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At least 271 records · Page 15

Molecular Dynamics Simulation of Pore-Size Effects on Gas Adsorption Kinetics in Zeolites

Strong gas-mineral interactions or slow adsorption kinetics require a molecular-level understanding of both adsorption and diffusion for these interactions to be properly described in transport models. In this combined molecular simulation and experimental study, noble gas adsorption and mobility is investigated in two naturally abundant zeolites whose pores are similar in size (clinoptilolite) and greater than (mordenite) the gas diameters. Simulated adsorption isotherms obtained from grand canonical Monte Carlo simulations indicate that both zeolites can accommodate even the largest gas (Rn). However, gas mobility in clinoptilolite is significantly hindered at pore-limiting window sites, as seen from molecular dynamics simulations in both bulk and slab zeolite models. Further, experimental gas adsorption isotherms for clinoptilolite confirm the presence of a kinetic barrier to Xe uptake, resulting in the unusual property of reverse Kr/Xe selectivity. Finally, a kinetic model is used to fit the simulated gas loading profiles, allowing a comparison of trends in gas diffusivity in the zeolite pores.

74 ATOMIC AND MOLECULAR PHYSICS↗

Al-26-Mg-26 ages of iron meteorites

An exposure age for an iron meteorite can be calculated from measurements of a radioactive nuclide and a stable nuclide that are produced by similar sets of nuclear reactions, provided that the stable nuclide is present with low initial abundance. The standard methods rely on either K-40 (t(sub 1/2) = 1.26 Gy), K-39, and K-41 or on a shorter-lived radionuclide and a stable, noble gas isotope. Widely used pairs of this type include Cl-36/Ar-36 and Al-26/Ne-21. Other pairs that may serve the purpose for iron meteorites contain many stable isotopes besides those of K and the noble gases that are produced partly by cosmic rays. We consider here the calculation of exposure ages, t(sub 26), from measurements of Al-26 (t(sub 1/2) = 0.7 My) and (stable) Mg-26. Ages based on Al-26/Mg-26 ratios, like those based on Cl-36/Ar-36 ratios, are 'buffered' against changes in relative production rates due to shielding because decay of the radioactive nuclide accounts for a good part of the inventory of the stable nuclide.

Herzog, G. F.↗

Galileo Probe Mass Spectrometer experiment

The chemical and isotopic composition of the Jupiter atmosphere's constituents, including their vertical variations, will be measured by the Galileo Probe Mass Spectrometer instrument through in situ sampling; batch sampling will also be undertaken for noble gas composition and isotopic ratio determinations. The instrument's gas-sampling system is connected to a quadrupole mass analyzer for molecular weight analysis. Threshold values are lowered through sample enrichment by a factor of 100-500 for stable hydrocarbons and by a factor of 10 for noble gases. The instrument follows a sampling sequence of 8192 steps, at a rate of 2 steps/sec.

Niemann, H. B.↗

Gas ionization solar spectral monitor (GISSMO)

We are currently developing an instrument free from optical components to measure the full-disk solar spectrum in the extreme ultraviolet regime covering wavelengths from 75-500 A. The instrument, which will be launched aboard a NASA Black Brant sounding rocket in September 1992, consists of a windowless noble gas ionization cell followed by a toroidal electrostatic analyzer to spatially disperse photoelectrons as a function of their energies. A microchannel plate based position sensitive detector will be used to detect individual electrons, indirectly returning the solar EUV spectrum.

Vickers, James S.↗

Inward electrostatic precipitation of interplanetary particles

An inward precipitator collects particles initially dispersed in a gas throughout either a cylindrical or spherical chamber onto a small central planchet. The instrument is effective for particle diameters greater than about 1 micron. One use is the collection of interplanetary dust particles (IDPs) which are stopped in a noble gas (xenon) by drag and ablation after perforating the wall of a thin-walled spacecraft-mounted chamber. First, the particles are positively charged for several seconds by the corona production of positive xenon ions from inward facing needles placed on the chamber wall. Then an electric field causes the particles to migrate toward the center of the instrument and onto the planchet. The collection time (on the order of hours for a 1 m radius spherical chamber) is greatly reduced by the use of optimally located screens which reapportion the electric field. Some of the electric field lines terminate on the wires of the screens so a fraction of the total number of particles in the chamber is lost. The operation of the instrument is demonstrated by experiments which show the migration of carbon soot particles with radius of approximately 1 micron in a 5 cm diameter cylindrical chamber with a single field enhancing screen toward a 3.2 mm central collection rod.

