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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
NASA NTRS1988

Silane and germane plasma diagnostics for depositing photosensitive a-SiGe:H films

Highly photosensitive a-SiGe:H films with a light-to-dark conductivity ratio of 8 x 103 and an optical bandgap of 1.40 eV have been produced by RF glow discharge using hydrogen dilution of SiH4 and GeH4 mixed gas plasma. The critical role of hydrogen dilution in GeH4 containing plasmas is to suppress the gas-phase polymerization and promote the incorporation of Ge into the film. It is observed that inelastic laser light scattering of the RF plasma is a sensitive method for monitoring the onset of the gas-phase polymerization. In situ coherent anti-Stokes Raman spectroscopy measurements have shown that the dissociation rate of GeH4 is a factor of three larger than that of SiH4.

Shing, Y. H.↗
DOE OSTI2021

Gas transport characteristics of supramolecular networks of metal-coordinated highly branched Poly(ethylene oxide)

Model systems are developed and investigated to better understand the effect of polyether-metal ion interactions on gas separation characteristics. These systems help answer current questions raised by the substantial body of research on metal-organic frameworks (MOFs) dispersed in polyethers to improve gas separation performance, where favorable interactions between the metal centers and polyethers are preferred to improve interfacial compatibility. Specifically, we investigate CO 2 /gas transport properties of supramolecular networks comprising cross-linked poly(ethylene oxide) (XLPEO) and dissociable salts, including LiClO 4 , Ni(BF 4 ) 2 , and Cu(BF 4 ) 2 . Increasing the salt content increases the glass transition temperature (T g ) and generally decreases gas diffusivity and permeability, which can be successfully described using a T g -integrated free volume model with an expression similar to the Vogel-Tammann-Fulcher (VTF) equation. Surprisingly, low loadings of LiClO 4 and Cu(BF 4 ) 2 (2 mass% or less) can increase gas permeability by 30%–70% without affecting the CO 2 /gas selectivity. This increase correlates with polyether-metal ion dynamics as measured by dielectric spectroscopy. Understanding how interaction-mediated dynamics affect gas transport will be instrumental to designing MOF-based mixed matrix materials for gas separations.

36 MATERIALS SCIENCE↗
NASA NTRS1982

Production and condensation of organic gases in the atmosphere of Titan

The rates and altitudes for the dissociation of atmospheric constituents on Titan are calculated for solar ultraviolet radiation, the solar wind, Saturn magnetospheric particles, the Saturn co-rotating plasma, and cosmic rays. Laboratory experiments show that a variety of simple gas phase organic molecules and more complex organic solids called tholins are produced by such irradiations of simulated Titanian atmospheres. Except for ultraviolet wavelengths longward of the methane photodissociation continuum, most dissociation events occur between about 3100 and 3600 km altitude, corresponding well to the region of EUV opacity detected by Voyager. For a wide variety of simple to moderately complex organic gases in the Titanian atmosphere, condensation occurs below the top of the main cloud deck at about 2825 km. It is proposed that such condensates, beginning with CH4 at about 2615 km, comprise the principal mass of the Titan clouds. There is a distinct tendency for the atmosphere of Titan to act as a fractional distillation device, molecules of greater complexity condensing out at higher altitudes.

Sagan, C.↗
NASA NTRS1984

Production and condensation of organic gases in the atmosphere of Titan

The rates and altitudes for the dissociation of atmospheric constituents on Titan are calculated for solar ultraviolet radiation, the solar wind, Saturn magnetospheric particles, the Saturn co-rotating plasma, and cosmic rays. Laboratory experiments show that a variety of simple gas phase organic molecules and more complex organic solids called tholins are produced by such irradiations of simulated Titanian atmospheres. Except for ultraviolet wavelengths longward of the methane photodissociation continuum, most dissociation events occur between about 3100 and 3600 km altitude, corresponding well to the region of EUV opacity detected by Voyager. For a wide variety of simple to moderately complex organic gases in the Titanian atmosphere, condensation occurs below the top of the main cloud deck at about 2825 km. It is proposed that such condensates, begining with CH4 at about 2615 km comprise the principal mass of the Titan clouds. There is a distinct tendency for the atmosphere of Titan to act as a fractional distillation device, molecules of greater complexity condensing out at higher altitudes.

