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NASA NTRS1997

The 2140 cm-1 (4.673 microns) solid CO band: the case for interstellar O2 and N2 and the photochemistry of nonpolar interstellar ice analogs

The infrared spectra of CO frozen in nonpolar ices containing N2, CO2, O2, and H2O and the UV photochemistry of these interstellar/precometary ice analogs are reported. The spectra are used to test the hypothesis that the narrow 2140 cm-1 (4.673 microns) interstellar absorption feature attributed to solid CO might be produced by CO frozen in ices containing nonpolar species such as N2 and O2. It is shown that mixed molecular ices containing CO, N2, O2, and CO2 provide a good match to the interstellar band at all temperatures between 12 and 30 K both before and after photolysis. The optical constants (real and imaginary parts of the index of refraction) in the region of the solid CO feature are reported for several of these ices. The N2 and O2 absorptions at 2328 cm-1 (4.296 microns) and 1549 cm-1 (6.456 microns), respectively, are also shown. The best matches between the narrow interstellar band and the feature in the laboratory spectra of nonpolar ices are for samples which contain comparable amounts of N2, O2, CO2, and CO. Co-adding the CO band from an N2:O2:CO2:CO = 1:5:1/2:1 ice with that of an H2O:CO = 20:1 ice provides an excellent fit across the entire interstellar CO feature. The four-component, nonpolar ice accounts for the narrow 2140 cm-1 portion of the feature which is associated with quiescent regions of dense molecular clouds. Using this mixture, and applying the most recent cosmic abundance values, we derive that between 15% and 70% of the available interstellar N is in the form of frozen N2 along several lines of sight toward background stars. This is reduced to a range of 1%-30% for embedded objects with lines of sight more dominated by warmer grains. The cosmic abundance of O tied up in frozen O2 lies in the 10%-45% range toward background sources, and it is between 1% and 20% toward embedded objects. The amount of oxygen tied up in CO and CO2 frozen in nonpolar ices can be as much as 2%-10% toward background sources and on the order of 0.2%-5% for embedded objects. Similarly 3%-13% of the carbon is tied up in CO and CO2 frozen in nonpolar ices toward field stars, and 0.2%-6% toward embedded objects. These numbers imply that most of the N is in N2, and a significant fraction of the available O is in O2 in the most quiescent regions of dense clouds. Ultraviolet photolysis of these ices produces a variety of photoproducts including CO2, N2O, O3, CO3, HCO, H2CO, and possibly NO and NO2. XCN is not produced in these experiments, placing important constraints on the origin of the enigmatic interstellar XCN feature. N2O and CO3 have not been previously considered as interstellar ice components.