Rulison, Aaron J.↗

Stratospheric Collection of Dust from Comet 73P/Schwassmann-Wachmann 3

Interplanetary dust particles (IDPs) collected in the stratosphere are unique materials that are compositionally distinct from meteorites. Astronomical observations and dynamical models indicate that both asteroids and short-period comets are significant sources of IDPs. IDPs having fragile, porous structures, unequilibrated, anhydrous mineralogy, and high atmospheric entry velocities are thought to derive from comets, whereas asteroidal IDPs are identified by their compact structure, hydrated mineralogy and low atmospheric entry velocities. Uncertainty remains in the classification of asteroidal and cometary IDPs owing to our limited sampling of comets and the asteroid belt and the complex dynamical histories of most IDPs in space. Most IDPs spend thousands of years in space prior to being accreted by the Earth. During this time, dust particles undergo orbital evolution, including gradual reduction in their perihelion and eccentricity as a result of Poynting-Robertson drag. Planetary encounters may also significantly change their orbital parameters. Consequently, it is generally not possible to identify the specific parent body of a given IDP. However, it has been proposed that it is possible to identify dust from comets that have formed Earth-crossing dust trails. In this case, the dust particles have been in space for such a short period of time (a few decades or less) that their orbits have not significantly changed. Furthermore, these fresh IDPs could be identified in the laboratory from their short space-exposure histories (low solar noble gas abundance and lack of solar flare tracks). NASA flew several dedicated IDP collection missions attempting to collect dust from comet 26P/Grigg-Skjellerup, the best candidate identified. Remarkably, many particles from those collectors exhibit unusual properties, including low abundances of solar noble gases and high abundances of presolar grains. These observations are consistent with the dust particles originating from comet Grigg-Skjellerup (hereafter G-S). This study considers the prospects for collection of dust from comet 73P/Schwassmann-Wachmann 3 (hereafter SW3). SW3 is a small (2 km diameter) Jupiter family comet whose perihelion is close to and just inside the Earth's orbit. The orbit of SW3 is suitable for producing a low-velocity Earth-crossing dust stream and is the likely parent of the Tau Herculid meteor stream. This study complements a previously published model of the SW3 meteor stream that predicted a very low level of activity for grains 100 micron -- 100 mm in size.

Messenger, Scott R.↗

Evaluation of subsurface transport processes of delayed gas signatures applicable to underground nuclear explosions

Radioactive gas signatures from underground nuclear explosions (UNEs) result from gas-migration processes occurring in the subsurface. The processes considered in this study either drive or retard upward migration of gases from the detonation cavity. The relative importance of these processes is evaluated by simulating subsurface transport in a dual-permeability medium for the multi-tracer Noble Gas Migration Experiment (NGME) originally intended to study some aspects of transport from a UNE. For this experiment, relevant driving processes include weak two-phase convection driven by the geothermal gradient, over pressuring of the detonation cavity, and barometric pumping while gas sorption, dissolution, radioactive decay, and usually diffusion represent retarding processes. From deterministic simulations we found that over-pressuring of the post-detonation chimney coupled with barometric pumping produced a synergistic effect amplifying the tracer-gas reaching the surface. Bounding simulations indicated that the sorption and dissolution of gases, tending to retard transport, were much smaller than anticipated by earlier laboratory studies. The NGME observations themselves show that differences in gas diffusivity have a larger effect on influencing upward transport than do the combined effects of tracer-gas sorption and dissolution, which is consistent with a Sobol’ sensitivity analysis. Both deterministic simulations and those considering parametric uncertainties of transport-related properties predict that the excess in concentration of SF 6 compared to 127 Xe as might be captured in small volumetric samples should be much smaller than the order-of-magnitude contrast found in the large-volume gas samples taken at the site. While extraction of large-volume subsurface gas samples is shown to be capable of distorting in situ gas compositions, the highly variable injection rate of SF 6 into the detonation cavity relative to that of 127 Xe at the start of the field experiment is the most likely explanation for the large difference in observed concentrations.

