Diverging effects of isotopic fractionation upon molecular diffusion of noble gases in water: mechanistic insights through ab initio molecular dynamics simulations.

PubMed

Pinto de Magalhães, Halua; Brennwald, Matthias S; Kipfer, Rolf

2017-03-22

Atmospheric noble gases are routinely used as natural tracers to analyze gas transfer processes in aquatic systems. Their isotopic ratios can be employed to discriminate between different physical transport mechanisms by comparison to the unfractionated atmospheric isotope composition. In many applications of aquatic systems molecular diffusion was thought to cause a mass dependent fractionation of noble gases and their isotopes according to the square root ratio of their masses. However, recent experiments focusing on isotopic fractionation within a single element challenged this broadly accepted assumption. The determined fractionation factors of Ne, Ar, Kr and Xe isotopes revealed that only Ar follows the prediction of the so-called square root relation, whereas within the Ne, Kr and Xe elements no mass-dependence was found. The reason for this unexpected divergence of Ar is not yet understood. The aim of our computational exercise is to establish the molecular-resolved mechanisms behind molecular diffusion of noble gases in water. We make the hypothesis that weak intermolecular interactions are relevant for the dynamical properties of noble gases dissolved in water. Therefore, we used ab initio molecular dynamics to explicitly account for the electronic degrees of freedom. Depending on the size and polarizability of the hydrophobic particles such as noble gases, their motion in dense and polar liquids like water is subject to different diffusive regimes: the inter-cavity hopping mechanism of small particles (He, Ne) breaks down if a critical particle size achieved. For the case of large particles (Kr, Xe), the motion through the water solvent is governed by mass-independent viscous friction leading to hydrodynamical diffusion. Finally, Ar falls in between the two diffusive regimes, where particle dispersion is propagated at the molecular collision time scale of the surrounding water molecules.

Noble gases in Mars atmosphere: new precise analysis with Paloma

NASA Astrophysics Data System (ADS)

Sarda, Ph.; Paloma Team

2003-04-01

The Viking mission embarked a mass spectrometer designed by Alfred O. Nier that yielded the first determination of the elemental and isotopic composition of noble gases in Mars atmosphere. For example, the 40Ar/36Ar ratio in martian air is roughly 10 fold that in terrestrial air. This extraordinary accomplishment, however, has furnished only partial results with large analytical uncertainties. For example, we do not know the isotopic composition of helium, and only very poorly that of Ne, Kr and Xe. In planetary science, it is fundamental to have a good knowledge of the atmosphere because this serves as a reference for all further studies of volatiles. In addition, part of our present knowledge of Mars atmosphere is based on the SNC meteorites, and again points to important differences between the atmospheres of Earth and Mars. For example the 129Xe/132Xe ratio of martian atmosphere would be twice that of terrestrial air and the 36Ar/38Ar ratio strongly different from the terrestrial or solar value. There is a need for confirming that the atmospheric components found in SNC meteorites actually represents the atmosphere of Mars, or to determine how different they are. Paloma is an instrument designed to generate elemental and isotopic data for He, Ne, Ar, Kr and Xe (and other gases) using a mass spectrometer with a purification and separation line. Gas purification and separation did not exist on the Vicking instrument. Because Paloma includes purification and separation, we expect strong improvement in precision. Ne, Ar and Xe isotope ratios should be obtained with an accuracy of better than 1%. Determination of the presently unknown ^3He/^4He ratio is also awaited from this experiment. Knowledge of noble gas isotopes in Mars atmosphere will allow some insight into major planetary processes such as degassing (^3He/^4He, 40Ar/36Ar, 129Xe/130Xe, 136Xe/130Xe), gravitational escape to space (^3He/^4He, 20Ne/22Ne), hydrodynamic escape and/or impact erosion of the

MRI using hyperpolarized noble gases.

PubMed

Kauczor, H; Surkau, R; Roberts, T

1998-01-01

The aim of this study was to review the physical basis of MRI using hyperpolarized noble gases as well as the present status of preclinical and clinical applications. Non-radioactive noble gases with a nuclear spin 1/2 (He-3, Xe-129) can be hyperpolarized by optical pumping. Polarization is transferred from circularly polarized laser light to the noble-gas atoms via alkali-metal vapors (spin exchange) or metastable atoms (metastability exchange). Hyperpolarization results in a non-equilibrium polarization five orders of magnitude higher than the Boltzmann equilibrium compensating for the several 1000 times lower density of noble gases as compared with liquid state hydrogen concentrations in tissue and allows for short imaging times. Hyperpolarization can be stored sufficiently long (3 h to 6 days) to allow for transport and application. Magnetic resonance systems require a broadband radio-frequency system - which is generally available for MR spectroscopy - and dedicated coils. The hyperpolarized gases are administered as inhalative "contrast agents" allowing for imaging of the airways and airspaces. Besides the known anesthetic effect of xenon, no adverse effects are observed in volunteers or patients. Pulse sequences are optimized to effectively use the non-renewable hyperpolarization before it decays or is destroyed, using fast low-flip-angles strategies to allow for dynamic/breath-hold imaging of highly diffusible (He) or soluble (Xe) gases with in vivo T1-times well below 1 min. Since helium is not absorbed in considerable amounts, its application is restricted to the lung. Xe-129 is also under investigation for imaging of white matter disease and functional studies of cerebral perfusion. Magnetic resonance imaging using hyperpolarized gases is emerging as a technical challenge and opportunity for the MR community. Preliminary experience suggests potential for functional imaging of pulmonary ventilation and cerebral perfusion.

Noble gases, nitrogen, cosmic ray exposure history and mineralogy of Beni M'hira (L6) chondrite

NASA Astrophysics Data System (ADS)

Mahajan, Ramakant R.; Nejia, Laridhi Ouazaa; Ray, Dwijesh; Naik, Sekhar

2018-03-01

The concentrations and isotopic composition of noble gases helium (He), neon (Ne), argon (Ar), krypton (Kr), xenon(Xe) and nitrogen were measured in the Beni M'hira L6 chondrite. The cosmic ray exposure age of Beni M'hira is estimated of 15.6 ± 3.7 (Ma). The radiogenic age, of around 485 ± 64 Ma, derived from 4He, and of around 504 ± 51 Ma from 40Ar, suggests an age resetting indicating the event impact. The heavy noble gases (Ar, Kr and Xe) concentrations imply that the gas is a mixture of trapped component Q and solar wind. The measured nitrogen abundance of 0.74 ppm and the isotopic signature of δ15N = 14.6‰ are within the range of ordinary chondrites. The homogeneous chemical composition of olivine (Fa:26 ± 0.25) and low-Ca pyroxene (Fs:22.4 ± 0.29) suggest that the Beni M'hira meteorite is an equilibrated chondrite. This is further corroborated by strong chondrule-matrix textural integration (lack of chondrules, except a few relict clast). Shock metamorphism generally corresponds to S5 (>45 GPa), however, locally disequilibrium melting (shock-melt veins) suggests, that the peak shock metamorphism was at ∼75 GPa, 950 °C.

Noble gases in CH 4-rich gas fields, Alberta, Canada

NASA Astrophysics Data System (ADS)

Hiyagon, H.; Kennedy, B. M.

1992-04-01

The elemental and isotopic compositions of helium, neon, argon, and xenon in twenty-one CH 4-rich natural gas samples from Cretaceous and Devonian reservoirs in the Alberta, Canada, sedimentary basin were measured. In all but a few cases, radiogenic ( 4He, 40Ar, and 131-136Xe) and nucleogenic ( 21,22Ne) isotopes dominated. Based solely on the noble gas composition, two types of natural gas reservoirs are identified. One (Group B) is highly enriched in radiogenic-nucleogenic noble gases and varies little in composition: 3He /4He = 1.5 ± 0.5 × 10 -8, 40Ar /36Ar = 5000-6500 , 40∗Ar /4He = 0.10 , 136∗Xe /4He ~ 0.7 × 10 -9, and 21∗Ne /22∗Ne = 0.452 ± 0.041 (∗ denotes radiogenic or nucleogenic origin; all 4He is radiogenic). High nitrogen content with 4He /N 2 ~ 0.06 is also characteristic of Group B samples. The remaining samples (Group A) contain a radiogenic-nucleogenic component with a different composition and, relative to Group B samples, the extent of enrichment in this component is less and more variable: 3He /4He = 10-70 × 10 -8, 40Ar /36Ar < 1550 , and 40∗Ar /4He ~ 0.25 . The composition of Group B radiogenic-nucleogenic noble gases is consistent with production in crust of average composition. Enrichment in Group B noble gases and nitrogen increases with proximity to the underlying Precambrian basement, consistent with a present-day mass flux into the overlying sedimentary basin. Inferred 40∗Ar /136∗Xe 4He ratios imply a basement source enriched in thorium relative to uranium and potassium (Th/U > 20). Combined, the overall lower total radiogenic-nucleogenic content of Group A reservoirs, the greater variability in composition, and the appearance of Group A noble gases in reservoirs higher in the sedimentary sequence relative to the underlying basement implies that the Group A radiogenic-nucleogenic noble gases are indigenous to the sediments. The most interesting aspect of the Group A noble gases are the very high 3He /4He ratios; ~ 10

Sorption of noble gases by solids, with reference to meteorites. II - Chromite and carbon. III - Sulfides, spinels, and other substances; on the origin of planetary gases

NASA Technical Reports Server (NTRS)

Yang, J.; Anders, E.

1982-01-01

The trapping of noble gases by chromite and carbon, two putative carriers of primordial noble gases in meteorites, was studied by synthesizing 19 samples in a Ne-Ar-Kr-Xe atmosphere at 440-720 K. Noble gas contents are found to approximately obey Henry's Law, but only slight correlations are found with composition, surface area, or adsorption temperature. Geometric mean distribution coefficients for bulk samples and HCl residues in 10 cu cm STP/g atm are: Xe 100, Kr 15, Ar 3.5, and Ne 0.62. Elemental fractionation data support the suggestion of Lewis et al. (1977) that chromite and carbon in C2 and C3 chondrites were formed by the reaction: Fe, Cr + 4CO yields (Fe, Cr)3O4 + 4C + carbides. In contrast to meteoritic minerals, the synthetic specimens show no isotopic fractionation of noble gases. In a subsequent study, attention is given to the cases of sulfides and spinels, on the way to consideration of the origin of planetary gases. Sulfides showed three distinctive trends relative to chromite or magnetite. The elemental fractionation pattern of Ar, Kr and Xe in meteorites, terrestrial rocks and planets resembles the adsorption patterns on the carbons, spinels, sulfides, and other solids studied. The high release temperature of meteoritic noble gases may be explained by transformation of the physisorbed or chemisorbed gas. The ready loss of meteoritic heavy gases on surficial oxidation is consistent with adsorption, as is the high abundance.

Heavy noble gases in solar wind delivered by Genesis mission.

PubMed

Meshik, Alex; Hohenberg, Charles; Pravdivtseva, Olga; Burnett, Donald

2014-02-15

One of the major goals of the Genesis Mission was to refine our knowledge of the isotopic composition of the heavy noble gases in solar wind and, by inference, the Sun, which represents the initial composition of the solar system. This has now been achieved with permil precision: 36 Ar/ 38 Ar = 5.5005 ± 0.0040, 86 Kr/ 84 Kr = .3012 ± .0004, 83 Kr/ 84 Kr = .2034 ± .0002, 82 Kr/ 84 Kr = .2054 ± .0002, 80 Kr/ 84 Kr = .0412 ± .0002, 78 Kr/ 84 Kr = .00642 ± .00005, 136 Xe/ 132 Xe = .3001 ± .0006, 134 Xe/ 132 Xe = .3691 ± .0007, 131 Xe/ 132 Xe = .8256 ± .0012, 130 Xe/ 132 Xe = .1650 ± .0004, 129 Xe/ 132 Xe = 1.0405 ± .0010, 128 Xe/ 132 Xe = .0842 ± .0003, 126 Xe/ 132 Xe = .00416 ± .00009, and 124 Xe/ 132 Xe = .00491 ± .00007 (error-weighted averages of all published data). The Kr and Xe ratios measured in the Genesis solar wind collectors generally agree with the less precise values obtained from lunar soils and breccias, which have accumulated solar wind over hundreds of millions of years, suggesting little if any temporal variability of the isotopic composition of solar wind krypton and xenon. The higher precision for the initial composition of the heavy noble gases in the solar system allows (1) to confirm that, exept 136 Xe and 134 Xe, the mathematically derived U-Xe is equivalent to Solar Wind Xe and (2) to provide an opportunity for better understanding the relationship between the starting composition and Xe-Q (and Q-Kr), the dominant current "planetary" component, and its host, the mysterious phase-Q.

