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NASA NTRS1998

Infrared Space Observatory Observations of Molecular Hydrogen in HH 54: Measurement of a Nonequilibrium Ratio of Ortho- to Para-H2

We have detected the S(1), S(2), S(3), S(4), and S(5) pure rotational lines of molecular hydrogen toward the outflow source HH 54 using the Short Wavelength Spectrometer on board the Infrared Space Observatory. The observed H2 line ratios indicate the presence of warm molecular gas with an H2 density of at least 10(exp 5) cm(exp -3) and a temperature approximately 650 K in which the ratio of ortho- to para-H2 is only 1.2 +/- 0.4, significantly smaller than the equilibrium ratio of 3 expected in gas at that temperature. These observations imply that the measured ratio of ortho- to para-H2 is the legacy of an earlier stage in the thermal history of the gas when the gas had reached equilibrium at a temperature approximately less than 90 K. Based upon the expected timescale for equilibration, we argue that the nonequilibrium ratio of ortho- to para-H2 observed in HH 54 serves as a chronometer that places a conservative upper limit of approximately 5000 yr on the period for which the emitting gas has been warm. The S(2)/S(1) and S(3)/S(1) H2 line ratios measured toward HH 54 are consistent with recent theoretical models of Timmermann for the conversion of para- to ortho-H2 behind slow, C-type shocks, but only if the preshock ratio of ortho- to para-H2 was approximately less than 0.2.

Neufeld, David A.↗
NASA NTRS2001

H2 cycling and microbial bioenergetics in anoxic sediments

The simple biochemistry of H2 is central to a large number of microbial processes, affecting the interaction of organisms with each other and with the environment. In anoxic sediments, the great majority of microbial redox processes involve H2 as a reactant, product, or potential by-product, and the thermodynamics of these processes are thus highly sensitive to fluctuations in environmental H2 concentrations. In turn, H2 concentrations are controlled by the activity of H2-consuming microorganisms, which efficiently utilize this substrate down to levels which correspond to their bioenergetic limitations. Consequently, any environmental change which impacts the thermodynamics of H2-consuming organisms is mirrored by a corresponding change in H2 concentrations. This phenomenon is illustrated in anoxic sediments from Cape Lookout Bight, NC, USA: H2 concentrations are controlled by a suite of environmental parameters (e.g., temperature, sulfate concentrations) in a fashion which can be quantitatively described by a simple thermodynamic model. These findings allow us to calculate the apparent minimum quantity of biologically useful energy in situ. We find that sulfate reducing bacteria are not active at energy yields below -18 kJ per mole sulfate, while methanogenic archaea exhibit a minimum close to -10 kJ per mole methane.

Hoehler, Tori M.↗
NASA NTRS2004

Quantitative Relationships between Photosynthetic, Nitrogen Fixing, and Fermentative H2 Metabolism in a Photosynthetic Microbial Mat

The ultimate potential of any microbial ecosystem to contribute chemically to its environment - and therefore, to impact planetary biogeochemistry or to generate recognizable biosignatures - depends not only on the individual metabolic capabilities of constituent organisms, but also on how those capabilities are expressed through interactions with neighboring organisms. This is particularly important for microbial mats, which compress an extremely broad range of metabolic potential into a small and dynamic system. H2 participates in many of these metabolic processes, including the major elemental cycling processes of photosynthesis, nitrogen fixation, sulfate reduction, and fermentation, and may therefore serve as a mediator of microbial interactions within the mat system. Collectively, the requirements of energy, electron transfer, and biomass element stoichiometry suggest quantitative relationships among the major element cycling processes, as regards H2 metabolism We determined experimentally the major contributions to 32 cycling in hypersaline microbial mats from Baja California, Mexico, and compared them to predicted relationships. Fermentation under dark, anoxic conditions is quantitatively the most important mechanism of H2 production, consistent with expectations for non-heterocystous mats such as those under study. Up to 16% of reducing equivalents fixed by photosynthesis during the day may be released by this mechanism. The direct contribution of nitrogen fixation to H2 production is small in comparison, but this process may indirectly stimulate substantial H2 generation, by requiring higher rates of fermentation. Sulfate reduction, aerobic consumption, diffusive and ebulitive loss, and possibly H2-based photoreduction of CO2 serve as the principal H2 sinks. Collectively, these processes interact to create an orders-of-magnitude daily variation in H2 concentrations and fluxes, and thereby in the oxidation-reduction potential that is imposed on microbial processes occuring within the mat matrix.