58 GEOSCIENCES↗

Isotopic fractionation of Kr and Xe implanted in solids at very low energies

Results on the implantation of Kr and Xe in W under closed system conditions at very low energies (50-500 eV) are reported. Investigation of the fraction of gas trapped as a function of time reveals the existence of competing trapping and release mechanisms, and analysis of recovered trapped gas and residual gas phases shows that both elemental and isotropic fractionation result from these mechanisms. It is determined that the mass dependence for the overall implantation process is at or near m exp 1, with heavier isotopes enriched in the implanted gas. This mass dependence is inferred to result from implantation and a combination of diffusive and gas sputtering release mechanisms. These results reaffirm the conclusion of Bernatowicz and Fahey (1986) that previously observed isotopic fractionation of Kr and Xe in carbonaceous material synthesized in electrical discharges owes its origin to low-energy ion implantation, and also suggest that this process may be relevant to incorporation of noble gases in early solar system materials. The implication of these results for noble gas mass spectrometry are discussed.

Bernatowicz, Thomas J.↗

Trapping of noble gases in proton-irradiated silicate smokes

We have measured Ne, Ar, Kr, and Xe in Si2O3 'smokes' that were condensed on Al substrates, vapor-deposited with various mixtures of CH4, NH3, H2O3 and noble gases at 10 K and subsequently irradiated with 1 MeV protons to simulate conditions during grain mantle formation in interstellar clouds. Neither Ne nor Ar is retained by the samples upon warming to room temperature, but Xe is very efficiently trapped and retained. Kr is somewhat less effectively retained, typically depleted by factors of about 10-20 relative to Xe. Isotopic fractionation favoring the heavy isotopes of Xe and Kr of about 5-10-percent/amu is observed. Correlations between the specific chemistry of the vapor deposition and heavy noble gas retention are most likely the result of competition by the various species for irradiation-produced trapping sites. The concentration of Xe retained by some of these smokes exceeds that observed in phase Q of meteorites and, like phase Q, they do not seem to be carriers of the light noble gases.

Nichols, R. H., Jr.↗

AGE (Argon Geochronology Experiment): An Instrument for Geochronology on the Surface of Mars

As our knowledge of the planet Mars continues to grow, one parameter that remains elusive is the absolute chronology of the planet s geological history. Although crater counts have provided a robust relative chronology, impactor fluxes are poorly enough known that there are places on Mars where the absolute age is uncertain by a factor of two or more. To resolve these uncertainties, it will be necessary to either analyze well-documented samples returned to the Earth from the Martian surface or to perform in situ measurements with sufficient precision. Sample return is still at least a decade away, and even then it might be from a biologically interesting area that might be geologically complex. Hence an in situ measurement, within an uncertainty of 20% or better, could greatly improve our knowledge of the history of Mars. With funding from the Planetary Instrument Definition and Development Program (PIDDP), we have been working on an instrument to perform potassium-argon (K-Ar) and cosmic-ray exposure (CRE) dating in situ on the surface of Mars. For either of these techniques, it is necessary to measure the abundance of one or more major or minor elements (K in the case of KAr; all majors and minors in the case of CRE) and the abundance and isotopes composition of a noble gas (Ar in the case of K-Ar; He, Ne and Ar for CRE dating). The technology for either of these types of measurements exists, but has never before been integrated for a spacecraft. We refer to the instrument as AGE, the Argon Geochronology Experiment (although we will measure the noble gases He and Ne as well for CRE ages). We report here on the basic components that go into such an instrument, both those that use existing technology and those that had to be developed to create the integrated package.

Swindle, T. D.↗

Investigating the Origin and Evolution of Venus with In Situ Mass Spectrometry

Measurement of noble gas abundances on Venus remain a high priority for planetary science. These studies are only possible through in situ measurement, and can be accomplished by a modern neutral mass spectrometer (NMS) such as that developed at NASA Goddard, based on flight-proven technology. Here we show how the measurement of noble gases can be secured using demonstrated enrichment techniques.