NASA Discipline Exobiology↗

NASA NTRS1988

The 2.5-12 micrometers spectrum of comet Halley from the IKS-VEGA experiment

The infrared instrument IKS flown on board the VEGA space probes was designed for the detection of emission bands of parent molecules, and for a measurement of the size and temperature of the thermal emitting nuclear region. The instrument had three channels with cooled detectors: an "imaging channel" designed to modulate the signal of the nucleus and two spectroscopic channels operating at 2.5-5 and 6-12 micrometers, respectively, equipped with circular variable filters of resolving power approximately 50. This paper presents and discusses the results from the spectral channels. On VEGA 1, usable spectra were obtained at distances D from the comet nucleus ranging from 250,000 to 40,000 km corresponding to fields of view 4000 and 700 km in diameter, respectively. The important internal background signal caused by the instrument itself, which could not be cooled, had to be eliminated. Since no sky chopping was performed, we obtain difference spectra between the current spectrum and a reference spectrum with little or no cometary signal taken at the beginning of the observing sequence (D approximately 200,000 km). Final discrimination between cometary signal and instrumental background is achieved using their different time evolution, since the instrumental background is proportional to the slow temperature drift of the instrument, and the cometary signal due to parent molecules or dust grains is expected to vary in first order as D-1. The 2.5-5 micrometers IKS spectra definitely show strong narrow signals at 2.7 and 4.25 micrometers, attributed to the nu 3 vibrational bands of H2O and CO2, respectively, and a broader signal in the region 3.2-3.5 micrometers, which may be attributed to CH-bearing molecules. All these signals present the expected D-1 intensity variation. Weaker emission features at 3.6 and 4.7 micrometers could correspond to the nu 1 and nu 5 bands of H2CO and the (1 - 0) band of CO, respectively. Molecular production rates are derived from the observed emissions, assuming that they are due to resonance fluorescence excited by the Sun's infrared radiation. For the strong bands of H2O and CO2, the rovibrational lines are optically thick, and radiative transfer is taken into account. We derive production rates, at the moment of the VEGA 1 flyby, of approximately 10(30) sec-1 for H2O, approximately 2.7 x 10(28) sec-1 for CO2, approximately 5 x 10(28) sec-1 for CO, and 4 x 10(28) sec-1 for H2CO, if attributions to CO and H2CO are correct. The production rate of carbon atoms in CH-bearing molecules is approximately 9 x 10(29) sec-1 assuming fluorescence of molecules in the gas phase, but could be much less if the 3.2-3.5 micrometers emission is attributed to C-H stretch in polycyclic aromatic hydrocarbons or small organic grains. In addition, marginal features are present at 4.85 and 4.45 micrometers, tentatively attributed to OCS and molecules with the CN group, respectively. Broad absorption at 2.8-3.0 micrometers, as well as a narrow emission at 3.15 micrometers, which follow well the D-1 intensity variation, might be due to water ice. Emission at 2.8 micrometers is also possibly present, and might be due to OH created in vibrationally excited states after water photodissociation. The 6-12 micrometers spectrum does not show any molecular emission, nor emission in the 7.5-micrometers region. The spectrum is dominated by silicate emission showing a double structure with maxima at 9.0 and 11.2 micrometers, which suggests the presence of olivine.

NASA Discipline Number 52-10↗

NASA NTRS1990

Radiolysis of aqueous solutions of acetic acid in the presence of Na-montmorillonite

The gamma-irradiation of 0.8 mol dm-3 aqueous, oxygen-free acetic acid solutions was investigated in the presence or absence of Na-montmorillonite. H2, CH4, CO, CO2, and several polycarboxylic acids were formed in all systems. The primary characteristics observed in the latter system were: (1) Higher yield of the decomposition of acetic acid; (2) Lower yield of the formation of polycarboxylic acids; (3) No effect on the formation of methane; (4) Higher yield of the formation of carbon dioxide; and (5) The reduction of Fe3+ in the octahedral sites of Na-montmorillonite. A possible reaction scheme was proposed to account for the observed changes. The results are important in understanding heterogeneous processes in radiation catalysis and might be significant to prebiotic chemistry.

Non-NASA Center↗

NASA NTRS1996

Evolutionary status of the pre-protostellar core L1498

L1498 is a classic example of a dense cold pre-protostellar core. To study the evolutionary status, the structure, dynamics, and chemical properties of this core we have obtained high spatial and high spectral resolution observations of molecules tracing densities of 10(3)-10(5) cm-3. We observed CCS, NH3, C3H2, and HC7N with NASA's DSN 70 m antennas. We also present large-scale maps of C18O and 13CO observed with the AT&T 7 m antenna. For the high spatial resolution maps of selected regions within the core we used the VLA for CCS at 22 GHz, and the Owens Valley Radio Observatory (OVRO) MMA for CCS at 94 GHz and CS (2-1). The 22 GHz CCS emission marks a high-density [n(H2) > 10(4) cm -3] core, which is elongated with a major axis along the SE-NW direction. NH3 and C3H2 emissions are located inside the boundary of the CCS emission. C18O emission traces a lower density gas extending beyond the CCS boundary. Along the major axis of the dense core, CCS, NH3 and C3H2 emission show evidence of limb brightening. The observations are consistent with a chemically differentiated onion-shell structure for the L1498 core, with NH3 in the inner and CCS in the outer parts of the core. The high angular resolution (9"-12") spectral line maps obtained by combining NASA Goldstone 70 m and VLA data resolve the CCS 22 GHz emission in the southeast and northwest boundaries into arclike enhancements, supporting the picture that CCS emission originates in a shell outside the NH3 emitting region. Interferometric maps of CCS at 94 GHz and CS at 98 GHz show that their emitting regions contain several small-scale dense condensations. We suggest that the differences between the CCS, CS, C3H2, and NH3 emission are caused by a time-dependent effect as the core evolves slowly. We interpret the chemical and physical properties of L1498 in terms of a quasi-static (or slowly contracting) dense core in which the outer envelope is still growing. The growth rate of the core is determined by the density increase in the CCS shell resulting from the accretion of the outer low-density gas traced by C18O. We conclude that L1498 could become unstable to rapid collapse to form a protostar in less than 5 x 10(6) yr.