Heavy noble gases in solar wind delivered by Genesis mission

PubMed Central

Meshik, Alex; Hohenberg, Charles; Pravdivtseva, Olga; Burnett, Donald

2017-01-01

One of the major goals of the Genesis Mission was to refine our knowledge of the isotopic composition of the heavy noble gases in solar wind and, by inference, the Sun, which represents the initial composition of the solar system. This has now been achieved with permil precision: 36Ar/38Ar = 5.5005 ± 0.0040, 86Kr/84Kr = .3012 ± .0004, 83Kr/84Kr = .2034 ± .0002, 82Kr/84Kr = .2054 ± .0002, 80Kr/84Kr = .0412 ± .0002, 78Kr/84Kr = .00642 ± .00005, 136Xe/132Xe = .3001 ± .0006, 134Xe/132Xe = .3691 ± .0007, 131Xe/132Xe = .8256 ± .0012, 130Xe/132Xe = .1650 ± .0004, 129Xe/132Xe = 1.0405 ± .0010, 128Xe/132Xe = .0842 ± .0003, 126Xe/132Xe = .00416 ± .00009, and 124Xe/132Xe = .00491 ± .00007 (error-weighted averages of all published data). The Kr and Xe ratios measured in the Genesis solar wind collectors generally agree with the less precise values obtained from lunar soils and breccias, which have accumulated solar wind over hundreds of millions of years, suggesting little if any temporal variability of the isotopic composition of solar wind krypton and xenon. The higher precision for the initial composition of the heavy noble gases in the solar system allows (1) to confirm that, exept 136Xe and 134Xe, the mathematically derived U–Xe is equivalent to Solar Wind Xe and (2) to provide an opportunity for better understanding the relationship between the starting composition and Xe-Q (and Q-Kr), the dominant current “planetary” component, and its host, the mysterious phase-Q. PMID:29151613

Monolayer adsorption of noble gases on graphene

NASA Astrophysics Data System (ADS)

Maiga, Sidi M.; Gatica, Silvina M.

2018-02-01

We report our results of simulations of the adsorption of noble gases (Kr, Ar, Xe) on graphene. For Kr, we consider two configurations: supported and free-standing graphene, where atoms are adsorbed only on one or two sides of the graphene. For Ar and Xe, we studied only the case of supported graphene. For the single-side adsorption, we calculated the two-dimensional gas-liquid critical temperature for each adsorbate. We determined the different phases of the monolayers and constructed the phase diagrams. We found two-dimensional incommensurate solid phases for krypton, argon and xenon, and a two-dimensional commensurate solid phase for krypton. For double side adsorption of Kr, we do not see evidence of an ordering transition driven by the interlayer forces.

Adsorption properties of fission gases Xe and Kr on pristine and doped graphene: A first principle DFT study

NASA Astrophysics Data System (ADS)

Vazhappilly, Tijo; Ghanty, Tapan K.; Jagatap, B. N.

2017-07-01

Graphene has excellent adsorption properties due to large surface area and has been used in applications related to gas sorption and separation. The separation of radioactive noble gases using graphene is an interesting area of research relevant to nuclear waste management. Radioactive noble gases Xe and Kr are present in the off-gas streams from nuclear fission reactors and spent nuclear fuel reprocessing plants. The entrapment of these volatile fission gases is important in the context of nuclear safety. The separation of Xe from Kr is extremely difficult, and energy intensive cryogenic distillation is generally employed. Physisorption based separation techniques using porous materials is a cost effective alternative to expensive cryogenic distillation. Thus, adsorption of noble gases on graphene is relevant for fundamental understanding of physisorption process. The properties of graphene can be tuned by doping and incorporation of defects. In this regard, we study the binding affinity of Xe and Kr in pristine and doped graphene sheets. We employ first principle calculations using density functional theory, corrected for dispersion interactions. The structural parameters obtained from the current study show excellent agreement with the available theoretical and experimental observations on similar systems. Noble gas adsorption energies on pristine graphene match very well with the available literature. Our results show that the binding energy of fission gases Xe and Kr on graphene can be considerably improved through doping the lattice with a heteroatom.

Santa Lucia (2008) (L6) Chondrite, a Recent Fall: Composition, Noble Gases, Nitrogen and Cosmic Ray Exposure Age

NASA Astrophysics Data System (ADS)

Mahajan, Ramakant R.; Varela, Maria Eugenia; Joron, Jean Louis

2016-04-01

The Santa Lucia (2008)—one the most recent Argentine meteorite fall, fell in San Juan province, Argentina, on 23 January 2008. Several masses (total ~6 kg) were recovered. Most are totally covered by fusion crust. The exposed interior is of light-grey colour. Chemical data [olivine (Fa24.4) and low-Ca pyroxene (En77.8 Fs20.7 Wo1.6)] indicate that Santa Luica (2008) is a member of the low iron L chondrite group, corresponding to the equilibrated petrologic type 6. The meteorite name was approved by the Nomenclature Committee (NomCom) of the Meteoritical Society (Meteoritic Bulletin, no. 97). We report about the chemical composition of the major mineral phases, its bulk trace element abundance, its noble gas and nitrogen data. The cosmic ray exposure age based on cosmogenic 3He, 21Ne, and 38Ar around 20 Ma is comparable to one peak of L chondrites. The radiogenic K-Ar age of 2.96 Ga, while the young U, Th-He are of 1.2 Ga indicates that Santa Lucia (2008) lost radiogenic 4He more recently. Low cosmogenic (22Ne/21Ne)c and absence of solar wind noble gases are consistent with irradiation in a large body. Heavy noble gases (Ar/Kr/Xe) indicated trapped gases similar to ordinary chondrites. Krypton and neon indicates irradiation in large body, implying large pre-atmospheric meteoroid.

Exploring the Effects on Lipid Bilayer Induced by Noble Gases via Molecular Dynamics Simulations

NASA Astrophysics Data System (ADS)

Chen, Junlang; Chen, Liang; Wang, Yu; Wang, Xiaogang; Zeng, Songwei

2015-11-01

Noble gases seem to have no significant effect on the anesthetic targets due to their simple, spherical shape. However, xenon has strong narcotic efficacy and can be used clinically, while other noble gases cannot. The mechanism remains unclear. Here, we performed molecular dynamics simulations on phospholipid bilayers with four kinds of noble gases to elucidate the difference of their effects on the membrane. Our results showed that the sequence of effects on membrane exerted by noble gases from weak to strong was Ne, Ar, Kr and Xe, the same order as their relative narcotic potencies as well as their lipid/water partition percentages. Compared with the other three kinds of noble gases, more xenon molecules were distributed between the lipid tails and headgroups, resulting in membrane’s lateral expansion and lipid tail disorder. It may contribute to xenon’s strong anesthetic potency. The results are well consistent with the membrane mediated mechanism of general anesthesia.

Noble Gases in the LEW 88663 L7 Chondrite

NASA Astrophysics Data System (ADS)

Miura, Y. N.; Sugiura, N.; Nagao, K.

1995-09-01

LEW88663 and some meteorites (e.g. Shaw) are the most highly metamorphosed meteorites among L group chondrites. Although the abundances of lithophile elements and oxygen isotopic compositions of the L7 chondrite LEW88663 (total recovered mass: 14.5g) are close to those of the range for L chondrites [1,2], metallic iron is absent and concentrations of siderophile elements are about half of typical values for L chondrites [3,4]. Petrographical and geochemical observation suggested that this meteorite has experienced partial melting [5]. As a part of our study on differentiated meteorites, we also investigated noble gases in this meteorite. We present here noble gas compositions of LEW88663 and discuss history of this meteorite. In addition, we will consider whether there is any evidence for bridging between chondrites and achondrites. Noble gases were extracted from a whole rock sample weighing 66.31 mg by total fusion, and all stable noble gas isotopes as well as cosmogenic radioactive 81Kr were analyzed using a mass spectrometer at ISEI, Okayama University. The results are summarized in the table. The concentrations of cosmogenic ^3He, ^21Ne, and ^38Ar are 7.3, 1.6 and 3.1x10^-8 cm^3STP/g, respectively. The cosmic-ray exposure ages based on them are calculated to be 4.7, 6.9 and 8.8 m.y., respectively, using the production rates proposed by [6, 7] and mean chemical compositions of L chondrites. The shorter cosmic-ray exposure ages T(sub)3 and T(sub)21 than T(sub)38 would be due to diffusive loss of lighter noble gases from the meteorite. The concentrations of trapped Kr and Xe in LEW88663 are lower than those for L6 chondrites [8], supporting thermal metamorphism for the meteorite higher than that for L6 chondrites. The Kr and Xe are isotopically close to those of the terrestrial atmospheric Kr and Xe, and elemental abundance ratios for Ar, Kr and Xe suggest adsorbed noble gas patterns of the terrestrial atmosphere. The terrestrial atmospheric Ar, Kr and Xe (most

Negligible fractionation of Kr and Xe isotopes by molecular diffusion in water

NASA Astrophysics Data System (ADS)

Tyroller, Lina; Brennwald, Matthias S.; Busemann, Henner; Maden, Colin; Baur, Heinrich; Kipfer, Rolf

2018-06-01

Molecular diffusion is a key transport process for noble gases in water. Such diffusive transport is often thought to cause a mass-dependent fractionation of noble gas isotopes that is inversely proportional to the square root of the ratio of their atomic mass, referred to as the square root relation. Previous studies, challenged the commonly held assumption that the square root relation adequately describes the behaviour of noble gas isotopes diffusing through water. However, the effect of diffusion on noble gas isotopes has only been determined experimentally for He, Ne and Ar to date, whereas the extent of fractionation of Kr and Xe has not been measured. In the present study the fractionation of Kr and Xe isotopes diffusing through water immobilised by adding agar was quantified through measuring the respective isotope ratio after diffusing through the immobilised water. No fractionation of Kr and Xe isotopes was observed, even using high-precision noble gas analytics. These results complement our current understanding on isotopic fractionation of noble gases diffusing through water. Therefore this complete data set builds a robust basis to describe molecular diffusion of noble gases in water in a physical sound manner which is fundamental to assess the physical aspects of gas dynamics in aquatic systems.

Noble Gases

NASA Astrophysics Data System (ADS)

Podosek, F. A.

2003-12-01

approximate abundance they are found, how they relate to non-noble neighbors, and, to some extent, how they are associated with specific nuclear processes. Figure 1 provides assistance in this regard. (6K)Figure 1. A display of the isotopes of the noble gases and neighboring isotopes in the familiar "chart of the nuclides" format. The abscissa is neutron number (N) and the ordinate is proton number (Z). The box corresponding to any pair (Z, N) represents an isotope; an element is represented by a horizontal row. Boxes for stable isotopes are shown with solid outline; for the noble gases, approximate solar (in the case of He, protosolar) isotope ratios are shown at the bottom of each box. Selected unstable isotopes are shown as boxes with broken line edges. The left-superscript isotope label is the atomic weight A (=Z+N). The five panels show regions around the five noble gases (excluding Rn). When the goal is to identify and quantify different noble-gas components that may be present in a sample or group of samples, a common approach to this goal is to try to unmix the components, at least partially, to provide some leverage. One path to this end, of course, is analysis of different samples that may contain the components in different proportions, and thus have different isotopic compositions. Another path, available in addition to or instead of the first, is stepwise heating analysis, which has traditionally been very extensively used in noble-gas studies. Noble gases may be released from solid samples by volume diffusion, or by reaction, recrystallization, melting, or even evaporation of their host phases. If different noble-gas components reside in physically distinct locations within a complex sample, they may be liberated, and thus become available for analysis, at different steps in a time-temperature heating sequence. Differential release of isotopically distinct components will then result in variation of the isotopic composition of gas released in different steps (e

Multidiffusion mechanisms for noble gases (He, Ne, Ar) in silicate glasses and melts in the transition temperature domain: Implications for glass polymerization

NASA Astrophysics Data System (ADS)

Amalberti, Julien; Burnard, Pete; Laporte, Didier; Tissandier, Laurent; Neuville, Daniel R.