Sagan, C.↗
NASA NTRS1984

Photodeposition of Nitride Insulators on 3-5 Substrates

Laser assisted chemical vapor deposition (LCVD) of nitride insulators, using an excimer laser operating on either KrF or ArF transitions (248 nm or 193 nm respectively) was explored. The properties of silicon nitride films Deposited with 193 nm photons on quartz and silicon substrates in a SiH4, NH3, N2 and He mixture are discussed. Aluminum films were deposited at substrate temperatures from room temperature to 200 C using 248 nm or 193 nm photons to dissociate trimethylaluminum (TMA). Deposition of Al films were investigated to isolate problems associated with TMA such as C and O contamination during AlN depositions. The Al film properties were evaluated on SiO2 and Si substrates. Preliminary results were obtained for aluminum nitride films using TMA and NH3 as the gas phase Al and N donors. The properties of Cr films deposited over areas 5 square cm using 193 nm or 248 nm photons to dissociate Cr(CO) were investigated.

Collins, G. J.↗
NASA NTRS1995

Heating And Cooling of the Interstellar Medium

This talk will review the various heating and cooling processes in the interstellar medium. The most important heating processes include the photoelectric effect on dust grains and PAH molecules. Cooling of the gas in the interstellar medium is dominated by emission in the far infrared fine structure lines of OI, CII, SiII, and CI, and the rotational transitions of CO. Many of these lines have been observed from air borne platform, in particular the Kuiper Airborne Observatory. Which of these heating and cooling processes dominates in a given region depends on its physical and especially chemical conditions, which in turn depend themselves on the interstellar UV radiation field. As a result of the interplay of these processes, the interstellar medium is organized in various structures with distinctly different physical conditions (ie., temperature, density, and degree of ionization). Over the last decade, the dominant cooling lines of the neutral interstellar medium have been studied using the Kuiper Airborne Observatory. Because of sensitivity, these observations have concentrated on dense regions illuminated by strong UV fields from nearby stars, so-called Photo Dissociation Regions (PDRs). These observations allow us to study in detail the interaction of UV photons and the interstellar gas and dust. Detailed theoretical models have been developed for PDRs. These will be reviewed and compared to the observations. Finally, anticipated crucial results of future space-based missions (SIRTF, ISO) will be pointed out.

Tielens, Alexander G. G.↗
DOE OSTI2020

Bypassing the Energy Functional in Density Functional Theory: Direct Calculation of Electronic Energies from Conditional Probability Densities

Density functional calculations can fail for want of an accurate exchange-correlation approximation. The energy can instead be extracted from a sequence of density functional calculations of conditional probabilities (CP DFT). Simple CP approximations yield usefully accurate results for two-electron ions, the hydrogen dimer, and the uniform gas at all temperatures. CP DFT has no self-interaction error for one electron, and correctly dissociates H2, both major challenges. For warm dense matter, classical CP DFT calculations can overcome the convergence problems of Kohn-Sham DFT.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2000

An abiotic origin for hydrocarbons in the Allan Hills 84001 martian meteorite through cooling of magmatic and impact-generated gases

Thermodynamic calculations of metastable equilibria were used to evaluate the potential for abiotic synthesis of aliphatic and polycyclic aromatic hydrocarbons (PAHs) in the martian meteorite Allan Hills (ALH) 84001. The calculations show that PAHs and normal alkanes could form metastably from CO, CO2, and H2 below approximately 250-300 degrees C during rapid cooling of trapped magmatic or impact-generated gases. Depending on temperature, bulk composition, and oxidation-reduction conditions, PAHs and normal alkanes can form simultaneously or separately. Moreover, PAHs can form at lower H/C ratios, higher CO/CO2 ratios, and higher temperatures than normal alkanes. Dry conditions with H/C ratios less than approximately 0.01-0.001 together with high CO/CO2 ratios also favor the formation of unalkylated PAHs. The observed abundance of PAHs, their low alkylation, and a variable but high aromatic to aliphatic ratio in ALH 84001 all correspond to low H/C and high CO/CO2 ratios in magmatic and impact gases and can be used to deduce spatial variations of these ratios. Some hydrocarbons could have been formed from trapped magmatic gases, especially if the cooling was fast enough to prevent reequilibration. We propose that subsequent impact heating(s) in ALH 84001 could have led to dissociation of ferrous carbonates to yield fine-grain magnetite, formation of a CO-rich local gas phase, reduction of water vapor to H2, reequilibration of the trapped magmatic gases, aromatization of hydrocarbons formed previously, and overprinting of the synthesis from magmatic gases, if any. Rapid cooling and high-temperature quenching of CO-, H2-rich impact gases could have led to magnetite-catalyzed hydrocarbon synthesis.