Hoehler, Tori M.↗
NASA NTRS1974

Neptune - Observations of the H2 quadrupole lines in the /4-0/ band

The first measurement of Neptune's quadrupole H2 lines is reported. The equivalent widths of the S(0) and S(1) lines of the (4-0) band are given along with the corresponding widths measured from comparison spectra of Uranus taken on the same nights. These are interpreted in terms of both an inhomogeneous atmosphere overlying a reflecting layer and a homogeneous, semi-infinite, scattering atmosphere. Only the scattering model proves to be consistent with Neptune's spectrum in this wavelength region. The H2 abundance along the scattering mean free path is found to be less than the value for Rayleigh scattering in pure H2. This result is interpreted in terms of the presence of H2, CH4, and at least one other gas, instead of the more conventional interpretation in terms of the presence of an aerosol mixed with H2. Weak features in the continuum were observed. Their widths and the strength of the H2 features indicate that H2 is more abundant than the sum of the remaining gases in these atmospheres.

Trafton, L.↗
NASA NTRS1978

H2 cooling, dissociation, and infrared emission in shocked molecular clouds

Models are presented of interstellar shocks in molecular clouds over ranges of ambient molecular density from 1000 to 10 million per cu cm and shock velocity from 6 to 14 km/s. Estimates of H2-H2 collisional-excitation rates are used to derive the H2 radiative cooling rates from vibrational-rotational quadrupole transitions as a function of n(H2) and temperature. The emissivities integrated through the shock of the strongest infrared lines in the v = 1-0, 2-0, and 2-1 bands of H2. The effectiveness of H2 dissociative cooling is considered for the highest-velocity shocks. The H2 line intensities from such shocks are compared with those produced by the 'competitive' mechanism of UV pumping for two likely driving mechanisms of shocks - wind-driven shells and expanding H II regions.

Shull, J. M.↗
NASA NTRS1995

Hopkins Ultraviolet Telescope observations of H2 toward the planetary nebula NGC 1535

We have observed the far-ultraviolet spectrum (912-1860 A) of the bright high-excitation planetary nebula NGC 1535 with approximately 3 A resolution using the Hopkins Ultraviolet Telescope (HUT) aboard the Astro-1 space shuttle pmission in 1990 December. We see strong continuum emission down to the Lyman limit and strong P Cygni profiles from high-excitation lines such as C IV wavelength 1549, N V wavelength 1240, O V wavelength 1371, and O VI wavelength 1035. Below 1150 A strong absorption bands of H2 are seen, which were unanticipated by us because of the low reddening and high galactic latitude of the object and the absence of detected H2 emission in the infrared. We construct model H2 spectra and convolve them to the HUT resolution for comparison with the NGC 1535 data. We find good agreement with a population distribution characterized by a single temperature (T = 300 K) or a two-temperature model (T = 144/500 K), and determine limits on the H2 column density. While both inter-stellar and circumstellar origins for the observed H2 absorption are plausible, we ascribe the material to the planetary nebula in order to estimate the conditions of excitation and place upper limits on the mass of both H2 and H1 in this system. Because the UV transitions are ground-state connected, we determine a stringent upper limit of 0.03 d(sup 2)(sub 1.6) solar mass on the mass of H2, where d(sub 1.6) is the distance relative to an assumed distance of 1.6 kpc. This value is less model-dependent than IR estimates. Along with the central star and nebular masses, these estimates allow us to limit the main-sequence mass of the progenitor star to less than 1.8 solar mass. This upper limit is consistent with a relatively low-mass extended thick disk or Population II progenitor, as expected for an object approximately 1 kpc off the galactic plane.