2016-01-01

Noble gases are ideal probes to study the structure of silicate glasses and melts as the modifications of the silicate network induced by the incorporation of noble gases are negligible. In addition, there are systematic variations in noble gas atomic radii and several noble gas isotopes with which the influence of the network itself on diffusion may be investigated. Noble gases are therefore ideally suited to constrain the time scales of magma degassing and cooling. In order to document noble gas diffusion behavior in silicate glass, we measured the diffusivities of three noble gases (4He, 20Ne and 40Ar) and the isotopic diffusivities of two Ar isotopes (36Ar and 40Ar) in two synthetic basaltic glasses (G1 and G2; 20Ne and 36Ar were only measured in sample G1). These new diffusion results are used to re-interpret time scales of the acquisition of fractionated atmospheric noble gas signatures in pumices. The noble gas bearing glasses were synthesized by exposing the liquids to high noble gas partial pressures at high temperature and pressure (1750-1770 K and 1.2 GPa) in a piston-cylinder apparatus. Diffusivities were measured by step heating the glasses between 423 and 1198 K and measuring the fraction of gas released at each temperature step by noble gas mass spectrometry. In addition we measured the viscosity of G1 between 996 and 1072 K in order to determine the precise glass transition temperature and to estimate network relaxation time scales. The results indicate that, to a first order, that the smaller the size of the diffusing atom, the greater its diffusivity at a given temperature: D(He) > D(Ne) > D(Ar) at constant T. Significantly, the diffusivities of the noble gases in the glasses investigated do not display simple Arrhenian behavior: there are well-defined departures from Arrhenian behavior which occur at lower temperatures for He than for Ne or Ar. We propose that the non-Arrhenian behavior of noble gases can be explained by structural modifications

Primordial Noble Gases from Earth's Core

NASA Astrophysics Data System (ADS)

Wang, K.; Lu, X.; Brodholt, J. P.

2016-12-01

Recent partitioning experiment suggests helium is more compatible in iron melt than in molten silicates at high pressures (> 10 GPa) (1), thus provide the possibility of the core as being the primordial noble gases warehouse that is responsible for the high primordial/radiogenic noble gas isotopic ratios observed in plume-related basalts. However, the possible transportation mechanism of the noble gases from the core to the overlying mantle is still ambiguous, understanding how this process would affect the noble gas isotopic characteristics of the mantle is critical to validate this core reservoir model. As diffusion is a dominant mass transport process that plays an important role in chemical exchange at the core-mantle boundary (CMB), we have determined the diffusion coefficients of helium, neon and argon in major lower mantle minerals, i.e. periclase (MgO), bridgemanite (MgSiO3-Pv) and post-perovskite (MgSiO3-PPv), by first-principles calculation based on density functional theory (DFT). As expected, the diffusion rate of helium is the fastest at the CMB, which is in the range of 3 × 10-10 to 1 × 10-8 m2/s. The neon diffusion is slightly slower, from 5 × 10-10 to 5 × 10-9 m2/s. Argon diffuses slowest at the rate from 1 × 10-10 to 2 × 10-10 m2/s. We have further simulated the evolution of noble gas isotopic ratios in the mantle near the CMB. Considering its close relationship with the mantle plumes and very likely to be the direct source of "hot-spot" basalts, we took a close investigation on the large low-shear-velocity provinces (LLSVPs). Under reasonable assumptions based on our diffusion parameters, the modelling results indicate that LLSVP is capable of generating all the noble gas isotope signals, e.g., 3He/4He = 55 Ra, 3He/22Ne = 3.1, 3He/36Ar = 0.82, 40Ar/36Ar = 9500, that are in good agreement with the observed values in "hot-spot" basalts (2). Therefore, this core-reservior hypothesis is a self-consistent model that can fits in multiple noble gas

A long-term change of the AR/KR/XE fractionation in the solar corpuscular radiation

NASA Technical Reports Server (NTRS)

Wieler, R.; Baur, H.; Signer, P.

1993-01-01

Solar noble gases in an ilmenite separate from breccia 79035 (antiquity greater than 1 Ga) were analyzed by closed system stepped etching (CSSE). All five gases show the familiar two-component structure: first solar-wind (SW) gases are released, followed by gases from solar energetic particles (SEP). Element patterns in 79035 are similar to those of 71501 ilmenite. SW-He-Ne were partly lost, but SEP-He-Ne-Ar are retained (nearly) unfractionated. Constant Ar/Kr/Xe ratios indicate that ilmenites contain an unfractionated sample of the heavy SW-SEP noble gases. Ar/Kr/Xe ratios in the solar corpuscular radiation are, however, different from 'solar system' values, whereby the Kr/Xe difference in 79035 is about twice as large as in 71501. We propose that Xe is less fractionated than Kr and Ar, though its first ionization potential (FIP) is higher than the 'cutoff' at approximately 11.5 eV, above which all elements in SEP are usually assumed to be depleted by a roughly constant factor. SW-Ne may be isotopically slightly heavier in the ancient SW trapped by 79035, as proposed earlier. In this work we extend our previous CSSE studies of solar noble gases including Kr and Xe to a lunar sample irradiated at least 1 Ga ago (breccia 79035, ilmenite separate, 42-64 microns). This sample was particularly gently etched in the first steps. Surprisingly, the first three steps, each releasing less than or equal to 0.5% of the total 36-Ar, showed an SEP-like trapped component plus relatively large concentrations of cosmogenic gases. Steps 4ff contain much less cosmogenic and more solar gas with a SW-like isotope pattern. Thus, a very minor easily etchable phase that has completely lost its SW-gases must be responsible for steps 1-3. We will not discuss these steps here and refer to the actual step 4 as the 'initial' etching step.

Noble gases in the moon

NASA Technical Reports Server (NTRS)

Manuel, O. K.; Srinivasan, B.; Hennecke, E. W.; Sinclair, D. E.

1972-01-01

The abundance and isotopic composition of helium, neon, argon, krypton, and xenon which were released by stepwise heating of lunar fines (15601.64) and (15271.65) were measured spectrometrically. The results of a composition of noble gases released from the lunar fines with noble gases in meteorites and in the earth are presented along with the isotopic composition of noble gases in lunar fines, in meteorites, and in the atmosphere. A study of two isotopically distinct components of trapped xenon in carbonaceous chondrites is also included.

Noble gases in gas shales : Implications for gas retention and circulating fluids.

NASA Astrophysics Data System (ADS)

Basu, Sudeshna; Jones, Adrian; Verchovsky, Alexander

2016-04-01

Gas shales from three cores of Haynesville-Bossier formation have been analysed simultaneously for carbon, nitrogen and noble gases (He, Ne, Ar, Xe) to constrain their source compositions and identify signatures associated with high gas retention. Ten samples from varying depths of 11785 to 12223 feet from each core, retrieved from their centres, have been combusted from 200-1200°C in incremental steps of 100°C, using 5 - 10 mg of each sample. Typically, Xe is released at 200°C and is largely adsorbed, observed in two of the three cores. The third core lacked any measureable Xe. High 40Ar/36Ar ratio up to 8000, is associated with peak release of nitrogen with distinctive isotopic signature, related to breakdown of clay minerals at 500°C. He and Ne are also mostly released at the same temperature step and predominantly hosted in the pore spaces of the organic matter associated with the clay. He may be produced from the uranium related to the organic matter. The enrichment factors of noble gases defined as (iX/36Ar)sample/(iX/36Ar)air where iX denotes any noble gas isotope, show Ne and Xe enrichment observed commonly in sedimentary rocks including shales (Podosek et al., 1980; Bernatowicz et al., 1984). This can be related to interaction of the shales with circulating fluids and diffusive separation of gases (Torgersen and Kennedy, 1999), implying the possibility of loss of gases from these shales. Interaction with circulating fluids (e.g. crustal fluids) have been further confirmed using 20Ne/N2, 36Ar/N2 and 4He/N2 ratios. Deviations of measured 4He/40Ar* (where 40Ar* represents radiogenic 40Ar after correcting for contribution from atmospheric Ar) from expected values has been used to monitor gas loss by degassing. Bernatowicz, T., Podosek, F.A., Honda, M., Kramer, F.E., 1984. The Atmospheric Inventory of Xenon and Noble Gases in Shales: The Plastic Bag Experiment. Journal of Geophysical Research 89, 4597-4611. Podosek, F.A., Honda, M., Ozima, M., 1980

Methane Sources and Migration Mechanisms in Shallow Groundwaters in Parker and Hood Counties, Texas-A Heavy Noble Gas Analysis.

PubMed

Wen, Tao; Castro, M Clara; Nicot, Jean-Philippe; Hall, Chris M; Larson, Toti; Mickler, Patrick; Darvari, Roxana

2016-11-01

This study places constraints on the source and transport mechanisms of methane found in groundwater within the Barnett Shale footprint in Texas using dissolved noble gases, with particular emphasis on 84 Kr and 132 Xe. Dissolved methane concentrations are positively correlated with crustal 4 He, 21 Ne, and 40 Ar and suggest that noble gases and methane originate from common sedimentary strata, likely the Strawn Group. In contrast to most samples, four water wells with the highest dissolved methane concentrations unequivocally show strong depletion of all atmospheric noble gases ( 20 Ne, 36 Ar, 84 Kr, 132 Xe) with respect to air-saturated water (ASW). This is consistent with predicted noble gas concentrations in a water phase in contact with a gas phase with initial ASW composition at 18 °C-25 °C and it suggests an in situ, highly localized gas source. All of these four water wells tap into the Strawn Group and it is likely that small gas accumulations known to be present in the shallow subsurface were reached. Additionally, lack of correlation of 84 Kr/ 36 Ar and 132 Xe/ 36 Ar fractionation levels along with 4 He/ 20 Ne with distance to the nearest gas production wells does not support the notion that methane present in these groundwaters migrated from nearby production wells either conventional or using hydraulic fracturing techniques.

Rubidium D1 collision shift by heavy noble gases

NASA Astrophysics Data System (ADS)

Wells, N. P.; Driskell, T. U.; Camparo, J. C.

2015-10-01

Using an isoclinic-point technique, we measured the D1 collision shift by Xe, ∂ [δ ν ]/∂ P , and the exponent κ of the shift's temperature dependence (i.e., δ ν ˜Tκ ). As demonstrated in our examination of the Rb-Kr system [N. P. Wells et al., Phys. Rev. A 89, 052516 (2014), 10.1103/PhysRevA.89.052516], the isoclinic point provides (arguably) the only means of assessing κ unambiguously: κKr=0.36 ±0.06 and in the present work κXe=0.32 ±0.05 . With our estimate of κ for the Rb-Kr and Rb-Xe systems, we were able to combine our Kr and Xe collision shift measurements with those of Rotondaro and Perram [M. D. Rotondaro and G. P. Perram, J. Quant. Spectrosc. Radiat. Transfer 57, 497 (1997), 10.1016/S0022-4073(96)00147-1] (another set of high quality ∂ [δ ν ]/∂ P measurements) to obtain a highly accurate experimental estimate for the D1 collision shift resulting from Rb's interaction with the heavy noble gases: For the Rb-Kr interaction ∂ [δ ν ] /∂ P |T =323 K=-5.02 ±0.07 MHz /torr and for the Rb-Xe interaction ∂ [δ ν ] /∂ P |T =323 K=-5.46 ±0.09 MHz /torr . These measured values for the collision-shift coefficient are approximately 20 % smaller (in magnitude) than the best theoretical estimates, suggesting that there is room for theoretical improvement regarding our present understanding of how noble-gas collisions perturb the alkali-metal P1 /2 state.

Barnett Shale or Strawn Group: Identifying the Source of Stray Gas through Noble Gases in the Trinity Aquifer, North-Central Texas

NASA Astrophysics Data System (ADS)

Wen, T.; Castro, M. C.; Nicot, J. P.; Hall, C. M.; Pinti, D. L.; Mickler, P. J.; Darvari, R.; Larson, T. E.

