 105-180-nm photoabsorption and fluorescence cross sections of H2CO are determined experimentally using a synchrotron-radiation light source and the apparatus described by Lee (1980). The results are presented in tables and graphs and discussed. VUV emission with threshold wavelength 140.3 nm is detected and attributed to the A 1Pi - X 1Sigma(+) system of CO, and UV emission from the HCO (B-X) system is found below a 147.5-nm threshold, the H-HCO dissociation energy having an upper limit of 3.61 + or - 0.03 eV. At 116 nm, the maximum quantum yields of the VUV and UV fluorescences are about 1.6 and 0.23 percent, respectively.

Suto, Masako↗
NASA NTRS1986

A Southern Hemisphere ammonia survey

A spectral line survey for interstellar NH3 is being carried out using the 64-m telescopes at Parkes and Tidbinbilla. Both telescopes are equipped with K-band maser receivers yielding system temperatures below 100 K. The preliminary survey is being made with the Parkes antenna (beam = 1.35 arcmin), with follow-up mapping of the more interesting sources at Tidbinbilla (beam = 0.9 arcmin). The selected sources have in general been H II regions from the H2CO surveys made at Parkes. Statistical results from initial observations of the (1,1), (2,2), and (3,3) lines in the preliminary survey are presented.

Peters, W. L.↗
NASA NTRS1988

Photochemical and thermal modeling in the early atmosphere of the earth

The simplest carbon compounds, present in the terrestrial and planetary atmospheres, exhibit a wide range of oxidation states, carbon dioxide and methane being the most oxidized and the most reduced form of carbon, respectively. The question arises as to the origin and the interconversion among the carbon species. The chemical pathways for the conversion of CH4 to CO and CO2 are for the most part known. The reverse process, the reduction of CO to CH4 is however, poorly understood. A new reaction is proposed, H2CO + H + M yields CH3O + M, which might play a fundamental role in the reduction of CO or CH4. An update is presented of nitrile photochemistry on Titan.

Yung, Yuk L.↗
NASA NTRS1988

Measurements of several atmospheric gases above the South Pole in December 1986 from high-resolution 3- to 4-micron solar spectra

This paper reports the quantitative analysis of absorption features of a number of atmospheric gases in 0.02/cm resolution 3- to 4-micron solar spectra recorded at the Amundsen-Scott South Pole Station. The measurements were obtained shortly after the austral spring ozone minimum and define, for the first time, the ambient levels of the species immediately following the breakup of the polar vortex. The retrieved total vertical column amounts in molecules per sq cm are: 2.4 + or - 0.4 x 10 to the 21st for H2(O-16), 4.5 + or - 0.5 x 10 to the 18th for H2(O-18), 3.9 + or - 0.4 x 10 to the 17th for HDO, 2.1 + or - 0.2 x 10 to the 19th for CH4, 5.1 + or - 0.5 x 10 to the 21st for CO2, 3.9 + or - 0.4 x 10 to the 18th for N2O, and 3.7 + or - 0.5 x 10 to the 15th for C2H6. Identification of (C-12)H3D absorption features and a search for H2CO absorption in the spectral data are also described.

Goldman, Aaron↗
NASA NTRS1988

Photochemical and thermal evolution of interstellar/precometary ice analogs

The photochemical and thermal evolution of H2O-, CH3OH-, NH3-, and CO-containing ices whose relative proportions in mixture are consistent with those of interstellar ice are presently studied experimentally. The UV photolysis of these ice analogs invariably generates H2CO, CO2, CO, CH4, and HCO, largely through the photofragmentation of CH3OH. CO and CH4 leave the samples as warmup proceeds to 100 K; most of the parent ice molecules are found to have sublimed upon the reaching of 200 K, with only a mixture of more refractory substances remaining. A residue of CH2 groups remains even after warmup to 300 K.

Allamandola, L. J.↗
NASA NTRS1989

Detection of the 2(0) to 3(-1) transition of C-13H3OH at 14.8 GHz

Observations of the 2(0) to 3(-1) E-type transition of C-13H3OH at 14.78 GHz have been made toward the continuum sources Sgr A, Sgr B2, and W33. For the cases of Sgr B2 and one position in Sgr A, a C-12/C-13 abundance ratio of 40 is obtained which is much higher than the values (20-25) found for other molecules. For W33, the value 50 obtained (50) is lower than that derived from H2CO observations, but is comparable to that noted from CO observations.

Kuiper, T. B. H.↗
NASA NTRS1989

Infrared fluorescence efficiencies for the nu1 and nu5 bands of formaldehyde in the solar radiation field

Formaldehyde scattering strengths have been determined for equilibrium distributions of 100 K, 50 K, 20 K, and for the the non-LTE case of an essentially fully relaxed distribution. Integrated band g factors of 2.89 x 10 to the -4th photons/s per molecule for nu1 and 3.83 x 10 to the -4th for nu 5 are obtained. The results indicate that the most promising regions to search for cometary H2CO are at about 2782/cm, at 2794.5/cm, and at about 2835/cm.

Reuter, D. C.↗
NASA NTRS1989

Correlation of molecular valence- and K-shell photoionization resonances with bond lengths

The relationship between the interatomic distance and the positions of valence-shell and K-shell sigma(asterisk) photoionization resonances is investigated theoretically for the molecules C2, F2, N2, O2, CO, NO, C2H2, C2H4, C2H6, HCN, H2CO, N20, CO2, and C2N2. The results of molecular-orbital computations are presented in three-dimensional diagrams, which are shown to be similar to the wave functions of a particle in a cylindrical well, confirming the validity of free-electron molecular-orbital (FEMO) approximations for modeling the potential along the symmetry axis. FEMO orbital energies and resonance positions are found to be in good agreement with previous theoretical and experimental results. Also included is a Feshbach-Fano analysis of the relevance of virtual-valence orbitals to the appearance of single-channel resonances in molecular photoionization cross sections.

Sheehy, J. A.↗