Bowers, Charles W.↗
NASA NTRS1995

Structure of V(H2)n(+) Clusters for n = 1-6

Geometries, vibrational frequencies, spin states, H2 binding energies, and Delta(S) values have been determined for V(H2)n(+), for n = 1-6, using the B3LYP hybrid functional. The binding energies and Delta(S) values are in good agreement with experiment, thus showing that the B3LYP functional offers a reliable approach for optimizing the geometry and determining the H2 binding energies for this system. The calculations show that the increase in the binding energy and entropy associated with the addition of the sixth H2 to V(+) is due to a change in spin state from quintet for the smaller clusters to triplet for V(H2)6(+). The results for V(H2)n(+) are compared with those for CO(H2)n(+).

Maitre, Philippe↗
NASA NTRS1996

Rate Coefficients of C2H with C2H4, C2H6, and H2 from 150 to 359 K

Rate coefficients for the reactions C2H with C2H4, C2H6, and H2 are measured over the temperature range 150-359 K using transient infrared laser absorption spectroscopy. The ethynyl radical is formed by photolysis of C2H2 with a pulsed excimer laser at 193 nm, and its transient absorption is monitored with a color center laser on the Q(sub 11)(9) line of the A(sup 2) Pi-Chi(sup 2) Sigma transition at 3593.68 cm(exp -1). Over the experimental temperature range 150-359 K the rate constants of C2H with C2H4, C2H6, and H2 can be fitted to the Arrhenius expressions k(sub C2H4) = (7.8 +/- 0.6) x 10(exp -11) exp[(134 +/- 44)/T], k(sub C2H6) = (3.5 +/- 0.3) x 10(exp -11) exp[(2.9 +/- 16)/T], and k(sub H2) = (1.2 +/- 0.3) x 10(exp -11) exp[(-998 +/- 57)]/T cm(exp 3) molecule(exp -1) sec(exp -1). The data for C2H with C2H4 and C2H6 indicate a negligible activation energy to product formation shown by the mild negative temperature dependence of both reactions. When the H2 data are plotted together with the most recent high-temperature results from 295 to 854 K, a slight curvature is observed. The H2 data can be fit to the non-Arrhenius form k(sub H2) = 9.2 x 10(exp -18) T(sup 2.17 +/- 0.50) exp[(-478 +/- 165)/T] cm(exp 3) molecules(exp -1) sec(exp -1). The curvature in the Arrhenius plot is discussed in terms of both quantum mechanical tunneling of the H atom from H2 to the C2H radical and bending mode contributions to the partition function.

Opansky, Brian J.↗
NASA NTRS1977

Saturn - Long-term variation of H2 and CH4 absorptions

Results are presented for observations of various H2 quadrupole lines and CH4 absorption bands in spectra of Saturn obtained with a coude scanner at each apparition since 1969. The data are found to indicate a long-term variation in Saturn's H2 equivalent widths, a seasonal dependence of H2 line strength, and a fairly steady increase in CH4 absorption during the period from 1973 to 1976. A possible correlation between planetary shading and the strength of H2 absorption features is discussed along with seasonal variations in Saturn's NH3 cloud deck and atmospheric models that correspond to the observed H2 equivalent widths. It is suggested that: (1) significant shadowing by the rings may cause dynamical atmospheric activity due to the occurrence of a temperature gradient in the penumbral boundaries of the ring shadow in the planet's upper atmosphere; (2) cooling in the shadow may be a source of a high-altitude CH4 mist; and (3) spreading of this mist over the globe by advective winds would reduce the H2 and CH4 absorptions, as observed.

Trafton, L.↗
NASA NTRS1981

H2 abundance in the atmosphere of Venus

The in situ measurements from the Pioneer Venus Orbiter (PVO) Ion Mass Spectrometer have led to the detection of H2(+) ions in the Venus ionosphere. Although H2(+) is a minor ion, its measurement provides the first direct clue for determining the H2 abundance in the upper atmosphere of Venus. A photochemical model using PVO measurements is used to derive an H2 mixing ratio of 10 ppm below 140 km altitude. The presence of this much H2 confirms a previous prediction that the reactions of O(+) with H2 and subsequent recombination of OH(+) provide an important source of nonthermal H observed in the Venus atmosphere. The estimated escape flux for H is 10 to the 8th per sq cm/s.