2017-12-01

The complete set of stable noble gases (He, Ne, Ar, Kr, Xe) is presented for Barnett Shale and Strawn Group production gas together with that of stray flowing gas present in the Trinity Aquifer, Texas. It places new constraints on the source of this stray gas and further shows that Barnett and Strawn gas have distinct crustal and atmospheric noble gas signatures, allowing clear identification of these two sources. Like Trinity Aquifer stray gas, Strawn gas is significantly more enriched in crustal 4He*, 21Ne*, and 40Ar* than Barnett gas. The similarity of Strawn and stray gas crustal noble gas signatures suggests that the Strawn is the source of stray gas in the Trinity Aquifer. Atmospheric 22Ne/36Ar ratios of stray gas mimic also that of Strawn, further reinforcing the notion that the source of stray gas in this aquifer is the Strawn. While noble gas signatures of Strawn and stray gas are consistent with a single-stage water degassing model, a two-stage oil modified groundwater exsolution fractionation model is required to explain the light atmospheric noble gas signature of Barnett Shale production gas. These distinct Strawn and Barnett noble gas signatures are likely the reflection of distinct evolution histories with Strawn gas being possibly older than that of Barnett Shale.

Laboratory simulation of meteoritic noble gases. III - Sorption of neon, argon, krypton, and xenon on carbon - Elemental fractionation

NASA Technical Reports Server (NTRS)

Wacker, John F.

1989-01-01

The sorption of Ne, Ar, Kr, and Xe was studied in carbon black, acridine carbon, and diamond in an attempt to understand the origin of trapped noble gases in meteorites. The results support a model in which gases are physically adsorbed on interior surfaces formed by a pore labyrinth within amorphous carbons. The data show that: (1) the adsorption/desorption times are controlled by choke points that restrict the movement of noble gas atoms within the pore labyrinth, and (2) the physical adsorption controls the temperature behavior and elemental fractionation patterns.

Solubility of noble gases in serpentine - Implications for meteoritic noble gas abundances

NASA Technical Reports Server (NTRS)

Zaikowski, A.; Schaeffer, O. A.

1979-01-01

An investigation of the solubilities of the noble gases from synthesis and solubility studies of the sheet silicate mineral serpentine in carbonaceous chondrites is presented. Hydrothermal synthesis and exchange experiments were made at 340C and 1 kbar with noble gas partial pressures from 2 times 10 to the -8th power to 0.1 atm. The measured distribution coefficients for noble gases are not sufficiently high to account for the trapped noble gases in carbonaceous chondrites by exchange in solar nebula if meteoritic minerals have comparable distribution coefficients. Also, serpentine gains and loses noble gases to approach equilibrium values with the terrestrial atmosphere, indicating that this exposure may have influenced the noble gas abundances in phyllosilicate minerals of these chondrites. The dispersion of K-Ar ages of carbonaceous chondrites could be the result of phyllosilicates approaching equilibrium solubility of atmospheric Ar-40.

Reactor experiments to study luminescence of He-Ne and He-Kr gaseous mixtures, excited by the products of 6Li (n, α) 3H nuclear reaction

NASA Astrophysics Data System (ADS)

Batyrbekov, E. G.; Gordienko, Yu. N.; Barsukov, N. I.; Ponkratov, Yu. V.; Kulsartov, T. V.; Khassenov, M. U.; Zaurbekova, Zh. A.; Tulubayev, Ye. Y.; Samarkhanov, K. K.

2018-04-01

The spectral studies of optical radiation of gaseous mixtures are of interest for solving problems associated with finding gaseous media with high energy conversion efficiency of nuclear reactions into the energy of laser or spontaneous emission [1, 2]. Such media can be used to extract energy from nuclear and fusion reactors in the form of optical radiation, and also to control and adjust the nuclear reactors parameters. This paper presents the preliminary results of the reactor experiments to study the spectral-luminescent properties of gas mixtures (based on He, Ne and Kr noble gases) excited by the products of 6Li(n,α)3H nuclear reaction at different levels of the stationary power of the IVG.1M reactor.

Mantle Noble Gas Contents Controlled by Serpentinite Subduction

NASA Astrophysics Data System (ADS)

Krantz, J. A.; Parman, S. W.; Kelley, S. P.; Smye, A.; Jackson, C.; Cooper, R. F.

2017-12-01

Noble gases serve as powerful tracers of the mantle's chemical and physical evolution. Analyses of material from subduction zones1, mid-ocean ridge basalts, and ocean island basalts2 indicate that heavy noble gases are being recycled from the surface of the earth into the mantle. The exact mechanism by which these uncharged atoms can be bound to a mineral and the subsequent path of recycling remains unclear, but experimental work suggests that ring structures in silicate minerals are ideal sites for noble gases3. Serpentine contains such ring structures and is abundant in subducting slabs. Developing an understanding of how noble gases are transported sheds light on the large-scale mantle dynamics associated with volatile transport, subduction, convection, and mantle heterogeneity. The solubilities of He, Ne, Ar, Kr, and Xe have been experimentally determined in natural samples of antigorite, the high-pressure polymorph of serpentine. The measured solubilities for all noble gases are high relative to mantle silicates (olivine and pyroxenes)4,5. Mixing lines between the noble gas contents of seawater and serpentinite may explain the noble gas composition of mid-ocean ridge basalts and constrain the source material of EM1, EM2 and HIMU ocean island basalts. 1. Kendrick, M.A. et al., Nature Geoscience, 4, 807-812, 2011 2. Parai, R. and Mukhopadhyay, S., GGG, 16, 719-735, 2015 3. Jackson, C.R.M. et al., GCA, 159, 1-15, 2015 4. Heber, V.S. et al., GCA, 71, 1041-1061, 2007 5. Jackson, C.R.M. et al., EPSL, 384, 178-187, 2013

Noble gases solubility models of hydrocarbon charge mechanism in the Sleipner Vest gas field

NASA Astrophysics Data System (ADS)

Barry, P. H.; Lawson, M.; Meurer, W. P.; Warr, O.; Mabry, J. C.; Byrne, D. J.; Ballentine, C. J.

2016-12-01

Noble gases are chemically inert and variably soluble in crustal fluids. They are primarily introduced into hydrocarbon reservoirs through exchange with formation waters, and can be used to assess migration pathways and mechanisms, as well as reservoir storage conditions. Of particular interest is the role groundwater plays in hydrocarbon transport, which is reflected in hydrocarbon-water volume ratios. Here, we present compositional, stable isotope and noble gas isotope and abundance data from the Sleipner Vest field, in the Norwegian North Sea. Sleipner Vest gases are generated from primary cracking of kerogen and the thermal cracking of oil. Gas was emplaced into the Sleipner Vest from the south and subsequently migrated to the east, filling and spilling into the Sleipner Ost fields. Gases principally consist of hydrocarbons (83-93%), CO2 (5.4-15.3%) and N2 (0.6-0.9%), as well as trace concentrations of noble gases. Helium isotopes (3He/4He) are predominantly radiogenic and range from 0.065 to 0.116 RA; reported relative to air (RA = 1.4 × 10-6; Clarke et al., 1976; Sano et al., 1988), showing predominantly (>98%) crustal contributions, consistent with Ne (20Ne/22Ne from 9.70 to 9.91; 21Ne/22Ne from 0.0290 to 0.0344) and Ar isotopes (40Ar/36Ar from 315 to 489). Air-derived noble gas isotopes (20Ne, 36Ar, 84Kr, 132Xe) are introduced into the hydrocarbon system by direct exchange with air-saturated water (ASW). The distribution of air-derived noble gas species are controlled by phase partitioning processes; in that they preferentially partition into the gas (i.e., methane) phase, due to their low solubilities in fluids. Therefore, the extent of exchange between hydrocarbon phases and formation waters - that have previously equilibrated with the atmosphere - can be determined by investigating air-derived noble gas species. We utilize both elemental ratios to address process (i.e., open vs. closed system) and concentrations to quantify the extent of hydrocarbon

Noble gases in SNC meteorites: Shergotty, Nakhla, Chassigny

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ott, U.

1988-07-01

The author reports the elemental and isotopic composition of the noble gases in various fragments of the Shergotty, Nakhla, and Chassigny meteorites. Conclusions presented earlier which were based on results for trapped Ar, Kr and Xe only, are reaffirmed by the complete set of data. Arguments are presented that Chassigny-type gases are a better choice than (fractionated) terrestrial air for the second component, that, when mixed with SPB-gases produces the Shergotty composition. The ratios {sup 40}Ar/{sup 36}Ar{sub t} and {sup 40}Ar/{sup 129}Xe* in Shergotty agree with the respective values for EETA 79001 glass. This is taken as evidence for amore » late introduction of the supposedly shock implanted atmospheric component into Shergotty; it is at odds with scenarios that introduce the atmospheric component {approximately}180 m.y. ago. Based on the variable ratio {sup 40}Ar/{sup 129}Xe* and its unshocked nature, Nakhla acquired its excess {sup 129}Xe by a different process. {sup 21}Ne-based cosmic-ray exposure ages agree well with values in the literature, but do not readily agree with the younger ages based on the abundance of cosmogenic {sup 126}Xe. Neutron capture products are present in Nakhla Kr and there is evidence for a fission-like component in Xe of both Shergotty and Nakhla. GCR interactions with the SPB are unlikely to be the reason for the low {sup 36}Ar/{sup 38}Ar ratio in SPB-Ar.« less

Angular correlation studies in noble gases

NASA Technical Reports Server (NTRS)

Coleman, P. G.

1990-01-01

There has been a recent revival of interest in the measurement of angular correlation of annihilation photons from the decay of positrons and positronium in gases. This revival has been stimulated by the possibility offered by the technique to shed new light on the apparently low positronium formation fraction in the heavier noble gases and to provide information on positronium quenching processes in gases such as oxygen. There is also the potential for learning about positronium slowing down in gases. This review focuses on experimental noble gas work and considers what new information has been, and may be, gained from these studies.

Interatomic potentials for HeAr, HeKr, and HeXe from multiproperty fits

DOE Office of Scientific and Technical Information (OSTI.GOV)

Danielson, L.J.; Keil, M.

1988-01-15

Crossed molecular beam measurements of differential cross sections (DCS) are reported for elastic scattering of He by Ar, Kr, and Xe at high resolution. Interatomic potentials are determined by simultaneously fitting the DCS's, as well as mixture viscosity and interaction second virial data. Bias due to systematic and potential model errors are examined and are used to estimate the accuracy of the potential energy curves obtained. Attractive well depths are 2.59, 2.67, and 2.64 meV +- 3% for HeAr, HeKr, and HeXe, respectively, agreeing with the best available HeAr potential and a previously proposed HeKr potential, but significantly deeper thanmore » previously reported potentials for HeXe. The HeXe attractive well is also considerably broader than previously reported. Attractive minimum positions are 3.48, 3.70, and 4.00 A ( +- 0.03 A) for HeAr, HeKr, and HeXe, respectively. Including the accurate diffusion data of Dunlop and co-workers (Physica A 95, 561 (1979)) and the absolute integral cross sections of Pirani and Vecchiocattivi (J. Chem. Phys. 66, 372 (1977) and revisions thereto) verify the error bounds for all three potentials.« less

Chalcogenide Aerogels as Sorbents for Noble Gases (Xe, Kr)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Subrahmanyam, Kota S.; Spanopoulos, Ioannis; Chun, Jaehun

High surface MoSx and SbSx chalcogels were studied for Xe/Kr gas separation. The intrinsic soft character of the chalcogel framework is a unique property among the large family of porous materials and offers a potential new approach towards the selective separation of Xe over Kr. Among these chalcogels, MoSx shows the highest Xe and Kr uptake, reaching 0.69 mmol g-1 (1.05 mmol cm-3) and 0.28 mmol g-1 (0.42 mmol cm-3) respectively, at 273 K and 1 bar. The corresponding isosteric heat of adsorption at zero coverage (Qst0) is 22.8 and 18.6 kJ mol-1 and both are the highest among themore » selected chalcogels. The IAST (10:90) Xe/Kr selectivity at 273 K for MoSx is 6.0 while for SbSx chalcogels varies in the range 2.0-2.8. The higher formal charge of molybdenum, Mo4+, in MoSx versus that of antimony, Sb3+, in SbSx coupled with its larger atomic size could induce higher polarizability in the MoSx framework and therefore higher Xe/Kr selectivity.« less

Noble gas isotopic composition, cosmic ray exposure history, and terrestrial age of the meteorite Allan Hills A81005 from the moon

NASA Astrophysics Data System (ADS)

Eugster, O.; Geiss, J.; Kraehenbuehl, U.; Niedermann, S.