NASA Discipline Exobiology↗

NASA NTRS1993

Mantle redox evolution and the oxidation state of the Archean atmosphere

Current models predict that the early atmosphere consisted mostly of CO2, N2, and H2O, along with traces of H2 and CO. Such models are based on the assumption that the redox state of the upper mantle has not changed, so that volcanic gas composition has remained approximately constant with time. We argue here that this assumption is probably incorrect: the upper mantle was originally more reduced than today, although not as reduced as the metal arrest level, and has become progressively more oxidized as a consequence of the release of reduced volcanic gases and the subduction of hydrated, oxidized seafloor. Data on the redox state of sulfide and chromite inclusions in diamonds imply that the process of mantle oxidation was slow, so that reduced conditions could have prevailed for as much as half of the earth's history. To be sure, other oxybarometers of ancient rocks give different results, so the question of when the mantle redox state has changed remains unresolved. Mantle redox evolution is intimately linked to the oxidation state of the primitive atmosphere: A reduced Archean atmosphere would have had a high hydrogen escape rate and should correspond to a changing mantle redox state; an oxidized Archean atmosphere should be associated with a constant mantle redox state. The converses of these statements are also true. Finally, our theory of mantle redox evolution may explain why the Archean atmosphere remained oxygen-deficient until approximately 2.0 billion years ago (Ga) despite a probable early origin for photosynthesis.

NASA Discipline Number 52-30↗

NASA NTRS2002

Development of a cw-laser-based cavity-ringdown sensor aboard a spacecraft for trace air constituents

The progress in the development of a sensor for the detection of trace air constituents to monitor spacecraft air quality is reported. A continuous-wave (cw), external-cavity tunable diode laser centered at 1.55 micrometers is used to pump an optical cavity absorption cell in cw-cavity ringdown spectroscopy (cw-CRDS). Preliminary results are presented that demonstrate the sensitivity, selectivity and reproducibility of this method. Detection limits of 2.0 ppm for CO, 2.5 ppm for CO2, 1.8 ppm for H2O, 19.4 ppb for NH3, 7.9 ppb for HCN and 4.0 ppb for C2H2 are calculated.

NASA Discipline Life Sciences Technologies↗

NASA NTRS2000

Novel diode laser-based sensors for gas sensing applications

The development of compact spectroscopic gas sensors and their applications to environmental sensing will be described. These sensors employ mid-infrared difference-frequency generation (DFG) in periodically poled lithium niobate (PPLN) crystals pumped by two single-frequency solid state lasers such as diode lasers, diode-pumped solid state, and fiber lasers. Ultrasensitive, highly selective, and real-time measurements of several important atmospheric trace gases, including carbon monoxide, nitrous oxide, carbon dioxide, formaldehyde [correction of formaldehye], and methane, have been demonstrated.