Non-NASA Center↗
NASA NTRS2020

High Angular Resolution ALMA Images of Dust and Molecules in the SN 1987A Ejecta

We present high angular resolution (∼80 mas) ALMA continuum images of the SN1987A system, together with CO J = 21, J = 65, and SiO J = 54 to J = 76 images, which clearly resolve the ejecta (dust continuum and molecules) and ring (synchrotron continuum) components. Dust in the ejecta is asymmetric and clumpy, and overall the dust fills the spatial void seen in Hα images, filling that region with material from heavier elements. The dust clumps generally fill the space where CO J = 6 5 is fainter, tentatively indicating that these dust clumps and CO are locationally and chemically linked. In these regions, carbonaceous dust grains might have formed after dissociation of CO. The dust grains would have cooled by radiation, and subsequent collisions of grains with gas would also cool the gas, suppressing the CO J = 6 5 intensity. The data show a dust peak spatially coincident with the molecular hole seen in previous ALMA CO J = 2 1 and SiO J = 5 4 images. That dust peak, combined with CO and SiO line spectra, suggests that the dust and gas could be at higher temperatures than the surrounding material, though higher density cannot be totally excluded. One of the possibilities is that a compact source provides additional heat at that location. Fits to the far-infrared–millimeter spectral energy distribution give ejecta dust temperatures of 18–23 K. We revise the ejecta dust mass to Mdust = 0.2–0.4 Mfor carbon or silicate grains, or a maximum of <0.7 Mfor a mixture of grain species, using the predicted nucleosynthesis yields as an upper limit.

Interstellar dust↗
NASA NTRS1986

Non-solar noble gas abundances in the atmosphere of Jupiter

The thermodynamic stability of clathrate hydrate is calculated to predict the formation conditions corresponding to a range of solar system parameters. The calculations were performed using the statistical mechanical theory developed by van der Waals and Platteeuw (1959) and existing experimental data concerning clathrate hydrate and its components. Dissociation pressures and partition functions (Langmuir constants) are predicted at low pressure for CO clathrate (hydrate) using the properties of chemicals similar to CO. It is argued that nonsolar but well constrained noble gas abundances may be measurable by the Galileo spacecraft in the Jovian atmosphere if the observed carbon enhancement is due to bombardment of the atmosphere by clathrate-bearing planetesimals sometime after planetary formation. The noble gas abundances of the Jovian satellite Titan are predicted, assuming that most of the methane in Titan is accreted as clathrate. It is suggested that under thermodynamically appropriate conditions, complete clathration of water ice could have occurred in high-pressure nebulas around giant planets, but probably not in the outer solar nebula. The stability of clathrate in other pressure ranges is also discussed.

Lunine, Jonathan I.↗
DOE OSTI2024

Photoinduced hydrogen dissociation in thymine predicted by coupled cluster theory

The fate of thymine upon excitation by ultraviolet radiation has been the subject of intense debate. Today, it is widely believed that its ultrafast excited state gas phase decay stems from a radiationless transition from the bright ππ* state to a dark nπ* state. However, conflicting theoretical predictions have made the experimental data difficult to interpret. Here we simulate the early gas phase ultrafast dynamics in thymine at the highest level of theory to date. This is made possible by performing wavepacket dynamics with a recently developed coupled cluster method. Our simulation confirms an ultrafast ππ* to nπ* transition (τ = 41 ± 14 fs). Furthermore, the predicted oxygen-edge X-ray absorption spectra agree quantitatively with experiment. We also predict an as-yet uncharacterized πσ* channel that leads to hydrogen dissociation at one of the two N-H bonds. Similar behavior has been identified in other heteroaromatic compounds, including adenine, and several authors have speculated that a similar pathway may exist in thymine. However, this was never confirmed theoretically or experimentally. This prediction calls for renewed efforts to experimentally identify or exclude the presence of this channel.

Kjønstad, Eirik F.↗
DOE OSTI2022

Ambient pressure X-ray photoelectron spectroscopy study of room-temperature oxygen adsorption on Cu(1 0 0) and Cu(1 1 1)

We investigated the room-temperature chemisorption of oxygen on Cu(1 0 0) and Cu(1 1 1) using ambient-pressure X-ray photoelectron spectroscopy (APXPS). A shoulder-to-shoulder comparison between the oxygen-gas titration on the two surfaces reveals that Cu(1 0 0) is the more active for oxygen dissociative chemisorption when the surfaces are clean. The (2 $\sqrt{2}$ × $\sqrt{2}$)R45o missing-row reconstruction appears in Cu(1 0 0)’s LEED image after about 10 4 Langmuir of oxygen exposure, whereas on Cu(1 1 1), no long-range ordering was observed throughout the whole experiment. An oxide layer consisting of cuprous and cupric oxide shows up on Cu(1 1 1) at an oxygen exposure that is significantly lower than for Cu(1 0 0). This observation suggests that the presence of (2 $\sqrt{2}$ × $\sqrt{2}$)R45o missing-row reconstruction layer slows down Cu(1 0 0) oxidation. Literature has widely reported that surface morphology influences the copper oxidation process. This study provides an XPS demonstration that copper surface oxide formation in O 2 at room temperature depends on the surface crystallographic orientation.