Kumar, S.↗
NASA NTRS1987

Measurement and analysis of the far infrared absorption spectrum of the gaseous mixture H2-CH4

The collision-induced absorption of H2-CH4 mixtures was measured from 20 to 900/cm at 195 and 297 K. By subtracting the absorption due to H2-H2 and CH4-CH4 collisions from that of the mixture, the absorption due to H2-CH4 collisions was obtained. This spectrum was analyzed using the BC model line shape to provide a way of estimating the far-IR spectrum of H2-CH4 for various concentrations of H2 and CH4. Theoretical spectral moments were computed with different potential functions and compared with experimental values.

Birnbaum, George↗
NASA NTRS1990

The 3.3 micron feature, H2, and ionized gas in the Orion bar

The results of spectroscopy of the 3.3 micron feature, H2 emission, P-alpha, and Br-alpha, obtained along a line perpendicular to the Orion ionization front, are presented. The intensity of the 3.3 micron feature reaches a maximum between the ionization front and the H2 peak. The 3.33 micron spatial distribution appears to be due to destruction of the emitting material within the H II region and extinction of the exciting radiation between the edge of the H II region and the H2 peak, resulting in a maximum between the ionization front and the H2 peak. The H2 peak is consistent with either being due to a shock front or being due to UV-pumped fluorescence from dense clumps of H2. The width of the 3.3 micron feature observed at high spectral resolution is constant in regions of varying UV flux. It is suggested that the strength of the UV field is not the cause of the variations in the 3.3 micron feature width observed in other sources, but rather that these variations are caused by a compositional change related to the age of the emitting material.

Sellgren, K.↗
NASA NTRS1993

H2 in interstellar and extragalactic ices - Infrared characteristics, ultraviolet production, and implications

H2 is the most abundant molecule in the universe. We demonstrate that this molecule may be an important component of interstellar and possibly intergalactic ices, both because it can be formed in situ, within the ices, and because gas-phase H2 can freeze out onto dust grains in some astrophysical environments. The condensation-sublimation and infrared spectral properties of ices containing H2 are presented. We show that solid H2 in H2O-rich ices can be detected by an infrared absorption band at 4137/cm (2.417 microns). The surface binding energy of H2 to H2O ice was measured to be Delta-H(s)/k = 555 +/- 35 K. Surface binding energies can be used to calculate the residence times of H2 on grain surfaces as a function of temperature. Some of the implications of these results are considered.

Sandford, Scott A.↗
NASA NTRS1994

H2-rich interstellar grain mantles: An equilibrium description

Experiments simulating the codeposition of molecular hydrogen and water ice on interstellar grains demonstrate that amorphous water ice at 12 K can incorporate a substantial amount of H2, up to a mole ratio of H2/H2O = 0.53. We find that the physical behavior of approximately 80% of the hydrogen can be explained satisfactorily in terms of an equilibrium population, thermodynamically governed by a wide distribution of binding site energies. Such a description predicts that gas phase accretion could lead to mole fractions of H2 in interstellar grain mantles of nearly 0.3; for the probable conditions of WL5 in the rho Ophiuchi cloud, an H2 mole fraction of between 0.05 and 0.3 is predicted, in possible agreement with the observed abundance reported by Sandford, Allamandola, & Geballe. Accretion of gas phase H2 onto grain mantles, rather than photochemical production of H2 within the ice, could be a general explanation for frozen H2 in interstellar ices. We speculate on the implications of such a composition for grain mantle chemistry and physics.