Venus↗

Comets, impacts, and atmospheres

Studies of element abundances and values of D/H in the atmospheres of the giant planets and Titan have emphasized the important role of icy planetesimals in the formation of these bodies. In these atmospheres, C/H and D/H increase as the relative masses of the 'cores' of the planets increase. N/H appears to deviate from this trend in an interesting way. In the inner solar system, the traditional approach of using carbonaceous chondrites as the source of planetary volatiles is in serious trouble because of the depletion of xenon and the unusual pattern of xenon isotopes found in the atmospheres of Earth and Mars, and because of the solar-type abundance ratios of argon, krypton and xenon and the large amounts of neon and argon on Venus. Recent studies of elemental abundances in comets, especially P/Halley, coupled with laboratory studies of the trapping of gas in ice formed at low temperatures by A. Bar-Nun et al. provide a consistent interpretation of all of these results. This interpretation emphasizes the fundamental importance of icy planetesimals (comets) and the randomness of early impacts in the formation of planetary systems. Cometary delivery by itself will not explain the noble gas abundances on the inner planets. There is good evidence for at least one additional source, which presumably consists of the rocky material making up the bulk of the planets. The existence of this rocky reservoir is manifested in the nucleogenic isotopes and in the neon which is found in all these atmospheres and is also present in the Earth's mantle. This neon may well be a relic of the planets' earliest, accretional atmospheres.

Owen, Tobias↗

Spectra from nuclear-excited plasmas

The paper discusses the spectra taken from He-3(n,p)H-3 nuclear-induced plasmas under high thermal neutron flux, lasing conditions. Also, initial spectra are presented for U-235F6 generated plasmas. From an evaluation of these spectra, important atomic and molecular processes that occur in the plasma can be inferred. The spectra presented are the first to be generated by He-3 and U-235F6 nuclear reactions under high neutron flux, lasing conditions. The U-235(n,ff)FF reaction, which liberates 165 MeV of fission-fragment kinetic energy, creates plasmas that are of great interest, since at sufficiently high densities of U-235F6 the gas becomes self-critical; thus, there is no need for an external driving reactor (source of neutrons). The spectra from mixtures of He-3 and Ar, Xe, Kr, Ne, Cl2, F2 and N2 indicate little difference between high-pressure nuclear-induced plasmas and high-pressure electrically pulsed afterglow plasmas for noble-gas systems

De Young, R. J.↗

Isotopic anomalies of noble gases in meteorites and their origins. IV - C3 /Ornans/ carbonaceous chondrites

The C3O chondrites Kainsaz, Lance, and Ornans were studied by an acid dissolution technique to characterize the noble gas components in 3 mineral fractions: HF, HCl-solubles, chromite and carbon, and 'phase Q', a trace mineral containing Ar, Kr, Xe. For all fractions, gas contents decline in the order Kainsaz, Lance, Ornans; this trend parallels volatile contents but not heterogeneity of olivine composition or degree of metamorphism, and reflects progressively higher condensation temperature from the solar nebula. The Ar/Xe ratios and compositions of the three mineral fractions are discussed, and it is concluded that in all primitive chondrites the amount and the chemical separability of CCFXe parallel the abundance of primordial noble gases and other volatiles, such as C, N, Tl, Bi, and In. The close correlation of CCFXe with properties of local origin, such as volatile content and petrologic type, is more consistent with a local than with an extrasolar origin of the component.

Alaerts, L.↗

Experimental technique to investigate the interstellar gas - Preliminary analysis

The Interstellar Gas Experiment (IGE) exposed thin metallic foils to collect neutral interstellar gas particles. These particles penetrate the solar system due to their motion relative to the sun. Thus, it was possible to entrap them in the collecting foils along with precipitating magnetospheric and perhaps some ambient atmospheric particles. For the entire duration of the Long Duration Exposure Facility mission, seven of these foils collected particles arriving from seven different directions as seen from the spacecraft. In the mass spectrometric analysis of the noble gas component of these particles, we have detected the isotopes of He-3, He-4, Ne-20, and Ne-22. In the foil analyses carried out so far, we find a distribution of particle arrival directions which shows that a significant part of the trapped particles are indeed interstellar atoms. The analysis needed to subtract the competing fluxes of magnetospheric and atmospheric particles is still in progress.

Lind, D. L.↗

Are the C delta light nitrogen and noble gases located in the same carrier?