36 MATERIALS SCIENCE↗
DOE OSTI2020

How Rh surface breaks CO 2 molecules under ambient pressure

Utilization of carbon dioxide (CO 2 ) molecules leads to increased interest in the sustainable synthesis of methane (CH 4 ) or methanol (CH 3 OH). The representative reaction intermediate consisting of a carbonyl or formate group determines yields of the fuel source during catalytic reactions. However, their selective initial surface reaction processes have been assumed without a fundamental understanding at the molecular level. Here, we report direct observations of spontaneous CO 2 dissociation over the model rhodium (Rh) catalyst at 0.1 mbar CO 2 . The linear geometry of CO 2 gas molecules turns into a chemically active bent-structure at the interface, which allows non-uniform charge transfers between chemisorbed CO 2 and surface Rh atoms. By combining scanning tunneling microscopy, X-ray photoelectron spectroscopy at near-ambient pressure, and computational calculations, we reveal strong evidence for chemical bond cleavage of O-CO* with ordered intermediates structure formation of (2 × 2)-CO on an atomically flat Rh(111) surface at room temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic states in molecules. We show with accurate calculations performed on gas-phase methyl iodide that electronic coherences of spin-orbit-split states persist in atomic iodine after dissociation. Our simulation predicts a maximum magnitude of vibronic coherence in the molecular regime of 0.75% of the initially photoexcited state population. Upon dissociation, one-third of this coherence magnitude is transferred to a long-lived atomic coherence where vibrational decoherence can no longer occur. To trace these dynamics, we propose a tabletop experimental approach—heterodyned attosecond four-wave-mixing spectroscopy. This technique can temporally resolve small electronic coherence magnitudes and reconstruct the full complex coherence function via phase cycling. Hence, heterodyned attosecond four-wave-mixing spectroscopy leads the way to a complete understanding and optimal control of spin-orbit-coupled electronic states in photochemistry.

Chemical Physics↗
DOE OSTI2023

Femtosecond Electronic and Hydrogen Structural Dynamics in Ammonia Imaged with Ultrafast Electron Diffraction

Directly imaging structural dynamics involving hydrogen atoms by ultrafast diffraction methods is complicated by their low scattering cross-sections. Here we demonstrate that megaelectronvolt ultrafast electron diffraction is sufficiently sensitive to follow hydrogen dynamics in isolated molecules. In a study of the photodissociation of gas phase ammonia, we simultaneously observe signatures of the nuclear and corresponding electronic structure changes resulting from the dissociation dynamics in the time-dependent diffraction. Both assignments are confirmed by ab initio simulations of the photochemical dynamics and the resulting diffraction observable. While the temporal resolution of the experiment is insufficient to resolve the dissociation in time, our results here represent an important step towards the observation of proton dynamics in real space and time.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1982

The NGC 7538 region - The distribution and dynamics of molecules compared with those of HI and H/+/

CO maps and preliminary H2S and H2CO data for the molecular cloud associated with the HII region NGC 7538 are compared with the distributions of ionized and neutral hydrogen. South of the optical HII region is a ridge of high (C-13)O column density with cold, self-absorbed HI gas just beyond it. A dense clump within thy ridge is found adjacent to the HII region in the southeast. The percentage of the hydrogen in atomic form varies from approximately 0.1% in the dense region to approximately 0.8% in the outskirts. The lower-density region of expanding gas seen next to the HII region in the southwest is attributed to the passage of a molecular dissociation wave.

Dickel, H. R.↗
NASA NTRS1991

Excited ionic and neutral fragments produced by dissociation of the N2(+)-asterisk H band

Atomic fluorescence produced by dissociative photoionization of N2 was observed and identified in experiments where fluorescent radiation was produced by irradiating N2 gas with undispersed synchrotron radiation. The spectrum was detected with a multichannel plate electron multiplier. Evidence is presented that the H band of N2(+)-asterisk does predissociate into excited neutral and ionic atoms.

Samson, James A. R.↗
NASA NTRS2003

Dissociation and Recombination Effects on the Performance of Pulse Detonation Engines

This paper summarizes major theoretical results for pulse detonation engine performance taking into account real gas chemistry, as well as significant performance differences resulting from the presence of ram and compression heating. An unsteady CFD analysis, as well as a thermodynamic cycle analysis, was conducted in order to determine the actual and the ideal performance for an air-breathing pulse detonation engine (PDE) using either a hydrogen-air or ethylene-air mixture over a flight Mach number range from 0 to 4. The results clearly elucidate the competitive regime of PDE application relative to ramjets and gas turbines.

Povinelli, Louis A.↗