NASA Discipline Life Sciences Technologies↗

NASA NTRS1999

Envelope structure of deeply embedded young stellar objects in the Serpens Molecular Cloud

Aperture-synthesis and single-dish (sub-) millimeter molecular-line and continuum observations reveal in great detail the envelope structure of deeply embedded young stellar objects (SMM 1 = FIRS 1, SMM 2, SMM 3, SMM 4) in the densely star-forming Serpens Molecular Cloud. SMM 1, 3, and 4 show partially resolved (>2" = 800 AU) continuum emission in the beam of the Owens Valley Millimeter Array at lambda = 3.4-1.4 mm. The continuum visibilities accurately constrain the density structure in the envelopes, which can be described by a radial power law with slope -2.0 +/- 0.5 on scales of 300 to 8000 AU. Inferred envelope masses within a radius of 8000 AU are 8.7, 3.0, and 5.3 Msolar for SMM 1, 3, and 4, respectively. A point source with 20%-30% of the total flux at 1.1 mm is required to fit the observations on long baselines, corresponding to warm envelope material within approximately 100 AU or a circumstellar disk. No continuum emission is detected interferometrically toward SMM 2, corresponding to an upper limit of 0.2 Msolar assuming Td = 24 K. The lack of any compact dust emission suggests that the SMM 2 core does not contain a central protostar. Aperture-synthesis observations of the 13CO, C18O, HCO+, H13CO+, HCN, H13CN, N2H+ 1-0, SiO 2-1, and SO 2(2)-1(1) transitions reveal compact emission toward SMM 1, 3, and 4. SMM 2 shows only a number of clumps scattered throughout the primary field of view, supporting the conclusion that this core does not contain a central star. The compact molecular emission around SMM 1, 3, and 4 traces 5"-10" (2000-4000 AU) diameter cores that correspond to the densest regions of the envelopes, as well as material directly associated with the molecular outflow. Especially prominent are the optically thick HCN and HCO+ lines that show up brightly along the walls of the outflow cavities. SO and SiO trace shocked material, where their abundances may be enhanced by 1-2 orders of magnitude over dark-cloud values. A total of 31 molecular transitions have been observed with the James Clerk Maxwell and Caltech Submillimeter telescopes in the 230, 345, 490, and 690 GHz atmospheric windows toward all four sources, containing, among others, lines of CO, HCO+, HCN, H2CO, SiO, SO, and their isotopomers. These lines show 20-30 km s-1 wide line wings, deep and narrow (1-2 km s-1) self-absorption, and 2-3 km s-1 FWHM line cores. The presence of highly excited lines like 12CO 4-3 and 6-5, 13CO 6-5, and several H2CO transitions indicates the presence of material with temperatures > or approximately 100 K. Monte Carlo calculations of the molecular excitation and line transfer show that the envelope model derived from the dust emission can successfully reproduce the observed line intensities. The depletion of CO in the cold gas is modest compared to values inferred in objects like NGC 1333 IRAS 4, suggesting that the phase of large depletions through the entire envelope is short lived and may be influenced by the local star formation density. Emission in high-excitation lines of CO and H2CO requires the presence of a small amount of approximately 100 K material, comprising less than 1% of the total envelope mass and probably associated with the outflow or the innermost region of the envelope. The derived molecular abundances in the warm (Tkin > 20 K) envelope are similar to those found toward other class 0 YSOs like IRAS 16293-2422, though some species appear enhanced toward SMM 1. Taken together, the presented observations and analysis provide the first comprehensive view of the physical and chemical structure of the envelopes of deeply embedded young stellar objects in a clustered environment on scales between 1000 and 10,000 AU.

NASA Discipline Exobiology↗

NASA NTRS1997

Chemical and physical gradients along the OMC-1 ridge

We present a survey of the distribution of 20 chemical and isotopic molecular species along the central ridge of the Orion molecular cloud from 6' north to 6' south of BN-KL observed with the QUARRY focal plane array on the FCRAO 14 m telescope, which provides an angular resolution of approximately 50" in the 3 mm wavelength region. We use standard tools of multivariate analysis for a systematic investigation of the similarities and differences among the maps of integrated intensities of the 32 lines observed. The maps fall in three broad classes: first, those strongly peaked toward BN-KL; second, those having rather flat distributions along the ridge; and third, those with a clear north-south gradient or contrast. We identify six positions or regions where we calculate relative abundances. Line velocities and line widths indicate that the optically thin lines generally trace the same volume of dense gas, except in the molecular bar, where C18O, C34S, H13CO+, CN, C2H, SO, and C3H2 have velocities characteristic of the bar itself, whereas the emission from other detected species is dominated by the background cloud. The strongest abundance variations in our data are the well-known enhancements seen in HCN, CH3OH, HC3N, and SO toward BN-KL and, less strongly, toward the Orion-South outflow 1'.3S. The principal result of this study is that along the extended quiescent ridge the chemical abundances, within factors of 3-4, exhibit an impressive degree of uniformity. The northern part of the ridge has a chemistry closest to that found in quiescent dense clouds. While temperature and density are similar around the northern radical-ion peak near 3'.5N and in the southern core near 4'.2S, some abundances, in particular, those of the ions HCO+ and N2H+, are significantly lower toward 4'.2S. The areas near 4.'2S and the molecular bar itself around (1'.7E, 2'.4S) stand out with peculiar and similar properties probably caused by stronger UV fields penetrating deeper into the clumpy molecular gas. This leads to higher electron abundances and thereby reduced abundances of the ions, as well as a lack of complex molecules.