1986-06-01

A comprehensive study of the elemental and isotopic abundances of the noble gases He, Ne, Ar, Kr, and Xe in the meteorite Allan Hills A81005 from the moon is presented. In addition to a bulk sample, five grain-size fractions were analyzed. Chemical abundances relevant to the interpretation of the cosmic-ray-produced noble gases were determined and indicate that the grain size fractions are chemically uniform. Except for the fact that the trapped noble gas concentrations appear to be grain size correlated, the isotopic and elemental pattern of the trapped solar wind noble gases in A81005 are very similar to those observed in lunar soils and breccias. The A81005 material resided during (580 + or - 180) Myr in the nuclear active zone of the lunar regolith at an average shielding depth of about 40 g/sq cm. From literature data, it is concluded that the moon-earth transit time lasted less than a few million years. Finally, A81005 was captured by the earth more than 140,000 years ago, as indicated by the abundance of cosmic-ray-produced Kr-81.

Closed System Step Etching of CI chondrite Ivuna reveals primordial noble gases in the HF-solubles

NASA Astrophysics Data System (ADS)

Riebe, My E. I.; Busemann, Henner; Wieler, Rainer; Maden, Colin

2017-05-01

We analyzed all the noble gases in HF-soluble phases in the CI chondrite Ivuna by in-vacuum gas release using the "Closed System Step Etching" (CSSE) technique, which allows for direct noble gas measurements of acid-soluble phases. The main motivation was to investigate if there are primordial noble gases in HF-soluble phases in Ivuna, something that has not been done before in CI chondrites, as most primordial noble gases are known to reside in HF-resistant phases. The first steps under mild etching released He, Ne, and Ar with solar-like elemental and isotopic compositions, confirming that Ivuna contains implanted solar wind (SW) noble gases acquired in the parent body regolith. The SW component released in some etch steps was elementally unfractionated. This is unusual as trapped SW noble gases are elementally fractionated in most meteoritic material. In the intermediate etch steps under slightly harsher etching, cosmogenic noble gases were more prominent than SW noble gases. The HF-soluble portion of Ivuna contained primordial Ne and Xe, that was most visible in the last etch steps after all cosmogenic and most SW gases had been released. The primordial Ne and Xe in the HF-solubles have isotopic and elemental ratios readily explained as a mixture of the two most abundant primordial noble gas components in Ivuna bulk samples: HL and Q. Only small fractions of the total HL and Q in Ivuna were released during CSSE analysis; ∼3% of 20NeHL and ∼4% of 132XeQ. HL is known to reside in nanodiamond-rich separates and Q-gases are most likely carried by a carbonaceous phase known as phase Q. Q-gases were likely released from an HF-soluble portion of phase Q. However, nanodiamonds might not be the source of the HL-gases released upon etching, since nanodiamond-rich separates are very HF-resistant and the less tightly bound nanodiamond component P3 was not detected.

Noble gas systematics of the Skaergaard intrusion

NASA Astrophysics Data System (ADS)

Horton, F.; Farley, K. A.; Taylor, H. P.

2017-12-01

The noble gas isotopic compositions of olivines from the Skaergaard layered mafic intrusion in Greenland reveal that magmas readily exchange noble gases with their environment after emplacement. Although Skaergaard magmas are thought to have derived from the upper mantle, all of the olivine separates we analyzed have 3He/4He ratios less than that of the upper mantle ( 8 Ra, where Ra = 3He/4He of the atmosphere, 1.39 x 10-6). This suggests that crustal and/or atmospheric noble gases have contaminated all Skaergaard magmas to some extent. We obtained the highest 3He/4He ratios ( 2 Ra) from olivines found in the lowermost exposed layers of the intrusion away from the margins. Excess radiogenic 4He (indicated by Ra<1) along the margin of the intrusion indicates that noble gases from the Archean host-rock were incorporated into the cooling magma chamber, probably via magmatic assimilation. Noble gases in olivines from the upper portions of the intrusion have atmospheric isotopic compositions, but higher relative helium abundances than the atmosphere. We suggest that post-crystallization hydrothermal circulation introduced atmosphere-derived noble gases into uppermost layers of the intrusion. Such high temperature exchanges of volatiles between plutons and their immediate surroundings may help explain why so few mantle-derived rocks retain mantle-like noble gas signatures.

Using Heavy Noble Gases to Help Determine Mantle vs Lithospheric Contributions and CO2 Residence Times in Southwestern US Hot Springs

NASA Astrophysics Data System (ADS)

Whyte, C. J.; Karlstrom, K. E.; Crossey, L. J.; Darrah, T.

2017-12-01

Climate change has placed a particular importance on the understanding of carbon cycling, especially on continental scales, resulting in the necessity to quantify the rates and timing on which CO2 is released into the atmosphere by volcanic and tectonic processes. Recent studies have identified mantle-derived 3He and excess CO2 in springs and groundwaters across the conterminous US, suggesting that there may be great unknowns in the rates and scales of magmatic CO2 release in the global carbon budget. Further, it remains uncertain if these fluids are merely passive remnants of past magmatic events or instead result from ongoing mantle degassing. Understanding these processes and timescales by studying CO2 fluxes alone can be challenging because CO2 is highly reactive in the subsurface. CO2 is both formed and degraded by microbial processes, rapidly dissolves into waters, and can be readily released from carbonate-rich lithologies by water-rock interactions. By comparison, chemically-inert tracers such as noble gases provide one potential technique for identifying and constraining fluid sources and migration histories in the subsurface. Primordial isotopes (e.g., 3He and 129Xe) provide unambiguous indications of mantle-derived fluids, and heavier noble gases (e.g., Ne, Ar, Kr, Xe) provide a suite of potential tracers that can help de-convolve the extent of mixing between crust and mantle and discern between lithospheric and asthenospheric mantle fluids. Additionally, the low production rate of the radiogenic xenon isotopes (e.g., 134Xe, 136Xe) may help determine the relative residence time of mantle CO2 degassing in continental settings, providing important constraints on CO2 storage in the mantle and lithosphere in quiescent tectonic settings. To test these hypotheses, we analyzed a suite of noble gas isotopic compositions in hot springs in the Colorado Plateau and Rocky Mountains, US. Many samples display resolvable excesses in 3He and 129Xe relative to air

Determining the source and genetic fingerprint of natural gases using noble gas geochemistry: a northern Appalachian Basin case study

USGS Publications Warehouse

Hunt, Andrew G.; Darrah, Thomas H.; Poreda, Robert J.

2012-01-01

Silurian and Devonian natural gas reservoirs present within New York state represent an example of unconventional gas accumulations within the northern Appalachian Basin. These unconventional energy resources, previously thought to be noneconomically viable, have come into play following advances in drilling (i.e., horizontal drilling) and extraction (i.e., hydraulic fracturing) capabilities. Therefore, efforts to understand these and other domestic and global natural gas reserves have recently increased. The suspicion of fugitive mass migration issues within current Appalachian production fields has catalyzed the need to develop a greater understanding of the genetic grouping (source) and migrational history of natural gases in this area. We introduce new noble gas data in the context of published hydrocarbon carbon (C1,C2+) (13C) data to explore the genesis of thermogenic gases in the Appalachian Basin. This study includes natural gases from two distinct genetic groups: group 1, Upper Devonian (Marcellus shale and Canadaway Group) gases generated in situ, characterized by early mature (13C[C1  C2][13C113C2]: –9), isotopically light methane, with low (4He) (average, 1  103 cc/cc) elevated 4He/40Ar and 21Ne/40Ar (where the asterisk denotes excess radiogenic or nucleogenic production beyond the atmospheric ratio), and a variable, atmospherically (air-saturated–water) derived noble gas component; and group 2, a migratory natural gas that emanated from Lower Ordovician source rocks (i.e., most likely, Middle Ordovician Trenton or Black River group) that is currently hosted primarily in Lower Silurian sands (i.e., Medina or Clinton group) characterized by isotopically heavy, mature methane (13C[C1 – C2] [13C113C2]: 3), with high (4He) (average, 1.85  103 cc/cc) 4He/40Ar and 21Ne/40Ar near crustal production levels and elevated crustal noble gas content (enriched 4He,21Ne, 40Ar). Because the release of each crustal noble gas (i.e., He, Ne, Ar

Methane Sources and Migration Mechanisms in the Shallow Trinity Aquifer in Parker and Hood Counties, Texas - a Noble Gas Analysis

NASA Astrophysics Data System (ADS)

Wen, T.; Castro, C.; Nicot, J. P.; Hall, C. M.; Mickler, P. J.; Darvari, R.

2016-12-01

The presence of elevated methane in groundwaters within the Barnett Shale footprint in Parker and Hood counties, Texas has caused public concern that hydrocarbon production may facilitate migration of natural gas into a critical groundwater resource. This study places constraints on the source of methane in these groundwaters by analyzing water and stray gas data from groundwater wells and gas production wells from both the Barnett Shale and Strawn Group for methane content and noble gases, both of crustal and atmospheric origin. Particular emphasis is given to the atmospheric heavier noble gases 84Kr and 132Xe, which are significantly less affected by the presence of excess air, commonly present in modern Texas groundwaters (e.g., [1]). Dissolved methane concentrations are positively correlated with crustal 4He, 21Ne and 40Ar and suggest that noble gases and methane in these groundwaters originate from a common source, likely the Strawn Group, which the sampled aquifer overlies unconformably. This finding is further supported by the noble gas isotopic signature of stray gas when compared to the gas isotopic signatures of both Barnett Shale and the Strawn Group. In contrast to most samples, four groundwater wells with the highest methane concentrations unequivocally show heavy depletion of the atmospheric noble gases 20Ne, 36Ar, 84Kr and 132Xe with respect to freshwater recharge equilibrated with the atmosphere (ASW). This is consistent with predicted noble gas concentrations in a residual water phase in contact with a gas phase with initial ASW composition at 18°C-25°C, assuming a closed-system and suggest a highly localized gas source. All these four wells, without exception, tap into the Strawn Group and it is likely that shallow gas accumulations, as they are known to exist, were reached. Additionally, lack of correlation between 84Kr/36Ar and 132Xe/36Ar fractionation levels and distance to the nearest production wells does not support the notion that methane

Extraterrestrial Helium (He@C60) Trapped in Fullerenes in the Sudbury Impact Structure

NASA Technical Reports Server (NTRS)

Becker, L.; Bada, J. L.; Poreda, R. J.; Bunch, T. E.

1997-01-01

Fullerenes (C60 and C70) have recently been identified in a shock-produced breccia (Onaping Formation) associated with the 1.85-Ga Sudbury Impact Crater. The presence of parts-per-million levels of fullerenes in this impact structure raises interesting questions about the processes that led to the formation of fullerenes and the potential for delivery of intact organic material to the Earth by a large bolide (e.g., asteroid or comet). Two possible scenarios for the presence of fullerenes in the Sudbury impact deposits are that (1) fullerenes are synthesized within the impact plume from the C contained in the bolide; or (2) fullerenes are already present in the bolide and survived the impact event. The correlation of C and trapped noble gas atoms in meteorites is well established. Primitive meteorites contain several trapped noble gas components that have anomalous isotopic compositions, some of which may have a presolar origin. Several C-bearing phases, including SiC, graphite, and diamond, have been recognized as carriers of trapped noble gases. It has also been suggested that fullerenes (C60 and C70) might be a carrier of noble gas components in carbonaceous chondrites. Recently, fullerenes have been detected in separate samples in the Allende meteorite. Carbon-60 is large enough to enclose the noble gases He, Ne, Ar, Kr, and Xe, but it is too small to contain diatomic gases such as N2 or triatomic gases such as CO2. Recent experimental work has demonstrated that noble gases of a specific isotopic composition can be introduced into synthetic fullerenes at high temperatures and pressures; these encapsulated gases can then be released by the breaking of one or more C bonds during step-heating under vacuum. These thermal-release patterns for He encapsulated within the C60 molecule (He@C60) are similar to the patterns for acid residues of carbonaceous chondrites, suggesting that fullerenes could be an additional carrier of trapped noble gases in acid residues of

Bubble formation, vesicularity and fractionation of noble gases during MORB degassing

NASA Astrophysics Data System (ADS)

Sator, N.; Guillot, B. B.; Aubry, G.