Dissly, Richard W.↗
NASA NTRS1997

Infrared Response of H2 to X-Rays in Dense Clouds

The excitation by X-rays and cosmic rays of molecular hydrogen in interstellar clouds is analyzed. We carried out detailed calculations of entry efficiencies in rovibrational levels of H2 following impact with fast electrons produced by X-ray ionization of the gas. The competing effect of collisional excitation, and quenching by the ambient gas is examined in detail. Up to date values for H-H2 collisional rate coefficients are adopted, and some derivations of H2-H2 rovibrational rate coefficients from existing literature data are proposed. Several models as a function of temperature, density, and ionization rate are presented. We found that H2 infrared emission in X-ray dominated regions (XDR) is potentially observable for temperatures and ionization rates lower than certain critical values (typically T < 1000 K and zeta/n(sub H) < 10(exp -15) cc/s where zeta is the ionization rate). At higher temperatures, collisional excitation by the ambient gas dominates the population of low vibrational levels, and at higher values of zeta/n(sub H) the abundance of H2 is negligible. If such conditions are satisfied, the resulting infrared emission spectrum can be used as a diagnostic of nearby X-ray sources such as in cooling flows in galaxy clusters, quasars, Seyfert galaxies and supernova remnants. The intensity ratio of the 2-1S(1) and 1-0S(1) lines measured for the Seyfert galaxy NGC 1275 is consistent with X-ray pumping.

Tine, S.↗
NASA NTRS2003

Measurement and Simulation of Spontaneous Raman Scattering Spectra in High-Pressure, Fuel-Rich H2-Air Flames

Rotational vibrational spontaneous Raman spectra (SRS) of H2, N2, and H2O have been measured in H2-air flames at pressures up to 30 atm as a first stem towards establishing a comprehensive Raman spectral database for temperatures and species in high-pressure combustion. A newly developed high-pressure burner facility provides steady, reproducible flames with a high degree of flow precision. We have obtained an initial set of measurements that indicate the spectra are of sufficient quality in terms of spectral resolution, wavelength coverage, and signal-to-noise ratio for use in future reference standards. The fully resolved Stokes and anti-Stokes shifted SRS spectra were collected in the visible wavelength range (400-700 nm) using pulse-stretched 532 nm excitation and a non-intensified CCD spectrograph with a high-speed shutter. Reasonable temperatures were determined via the intensity distribution of rotational H2 lines at stoichiometry and fuel-rich conditions. Theoretical Raman spectra of H2 were computed using a semi-classical harmonic-oscillator model with recent pressure broadening data and were compared with experimental results. The data and simulation indicated that high-J rotational lines of H2 might interfere with the N2 vibrational Q-branch lines, and this could lead to errors in N2-Raman thermometry based on the line-fitting method. From a comparison of N2 Q-branch spectra in lean H2 low-pressure (1.2 atm) and high-pressure (30 atm) flames, we found no significant line-narrowing or -broadening effects at the current spectrometer resolution of 0.04 nm.

Kojima, Jun↗
NASA NTRS1974

Formation of HO2/+/ by reaction of metastable O2/+/ ions with H2

The photoionization efficiency curves of H2(+), O2(+), and HO2(+) have been studied in a mixture of hydrogen and oxygen over the wavelength range from 650 to 810 A. The HO2(+) ion appears at 804 A, the threshold for ionization of H2, by the reaction H2(+) + O2 yields HO2(+) + H. The relative photoionization efficiency curves of H2(+) and HO2(+) are the same from 804 to 764 A. Below 764 A production of the 4 Pi u metastable electronic state of O2(+) leads to the formation of HO2(+) by the reaction O2(+)(a 4 Pi u) + H2 yields HO2(+) + H.

Ajello, J. M.↗
NASA NTRS1976

H2 recombination on interstellar grains

From a consideration of relevant theoretical and experimental data it is concluded that H atoms (but not H2 molecules) will be chemisorbed on interstellar graphite grains, with H2 formation proceeding efficiently for graphite grain temperatures less than 70 K. It is argued that graphite grains will act as the principal sites for H2 formation, with a formation rate of about 4 to the minus 17th cu cm per sec. Heating by H2 molecules formed by surface recombination is analyzed in the context of the available experimental data, and a heating rate is derived and compared with other suggested cloud heating mechanisms. It is concluded that H2 recombination will provide the largest heat source in diffuse clouds if the albedo of interstellar dust in the 912-1200 A region is high (about 0.9), whereas if the albedo in this wavelength region is lower (about 0.5), photoelectron ejection from grains will tend to predominate, and can explain observed cloud temperatures with a carbon depletion factor of approximately 2, a factor attributable to a normal interstellar abundance of graphite grains.

Barlow, M. J.↗