Light nitrogen and the HL family noble gas components of C(sub delta) appear to be separable by high resolution pyrolysis experiments. Thus C(sub delta) is not a homogeneous material and probably consists of debris of many stars. The question of whether the N and Xe(HL) actually reside in different carriers continues to be addressed. It is well known that C(sub delta) which was identified as nanometer sized diamonds contains isotopically anamalous elements, in particular noble gases including Xe(HL) and its family and light nitrogen (delta(N-15) down to -350 percent). Before the true nature of C(sub delta) was recognized, it was easy to suppose that the Xe(HL) and light nitrogen were located in the same carrier. However, recognition that light nitrogen in diamond from different samples varies by greater than a factor of six compared to Xe(HL) fluctuations of ca. 20 percent makes such an assumption questionable. On the basis of simple arithmetic logic, the Xe and nitrogen cannot be absolutely co-located. The average diamond grain consists of only about 1000-2000 atoms of carbon; one grain among a few x 10(exp 6) contains an atom of Xe(HL) while 5-30 atoms of light nitrogen are the typical number which need to be in every diamond grain to account for observed concentrations. If some grains are devoid of N, the others have to have a higher N concentration. Even if we were able to analyze an individual grain of the diamond for noble gases and nitrogen, we would be faced with the monumental task of locating the one amongst 10(exp 6) identical grains containing the Xe atom to examine its nitrogen content. The problem can be simplified to some extent if instead of Xe, He which is 10(exp 4) times more abundant is assumed to be a member of the HL family. Attempts to fractionate the separate carriers might be attempted using He and N as guiding indicators but even experiments of this nature are for the future. Faced with apparently insoluble problems, we have returned to an investigation we last used in our original efforts to find isotopically light nitrogen, that is to compare release patterns of the different components during stepped pyrolysis and combustion.

Verchovsky, A. B.↗

The interstellar gas experiment

The Interstellar Gas Experiment (IGE) exposed thin metallic foils to collect neutral interstellar gas particles. These particles penetrate the solar system due to their motion relative to the sun. Thus, it is possible to entrap them in the collecting foils along with precipitating magnetospheric and perhaps some ambient atmospheric particles. For the entire duration of the Long Duration Exposure Facility (LDEF) mission, seven of these foils collected particles arriving from seven different directions as seen from the spacecraft. In the mass spectroscopic analysis of the noble gas component of these particles, we have detected the isotopes of He-3, He-4, Ne-20, and Ne-22. In the foil analyses carried out so far, we find a distribution of particle arrival directions which shows that a significant part of the trapped particles are indeed interstellar atoms. The analysis needed to subtract the competing fluxes of magnetospheric and atmospheric particles is still in progress.

Lind, D. L.↗

Distinct Chlorine Isotopic Reservoirs on Mars: Implications for Character, Extent and Relative Timing of Crustal Interaction with Mantle-Derived Magmas, Evolution of the Martian Atmosphere, and the Building Blocks of an Early Mars

The style, magnitude, timing, and mixing components involved in the interaction between mantle derived Martian magmas and Martian crust have long been a point of debate. Understanding this process is fundamental to deciphering the composition of the Martian crust and its interaction with the atmosphere, the compositional diversity and oxygen fugacity variations in the Martian mantle, the bulk composition of Mars and the materials from which it accreted, and the noble gas composition of Mars and the Sun. Recent studies of the chlorine isotopic composition of Martian meteorites imply that although the variation in delta (sup 37) Cl is limited (total range of approximately14 per mille), there appears to be distinct signatures for the Martian crust and mantle. However, there are potential issues with this interpretation. New Cl isotope data from the SAM (Sample Analysis at Mars) instrument on the Mars Science Lab indicate a very wide range of Cl isotopic compositions on the Martian surface. Recent measurements by [10] duplicated the results of [7,8], but placed them within the context of SAM surface data. In addition, Martian meteorite Chassigny contains trapped noble gases with isotopic ratios similar to solar abundance, and has long been considered a pristine, mantle derived sample. However, previous studies of apatite in Chassigny indicate that crustal fluids have interacted with regions interstitial to the cumulus olivine. The initial Cl isotope measurements of apatite in Chassigny suggest an addition of crustal component to this lithology, apparently contradicting the rare gas data. Here, we examine the Cl isotopic composition of multiple generations and textures of apatite in Chassigny to extricate the crustal and mantle components in this meteorite and to reveal the style and timing of the addition of crustal components to mantle-derived magmas. These data reveal distinct Martian Cl sources whose signatures have their origins linked to both the early Solar System and the evolving Martian atmosphere.

Shearer, C. K.↗