2012-12-01

The fractionation of noble gases in oceanic basalts gives information on the source region and on the transport of volatiles up to the seafloor. For instance, the large distribution (~1-1,000) of the 4He/40Ar* ratio in mid-ocean ridge basalts (MORB), is interpreted as the signature of different degassing scenarios taking place at depth. Thus, a low value of this ratio is explained by a closed system degassing whereas a high value is assigned either to an open system degassing (where vesicles are lost in a magma chamber or at depth during magma ascent) or to a kinetic disequilibrium induced by a rapid magma ascent just prior eruption. Unfortunately, CO2 has a very low solubility in basaltic melts at pressure corresponding to the seafloor and an overwhelming majority of erupted lavas have lost their pristine volatile contents. However notable exceptions are the popping rocks characterized by a large vesicularity, a high CO2 content and a 4He/40Ar* ratio compatible with the expected U/K ratio of the upper mantle. Those samples likely have experienced a CO2 exsolution at about 35 km depth in the oceanic mantle. So, the very existence of these exceptional MORB samples suggests that CO2-rich melts could be present at a greater depth. Thus, explosive eruptions near ocean spreading centers are well documented (Hekinian et al., 2000) and are associated with volcaniclastic deposits containing highly vesicular basalts, a feature which suggests that this volcanism is driven by CO2-rich magmas (Helo et al., 2011). But how much CO2-rich are these magmas, that is the question. The objective of this study is to use molecular dynamics simulation (MD) to evaluate the vesicularity and the fractionation of noble gases in a degassing MORB melt. A previous simulation study (Guillot and Sator, 2011) has shown that the solubility of CO2 in basaltic melts increases steadily with the pressure and deviates significantly from the Henry's law at high pressures. From the CO2 solubility curve

Release of radiogenic noble gases as a new signal of rock deformation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bauer, Stephen J.; Gardner, W. Payton; Lee, Hyunwoo

In this paper we investigate the release of radiogenic noble gas isotopes during mechanical deformation. We developed an analytical system for dynamic mass spectrometry of noble gas composition and helium release rate of gas produced during mechanical deformation of rocks. Our results indicate that rocks release accumulated radiogenic helium and argon from mineral grains as they undergo deformation. We found that the release of accumulated 4He and 40Ar from rocks follows a reproducible pattern and can provide insight into the deformation process. Increased gas release can be observed before dilation, and macroscopic failure is observed during high-pressure triaxial rock deformationmore » experiments. Accumulated radiogenic noble gases can be released due to fracturing of mineral grains during small-scale strain in Earth materials. Helium and argon are highly mobile, conservative species and could be used to provide information on changes in the state of stress and strain in Earth materials, and as an early warning signal of macroscopic failure. These results pave the way for the use of noble gases to trace and monitor rock deformation for earthquake prediction and a variety of other subsurface engineering projects.« less

Release of radiogenic noble gases as a new signal of rock deformation

DOE PAGES

Bauer, Stephen J.; Gardner, W. Payton; Lee, Hyunwoo

2016-10-09

In this paper we investigate the release of radiogenic noble gas isotopes during mechanical deformation. We developed an analytical system for dynamic mass spectrometry of noble gas composition and helium release rate of gas produced during mechanical deformation of rocks. Our results indicate that rocks release accumulated radiogenic helium and argon from mineral grains as they undergo deformation. We found that the release of accumulated 4He and 40Ar from rocks follows a reproducible pattern and can provide insight into the deformation process. Increased gas release can be observed before dilation, and macroscopic failure is observed during high-pressure triaxial rock deformationmore » experiments. Accumulated radiogenic noble gases can be released due to fracturing of mineral grains during small-scale strain in Earth materials. Helium and argon are highly mobile, conservative species and could be used to provide information on changes in the state of stress and strain in Earth materials, and as an early warning signal of macroscopic failure. These results pave the way for the use of noble gases to trace and monitor rock deformation for earthquake prediction and a variety of other subsurface engineering projects.« less

Solar Noble Gases in Polymict Ureilites and an Update on Ureilite Noble Gas Data

NASA Astrophysics Data System (ADS)

Ott, U.; Lohr, H. P.; Begemann, F.

1993-07-01

Ureilites are one of the least understood classes of meteorites; they show signs of being processed, but also appear to be primitive, with abundant carbon and trapped noble gases [1-6]. We have now begun to analyze a number of recently recovered specimens: one from the Saharan desert (Acfer 277) amd five from the Antarctic (LEW 85328, LEW 85440, EET 87720, FRO 90036, and FRO 90054). Analyses of Acfer 277, LEW 85328, and EET 87720 are complete (Table 1). Solar noble gases are present in polymict EET 87720, as shown by the three- isotope plot of Fig. 1. There, in contrast to the bulk data point for Acfer 277, data points for EET 87720 deviate from a mixing line between "typical" spallation Ne (as approximated here by the spallation-dominated 1800 degrees C step for EET 87720) and Ne-U [7] toward higher ^20Ne/^22Ne. A line fitted to the EET 87720 data points passes slightly below Ne-B [8]. The situation is similar for sample F1 from polymict EET 83309 [9], which is shown for comparison. Additional support for the presence of solar gases arises from the abundance of ^4He (~9 x 10^-5 cm^3 STP/g in EET 87720-F1, corrected for spallogenic contributions), which in both cases is far higher than in other ureilite bulk samples [6,10]. Also, in the ratio of spallation-corrected ^4He to trapped ^36Ar, these two polymict ureilites clearly stand out. Helium-4/argon-36 ratios in EET 87720-F1 and EET 83309-F1 are ~20 and ~28 respectively, at least 1 order of magnitude higher than in bulk monomict ureilites and 2 orders of magnitude higher than what appears typical of ureilite diamonds [6]. Nilpena, another polymict ureilite [11], also has a ^4He/^36Ar ratio (2.1 in Nilpena II-1 [7]) higher than all monomict ureilites but one (Dingo Pup Donga), indicating the presence of solar noble gases (in variable contents) as a possible general feature of polymict ureilites, similar to the presence in them of nitrogen with high delta(^15N/^14N) [12]. Monomict LEW 85328 has a very high (^22Ne

Isotopic Composition of Trapped and Cosmogenic Noble Gases in Several Martian Meteorites

NASA Technical Reports Server (NTRS)

Garrison, Daniel H.; Bogard, Donald D.

1997-01-01

Isotopic abundances of the noble gases were measured in the following Martian meteorites: two shock glass inclusions from EET79001, shock vein glass from Shergotty and Y793605, and whole rock samples of ALH84001 and QUE94201. These glass samples, when combined with literature data on a separate single glass inclusion from EET79001 and a glass vein from Zagami, permit examination of the isotopic composition of Ne, Ar, Kr, and Xe trapped from the Martian atmosphere in greater detail. The isotopic composition of Martian Ne, if actually present in these glasses, remains poorly defined. The Ar-40/Ar-36 ratio of Martian atmospheric Ar may be much less than the ratio measured by Viking and possibly as low as approx. 1900. The atmospheric Ar-36/Ar-38 ratio is less than or equal to 4.0. Martian atmospheric Kr appears to be enriched in lighter isotopes by approx. 0.4%/amu compared to both solar wind Kr and to the Martian composition previously reported. The Martian atmospheric Ar-36/Xe-132 and Kr-84/Xe-132 Xe elemental ratios are higher than those reported by Viking by factors of approx. 3.3 and approx. 2.5, respectively. Cosmogenic gases indicate space exposure ages of 13.9 +/- 1 Myr for ALH84001 and 2.7 +/- 0.6 Myr for QUE94201. Small amounts of Ne-21 produced by energetic solar protons may be present in QUE94201, but are not present in ALH84001 or Y793605. The space exposure age for Y793605 is 4.9 +/- 0.6 Myr and appears to be distinctly older than the ages for basaltic shergottites.

Noble gases recycled into the mantle through cold subduction zones

NASA Astrophysics Data System (ADS)

Smye, Andrew J.; Jackson, Colin R. M.; Konrad-Schmolke, Matthias; Hesse, Marc A.; Parman, Steve W.; Shuster, David L.; Ballentine, Chris J.

2017-08-01

Subduction of hydrous and carbonated oceanic lithosphere replenishes the mantle volatile inventory. Substantial uncertainties exist on the magnitudes of the recycled volatile fluxes and it is unclear whether Earth surface reservoirs are undergoing net-loss or net-gain of H2O and CO2. Here, we use noble gases as tracers for deep volatile cycling. Specifically, we construct and apply a kinetic model to estimate the effect of subduction zone metamorphism on the elemental composition of noble gases in amphibole - a common constituent of altered oceanic crust. We show that progressive dehydration of the slab leads to the extraction of noble gases, linking noble gas recycling to H2O. Noble gases are strongly fractionated within hot subduction zones, whereas minimal fractionation occurs along colder subduction geotherms. In the context of our modelling, this implies that the mantle heavy noble gas inventory is dominated by the injection of noble gases through cold subduction zones. For cold subduction zones, we estimate a present-day bulk recycling efficiency, past the depth of amphibole breakdown, of 5-35% and 60-80% for 36Ar and H2O bound within oceanic crust, respectively. Given that hotter subduction dominates over geologic history, this result highlights the importance of cooler subduction zones in regassing the mantle and in affecting the modern volatile budget of Earth's interior.

Recycling of volatiles at subduction zones: Noble gas evidence from the Tabar-Lihir-Tanga-Feni arc of papua New Guinea

NASA Technical Reports Server (NTRS)

Farley, Kenneth; Mcinnes, Brent; Patterson, Desmond

1994-01-01

Convergent margin processes play an important but poorly understood role in the distribution of terrestrial volatile species. For example, subduction processes filter volatiles from the subducting package, thereby restricting their return to the mantle. In addition, once extracted from the downgoing slab, volatiles become an essential component in the petrogenesis of island arc magmas. The noble gases, with their systematic variation in physical properties and diversity of radiogenic isotopes, should carry a uniquely valuable record of these processes. However, thus far studies of noble gases in arc volcanics have achieved only limited success in this regard. Subduction-related lavas and geothermal fluids carry (3)He/(4)He ratios equal to or slightly lower than those found in the depleted upper mantle source of mid-ocean ridge basalts. Apparently slab-derived helium (which should have (3)He/(4)He much less than MORB) is extensively diluted by MORB-like helium from the mantle wedge, making it difficult to use helium as a tracer of convergent margin processes. Interpretation of the heavier noble gases (Ne-Ar-Kr-Xe) in arc lavas has also proven difficult, because the lavas carry low noble gas concentrations and hence are subject to pervasive atmospheric contamination. The low noble gas concentrations may be a consequence of degassing in the high level magma chambers characteristic of arc stratovolcanos. We have recently initiated a project to better constrain the behavior of volatiles in subduction zones through geochemical studies of the tectonically unusual volcanoes of the Tabar-Lihir-Tanga-Feni (TLTF) arc in the Bismarck Archipelago, Papua New Guinea.

Noble Gas Recycling: Experimental Constraints on Ar, Kr, and Xe Solubility in Serpentinite

NASA Astrophysics Data System (ADS)

Krantz, J. A.; Parman, S. W.; Kelley, S. P.; Smye, A.; Jackson, C.; Cooper, R. F.