NASA Discipline Exobiology↗

NASA NTRS1988

Trapping of gas mixtures by amorphous water ice

Our studies on gas trapping in amorphous water ice at 24-100 K were extended, by using mixtures of CH4, CO, N2, and Ar, rather than single gases. In 1:1 gas:(water vapor) mixtures, the competition among these gases on the available sites in the ice showed that the trapping capacity for the various gases is determined not only by the structure and dynamics of the ice, but is also influenced by the gas itself. Whereas at 24-35 K all four gases are trapped in the ice indiscriminantly, at 50-75 K there is a clear enhancement, in the order of CH4 > CO > N2 > or approximately Ar. This order is influenced by the gas-water interaction energy, the size of the trapped gas atom or molecule, the type of clathrate-hydrate formed (I or II) and, possibly, other factors. It seems that the gas can be trapped in the amorphous ice in several different locations, each being affected in a different way by the deposition temperature and gas composition. Once a gas atom or molecule is trapped in a specific location, it is predestined to emerge in one of eight different temperature ranges, which are associated with changes in the ice. The experimentally observed enhancements, together with the findings on the gas composition of comet Halley, might enable an estimation of the gas composition in the region of comet formation.

NASA Discipline Number 52-10↗

NASA NTRS1996

Detection of abundant ethane and methane, along with carbon monoxide and water, in comet C/1996 B2 Hyakutake: evidence for interstellar origin

The saturated hydrocarbons ethane (C2H6) and methane (CH4) along with carbon monoxide (CO) and water (H2O) were detected in comet C/1996 B2 Hyakutake with the use of high-resolution infrared spectroscopy at the NASA Infrared Telescope Facility on Mauna Kea, Hawaii. The inferred production rates of molecular gases from the icy, cometary nucleus (in molecules per second) are 6.4 X 10(26) for C2H6, 1.2 X 10(27) for CH4, 9.8 X 10(27) for CO, and 1.7 X 10(29) for H2O. An abundance of C2H6 comparable to that of CH4 implies that ices in C/1996 B2 Hyakutake did not originate in a thermochemically equilibrated region of the solar nebula. The abundances are consistent with a kinetically controlled production process, but production of C2H6 by gas-phase ion molecule reactions in the natal cloud core is energetically forbidden. The high C2H6/CH4 ratio is consistent with production of C2H6 in icy grain mantles in the natal cloud, either by photolysis of CH4-rich ice or by hydrogen-addition reactions to acetylene condensed from the gas phase.

Non-programmatic↗

NASA NTRS1995

Collision of comet Shoemaker-Levy 9 with Jupiter observed by the NASA infrared telescope facility

The National Aeronautics and Space Administration (NASA) Infrared Telescope Facility was used to investigate the collision of comet Shoemaker-Levy 9 with Jupiter from 12 July to 7 August 1994. Strong thermal infrared emission lasting several minutes was observed after the impacts of fragments C, G, and R. All impacts warmed the stratosphere and some the troposphere up to several degrees. The abundance of stratospheric ammonia increased by more than 50 times. Impact-related particles extended up to a level where the atmospheric pressure measured several millibars. The north polar near-infrared aurora brightened by nearly a factor of 5 a week after the impacts.

NASA Discipline Exobiology↗