2016-12-01

To constrain the rate of noble gas (NG) recycling at subduction zones, experiments have been performed to constrain the solubility of NG in natural antigorite. Geochemical analyses of exhumed subduction zone material1, well gases2, OIB and MORB3 indicate that NG are recycled from the surface of the earth into the mantle. The mechanism by which uncharged atoms can be bound to a mineral and subsequently recycled remains unclear, but experimental work suggests that ring structures in silicate minerals are ideal sites for NG4. Serpentine contains such ring structures and is abundant in subducting slabs, providing significant potential for control of the recycling of NG. Developing an understanding of how NG are transported may shed light on the large scale mantle dynamics associated with subduction, convection, and mantle heterogeneity. Experiments were performed in a cold seal pressure vessel at 350°C using a mix of either equal parts He, Ne, and Ar or Ar, Kr, and Xe as the pressure medium. Pressures varied from 0.15 to 1.13 kbar total pressure and durations varied from 20 to 188 hours. Samples were analyzed by UV laser ablation, noble gas mass spectrometry at The Open University, UK. White light interferometry was used to determine the volume of laser ablation pits from which concentrations were calculated. The data indicate that solubilities of NG in serpentinite are high in antigorite, and that variations in the solubility of NG could fractionate NG during recycling. 1. Kendrick, M.A., Scambelluri, M., Honda, M., Phillips, D., Nature Geoscience, 4, 807-812, 2011 2. Holland, G., and Ballentine, C.J., Nature, 441, 186-191, 2006 3. Parai, R. and Mukhopadhyay, S., GGG, 16, 719-735, 2015 4. Jackson, C.R.M., Parman, S.W., Kelley, S.P., Cooper, R.F., GCA, 159, 1-15, 2015

The diverse biological properties of the chemically inert noble gases.

PubMed

Winkler, David A; Thornton, Aaron; Farjot, Géraldine; Katz, Ira

2016-04-01

The noble gases represent an intriguing scientific paradox. They are extremely inert chemically but display a remarkable spectrum of clinically useful biological properties. Despite a relative paucity of knowledge of their mechanisms of action, some of the noble gases have been used successfully in the clinic. Studies with xenon have suggested that the noble gases as a class may exhibit valuable biological properties such as anaesthesia; amelioration of ischemic damage; tissue protection prior to transplantation; analgesic properties; and a potentially wide range of other clinically useful effects. Xenon has been shown to be safe in humans, and has useful pharmacokinetic properties such as rapid onset, fast wash out etc. The main limitations in wider use are that: many of the fundamental biochemical studies are still lacking; the lighter noble gases are likely to manifest their properties only under hyperbaric conditions, impractical in surgery; and administration of xenon using convectional gaseous anaesthesia equipment is inefficient, making its use very expensive. There is nonetheless a significant body of published literature on the biochemical, pharmacological, and clinical properties of noble gases but no comprehensive reviews exist that summarize their properties and the existing knowledge of their models of action at the molecular (atomic) level. This review provides such an up-to-date summary of the extensive, useful biological properties of noble gases as drugs and prospects for wider application of these atoms. Crown Copyright © 2016. Published by Elsevier Inc. All rights reserved.

On the size and structure of helium snowballs formed around charged atoms and clusters of noble gases.

PubMed

Bartl, Peter; Leidlmair, Christian; Denifl, Stephan; Scheier, Paul; Echt, Olof

2014-09-18

Helium nanodroplets doped with argon, krypton, or xenon are ionized by electrons and analyzed in a mass spectrometer. HenNgx(+) ions containing up to seven noble gas (Ng) atoms and dozens of helium atoms are identified; the high resolution of the mass spectrometer combined with advanced data analysis make it possible to unscramble contributions from isotopologues that have the same nominal mass but different numbers of helium or Ng atoms, such as the magic He20(84)Kr2(+) and the isobaric, nonmagic He41(84)Kr(+). Anomalies in these ion abundances reveal particularly stable ions; several intriguing patterns emerge. Perhaps most astounding are the results for HenAr(+), which show evidence for three distinct, solid-like solvation shells containing 12, 20, and 12 helium atoms. This observation runs counter to the common notion that only the first solvation shell is solid-like but agrees with calculations by Galli et al. for HenNa(+) [J. Phys. Chem. A 2011, 115, 7300] that reveal three shells of icosahedral symmetry. HenArx(+) (2 ≤ x ≤ 7) ions appear to be especially stable if they contain a total of n + x = 19 atoms. A sequence of anomalies in the abundance distribution of HenKrx(+) suggests that rings of six helium atoms are inserted into the solvation shell each time a krypton atom is added to the ionic core, from Kr(+) to Kr3(+). Previously reported strong anomalies at He12Kr2(+) and He12Kr3(+) [Kim , J. H.; et al. J. Chem. Phys. 2006, 124, 214301] are attributed to a contamination. Only minor local anomalies appear in the distributions of HenXex(+) (x ≤ 3). The distributions of HenKr(+) and HenXe(+) show strikingly similar, broad features that are absent from the distribution of HenAr(+); differences are tentatively ascribed to the very different fragmentation dynamics of these ions.

On the Size and Structure of Helium Snowballs Formed around Charged Atoms and Clusters of Noble Gases

PubMed Central

2013-01-01

Helium nanodroplets doped with argon, krypton, or xenon are ionized by electrons and analyzed in a mass spectrometer. HenNgx+ ions containing up to seven noble gas (Ng) atoms and dozens of helium atoms are identified; the high resolution of the mass spectrometer combined with advanced data analysis make it possible to unscramble contributions from isotopologues that have the same nominal mass but different numbers of helium or Ng atoms, such as the magic He2084Kr2+ and the isobaric, nonmagic He4184Kr+. Anomalies in these ion abundances reveal particularly stable ions; several intriguing patterns emerge. Perhaps most astounding are the results for HenAr+, which show evidence for three distinct, solid-like solvation shells containing 12, 20, and 12 helium atoms. This observation runs counter to the common notion that only the first solvation shell is solid-like but agrees with calculations by Galli et al. for HenNa+ [J. Phys. Chem. A2011, 115, 730021568337] that reveal three shells of icosahedral symmetry. HenArx+ (2 ≤ x ≤ 7) ions appear to be especially stable if they contain a total of n + x = 19 atoms. A sequence of anomalies in the abundance distribution of HenKrx+ suggests that rings of six helium atoms are inserted into the solvation shell each time a krypton atom is added to the ionic core, from Kr+ to Kr3+. Previously reported strong anomalies at He12Kr2+ and He12Kr3+ [KimJ. H.; et al. J. Chem. Phys.2006, 124, 21430116774401] are attributed to a contamination. Only minor local anomalies appear in the distributions of HenXex+ (x ≤ 3). The distributions of HenKr+ and HenXe+ show strikingly similar, broad features that are absent from the distribution of HenAr+; differences are tentatively ascribed to the very different fragmentation dynamics of these ions. PMID:24128371

Trapping of Noble Gases by Radiative Association with H3 + in the Protosolar Nebula

NASA Astrophysics Data System (ADS)

Pauzat, F.; Bacchus-Montabonel, M.-C.; Ellinger, Y.; Mousis, O.

2016-04-01

The heavy noble gas deficiencies observed in Titan’s atmosphere and in comets have been proposed to be related to a sequestration process by {{{H}}}3+ in the gas phase at the early protosolar nebula. Chemical thermodynamics and astrophysics modeling are favorable to this hypothesis, as presented in preceding papers. However, there is a point still to be raised, I.e., that no dynamical study of the efficiency of the collisional processes had been performed so far. Here, we show that, apart from the expected exception of Ne, the rate constants obtained, I.e., 0.7 × 10-18, 0.5 × 10-16, and 10-16 (cm3 s-1) for Ar, Kr, and Xe, respectively, are reasonably high for such processes, particularly in the case of Kr and Xe. The temperature dependence is also considered, showing a similar behavior for all noble gases with a peak efficiency in the range 50-60 K. Globally, we can conclude that the scenario of sequestration by {{{H}}}3+ is definitively comforted by the results of our quantum dynamical treatment. This process may also be responsible of the Ar impoverishment just measured in comet 67P/Churyumov-Gerasimenko by the ROSINA mass spectrometer on board the Rosetta spacecraft.

Mantle Noble Gas Contents Controlled by Subduction of Serpentinite

NASA Astrophysics Data System (ADS)

Krantz, J. A.; Parman, S. W.; Kelley, S. P.; Smye, A.; Jackson, C.

2017-12-01

Geochemical analyses of exhumed subduction zone material1, well gases2, MORB, and OIBs3 indicate that noble gases are being recycled from the surface of the earth into the mantle. However, the path taken by these noble gases is unclear. To estimate the distribution and quantity of Ar, Kr, and Xe in subducting slabs, a model consisting of layers of sediments, altered oceanic crust (AOC), and serpentinite (hydrously altered mantle) has been developed. The noble gas contents of sediments and AOC were calculated using the least air-like and most gas-rich analyses from natural systems4,5, while serpentinite was modelled using both data from natural systems1 and experimentally determined solubilities. Layer thicknesses were assessed over a range of values: 1 to 12 km of sediments, 5 to 9 km of AOC, and 1 to 30 km of serpentinite. In all cases, the serpentinite layer contains at least an order of magnitude more Ar and Kr than the other layers. For realistic layer thicknesses (1 km of sediments, 6 km of AOC, and 3 km of serpentinite), Xe is distributed roughly equally between the three layers. By incorporating global subduction rates6, fluxes of the heavy noble gases into the mantle have been calculated as 4 · 1012 mol/Ma for 36Ar, 6 · 1011 mol/Ma for 84Kr, and 8 · 109 mol/Ma for 130Xe. These fluxes are equivalent to the total 84Kr and 130Xe contents of the depleted and bulk mantle over 1 and 10 Ma7. Similarly, the flux of 36Ar is equivalent over 1 and 100 Ma. Since the Kr and Xe have not been completely overprinted by recycling, the large majority of subducted noble gases must escape in the subduction zone. However, even the small amounts that are subducted deeper have affected the mantle as measured in both MORB and OIBs. 1. Kendrick, M.A. et al., Nature Geoscience, 4, 807-812, 2011 2. Holland, G. and Ballentine, C.J., Nature, 441, 186-191, 2006 3. Parai, R. and Mukhopadhyay, S., G3, 16, 719-735, 2015 4. Matsuda, J. and Nagao, K., Geochemical Journal, 20, 71-80, 1986

The Noble Gases in A-Level Chemistry.

ERIC Educational Resources Information Center

Marchant, G. W.

1983-01-01

Suggests two methods of developing the study of the noble gases: first, the discovery of the elements and recent discovery of xenon show the human face of chemistry (historical development); second, the properties of noble gas compounds (particularly xenon) can be used to test the framework of conventional chemistry. (Author/JM)

Noble Gases in the Lunar Meteorites Calcalong Creek and QUE 93069

NASA Astrophysics Data System (ADS)

Swindle, T. D.; Burkland, M. K.; Grier, J. A.

1995-09-01

Although the world's collections contain comparable numbers of martian and lunar meteorites (about 10 each), their ejection histories seem to be quite different [1]. We have sampled no more than four martian craters, but almost every one of the lunar meteorites apparently represents a separate cratering event. Furthermore, most lunar meteorites were apparently ejected from the top meter of the surface, unlike any of the martian meteorites. We have measured noble gases in two bulk samples of the lunar meteorite QUE93069 and three of Calcalong Creek, ranging in size from 7 to 15 mg. Averaged results are given in Table 1. Both meteorites contain solar-wind-implanted noble gas. QUE 93069, which is a mature anorthositic regolith breccia [2], contains amounts comparable to the most gas-rich lunar meteorites. The relatively low 40Ar/36Ar ratios of both meteorites suggest surface exposures no more than 2.5 Ga ago [3]. Calcalong Creek has readily observable spallogenic gas. The 131Xe/126Xe ratio of 4.8+/-0.3 corresponds to an average shielding depth of slightly more than 40 gm/cm^2 [4]. In common with many lunar breccias, Calcalong Creek has been exposed to cosmic rays for several hundred Ma (calculations based on [4] and [5]). The 3He apparent exposure age is much shorter, suggesting diffusive loss of He. To determine the detailed exposure history, it is necessary to have measurements of cosmogenic radionuclides. Our samples were too small to measure 81Kr, but [6] have measured 10Be, 26Al and 36Cl. Their data are consistent with either extended exposure at <70 gm/cm^2 in the lunar regolith followed by a short (200,000 years) transit to Earth, or with ejection from several meters depth about 2 Ma ago [6]. Our data, requiring several hundred Ma of exposure at an average depth of 40-50 gm/cm^2, are clearly more consistent with the first scenario. The only other lunar meteorite which could have been ejected at the same time is MAC 88104/5 [1], but the chemical differences

Petrography, classification, oxygen isotopes, noble gases, and cosmogenic records of Kamargaon (L6) meteorite: The latest fall in India

NASA Astrophysics Data System (ADS)

Ray, D.; Mahajan, R. R.; Shukla, A. D.; Goswami, T. K.; Chakraborty, S.

2017-08-01

A single piece of meteorite fell on Kamargaon village in the state of Assam in India on November 13, 2015. Based on mineralogical, chemical, and oxygen isotope data, Kamargaon is classified as an L-chondrite. Homogeneous olivine (Fa: 25 ± 0.7) and low-Ca pyroxene (Fs: 21 ± 0.4) compositions with percent mean deviation of <2, further suggest that Kamargaon is a coarsely equilibrated, petrologic type 6 chondrite. Kamargaon is thermally metamorphosed with an estimated peak metamorphic temperature of 800 °C as determined by two-pyroxene thermometry. Shock metamorphism studies suggest that this meteorite include portions of different shock stages, e.g., S3 and S4 (Stöffler et al.; however, local presence of quenched metal-sulfide melt within shock veins/pockets suggest disequilibrium melting and relatively higher shock stage of up to S5 (Bennett and McSween). Based on noble gas isotopes, the cosmic-ray exposure age is estimated as 7.03 ± 1.60 Ma and nitrogen isotope composition (δ15N = 18‰) also correspond well with the L-chondrite group. The He-U, Th, and K-Ar yield younger ages (170 ± 25 Ma 684 ± 93, respectively) and are discordant. A loss of He during the resetting event is implied by the lower He-U and Th age. Elemental ratios of trapped Ar, Kr, and Xe can be explained through the presence of a normal Q noble gas component. Relatively low activity of 26Al (39 dpm/kg) and the absence of 60Co activity suggest a likely low shielding depth and envisage a small preatmospheric size of the meteoroid (<10 cm in radius). The Kr isotopic ratios (82Kr/84Kr) further argue that the meteorite was derived from a shallow depth.

Noble Gases in Alpine Gold: U/Th-He Dating and Excesses of Radiogenic He and AR

NASA Astrophysics Data System (ADS)

Eugster, O.; Hofmann, B.; Krahenbuhl, U.; Neuenschwander, J.

1992-07-01

quantity of trapped atmospheric noble gases we estimate atmospheric ^4He in the gold samples to be three to five orders of magnitude below the observed ^4He concentration. Placer gold is finely distributed in rock material and might be exposed to an alpha-particle irradiation from neighboring U/Th-rich minerals. An alternative He source are inclusions of U/Th-rich minerals, such as zircon, either within the gold material or mechanically worked into the spangles as they were part of the river detritus. Acknowledgement: We thank the Swiss NSF for their support. References: Diamond L.W. (1990) Am. J. of Science 290, 912-958. Schmid K. (1973) Schw. Min. Petr. Mitt. 53, 125-156. Table 1, which in the hard copy appears here, shows concentrations of He, Ne, and Ar (10^-8 cm^3 STP/g) and of K, Th, and U (ppm) in vein-type free gold, placer gold, and quartz. The ^3He and ^21Ne signals were below detection limits, that is ^4He/^3He in gold is >100'000. Average ^20Ne/^22Ne ratios in gold and quartz are 10.2 +- 0.2, that is about 4% larger than in the terrestrial atmosphere. Average ^36Ar/^38Ar = 5.2 +- 0.2 (within errors identical to ^36Ar/^38Ar in air). 1) Sample sizes 50-100 mg. 2) Radiogenic ^40Ar = ^40Ar-295.5 x ^36Ar. 3) Calculated from U/Th and ^40K decay.

Noble gases in twenty Yamato H-chondrites: Comparison with Allan Hills chondrites and modern falls

NASA Technical Reports Server (NTRS)

Loeken, TH.; Scherer, P.; Schultz, L.

1993-01-01

Concentration and isotopic composition of noble gases have been measured in 20 H-chrondrites found on the Yamato Mountains ice fields in Antarctica. The distribution of exposure ages as well as of radiogenic He-4 contents is similar to that of H-chrondrites collected at the Allan Hills site. Furthermore, a comparison of the noble gas record of Antarctic H-chrondrites and finds or falls from non-Antarctic areas gives no support to the suggestion that Antarctic H-chrondrites and modern falls derive from differing interplanetary meteorite populations.

Sedimentary halogens and noble gases within Western Antarctic xenoliths: Implications of extensive volatile recycling to the sub continental lithospheric mantle

NASA Astrophysics Data System (ADS)

Broadley, Michael W.; Ballentine, Chris J.; Chavrit, Déborah; Dallai, Luigi; Burgess, Ray

2016-03-01

Recycling of marine volatiles back into the mantle at subduction zones has a profound, yet poorly constrained impact on the geochemical evolution of the Earth's mantle. Here we present a combined noble gas and halogen study on mantle xenoliths from the Western Antarctic Rift System (WARS) to better understand the flux of subducted volatiles to the sub continental lithospheric mantle (SCLM) and assess the impact this has on mantle chemistry. The xenoliths are extremely enriched in the heavy halogens (Br and I), with I concentrations up to 1 ppm and maximum measured I/Cl ratios (85.2 × 10-3) being ∼2000 times greater than mid ocean ridge basalts (MORB). The Br/Cl and I/Cl ratios of the xenoliths span a range from MORB-like ratios to values similar to marine pore fluids and serpentinites, whilst the 84Kr/36Ar and 130Xe/36Ar ratios range from modern atmosphere to oceanic sediments. This indicates that marine derived volatiles have been incorporated into the SCLM during an episode of subduction related metasomatism. Helium isotopic analysis of the xenoliths show average 3He/4He ratios of 7.5 ± 0.5 RA (where RA is the 3He/4He ratio of air = 1.39 × 10-6), similar to that of MORB. The 3He/4He ratios within the xenoliths are higher than expected for the xenoliths originating from the SCLM which has been extensively modified by the addition of subducted volatiles, indicating that the SCLM beneath the WARS must have seen a secondary alteration from the infiltration and rise of asthenospheric fluids/melts as a consequence of rifting and lithospheric thinning. Noble gases and halogens within these xenoliths have recorded past episodes of volatile interaction within the SCLM and can be used to reconstruct a tectonic history of the WARS. Marine halogen and noble gas signatures within the SCLM xenoliths provide evidence for the introduction and retention of recycled volatiles within the SCLM by subduction related metasomatism, signifying that not all volatiles that survive

Excitation mechanism in a hollow cathode He-Kr ion laser

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hazama, J.; Arai, T.; Goto, M.

1995-12-31

Pulsed laser operation in the afterglow of a positive column He-Kr discharge on the 469.4 nm (6s{sup 4}P{sub 5/2} {yields} 5p{sup 4}P{sub 5/2}) transition of Kr(II) was observed for the first time by Dana and Laure`s. It appears that the upper level of Kr(II) laser line is populated by the second kind collisions between He 2{sup 3}S metastable atoms and ground state Kr ions. CW oscillations on Kr(II) transitions have been obtained in a hollow cathode discharge. In this work, we have estimated the excitation mechanism for the upper state of 469.4 nm laser line from the measurements of themore » decay of endlight intensity in the hollow cathode He-Kr discharge.« less

Protonated ions as systemic trapping agents for noble gases: From electronic structure to radiative association.

PubMed

Ozgurel, O; Pauzat, F; Pilmé, J; Ellinger, Y; Bacchus-Montabonel, M-C; Mousis, O

2017-10-07

The deficiencies of argon, krypton, and xenon observed in the atmosphere of Titan as well as anticipated in some comets might be related to a scenario of sequestration by H 3 + in the gas phase at the early evolution of the solar nebula. The chemical process implied is a radiative association, evaluated as rather efficient in the case of H 3 + , especially for krypton and xenon. This mechanism of chemical trapping might not be limited to H 3 + only, considering that the protonated ions produced in the destruction of H 3 + by its main competitors present in the primitive nebula, i.e., H 2 O, CO, and N 2 , might also give stable complexes with the noble gases. However the effective efficiency of such processes is still to be proven. Here, the reactivity of the noble gases Ar, Kr, and Xe, with all protonated ions issued from H 2 O, CO, and N 2 , expected to be present in the nebula with reasonably high abundances, has been studied with quantum simulation method dynamics included. All of them give stable complexes and the rate coefficients of their radiative associations range from 10 -16 to 10 -19 cm 3 s -1 , which is reasonable for such reactions and has to be compared to the rates of 10 -16 to 10 -18 cm 3 s -1 , obtained with H 3 + . We can consider this process as universal for all protonated ions which, if present in the primitive nebula as astrophysical models predict, should act as sequestration agents for all three noble gases with increasing efficiency from Ar to Xe.

Coordination of ScO+ and YO+ by multiple Ar, Kr, and Xe atoms in noble gas matrixes: a matrix isolation infrared spectroscopic and theoretical study.

PubMed

Zhao, Yanying; Gong, Yu; Chen, Mohua; Ding, Chuanfan; Zhou, Mingfei

2005-12-29

The combination of matrix isolation infrared spectroscopic and quantum chemical calculation results provide strong evidence that scandium and yttrium monoxide cations, ScO+ and YO+, coordinate multiple noble gas atoms in forming noble gas complexes. The results showed that ScO+ coordinates five Ar, Kr, or Xe atoms, and YO+ coordinates six Ar or Kr and five Xe atoms in solid noble gas matrixes. Hence, the ScO+ and YO+ cations trapped in solid noble gas matrixes should be regarded as the [ScO(Ng)5]+ (Ng = Ar, Kr, or Xe), [YO(Ng)6]+ (Ng = Ar or Kr) or [YO(Xe)5]+ complexes. Experiments with dilute krypton or xenon in argon or krypton in xenon produced new IR bands, which are due to the stepwise formation of the [ScO(Ar)(5-n)(Kr)n]+, [ScO(Kr)(5-n)(Xe)n]+ (n = 1-5), [YO(Ar)(6-n)(Kr)n]+ (n = 1-6), and [YO(Ar)(6-n)(Xe)n]+ (n = 1-4) complexes.

Noble-gas-rich separates from ordinary chondrites

NASA Astrophysics Data System (ADS)

Moniot, R. K.

1980-02-01

Acid-resistant residues were prepared by HCl-HF demineralization of three H-type ordinary chondrites: Brownfield 1937 (H3), Dimmitt (H3, 4), and Estacado (H6). These residues were found to contain a large proportion of the planetary-type trapped Ar, Kr, and Xe in the meteorites. The similarity of these acid residues to those from carbonaceous chondrites and LL-type ordinary chondrites suggests that the same phase carries the trapped noble gases in all these diverse meteorite types. Because the H group represents a large fraction of all meteorites, this result indicates that the gas-rich carrier phase is as universal as the trapped noble-gas component itself. When treated with an oxidizing etchant, the acid residues lost almost all their complement of noble gases.

Energy-loss straggling of 2-10 MeV/u Kr ions in gases

NASA Astrophysics Data System (ADS)

Vockenhuber, Christof; Jensen, Jens; Julin, Jaakko; Kettunen, Heikki; Laitinen, Mikko; Rossi, Mikko; Sajavaara, Timo; Osmani, Orkhan; Schinner, Andreas; Sigmund, Peter; Whitlow, Harry J.

2013-07-01

Measurements have been performed on a time-of-flight setup at the Jyväskylä K130 cyclotron, aiming at energy-loss straggling of heavy ions in gases. Theoretical predictions based on recently developed theory as well as an empirical interpolation formula predict that straggling can be more than ten times higher than Bohr straggling in the MeV/u regime. Our measurements with up to 9.3 MeV/u Kr ions on He, N2, Ne and Kr targets confirm this feature. Our calculations show the relative contributions of linear straggling, bunching including packing, and charge exchange. Our results for stopping cross sections are compatible with values from the literature.

Theoretical study of metal noble-gas positive ions

NASA Technical Reports Server (NTRS)

Bauschlicher, Charles W., Jr.; Partridge, Harry; Langhoff, Stephen R.

1989-01-01

Theoretical calculations have been performed to determine the spectroscopic constant for the ground and selected low-lying electronic states of the transition-metal noble-gas ions Var(+), FeAr(+), CoAr(+), CuHe(+), CuAr(+), and CuKr(+). Analogous calculations have been performed for the ground states of the alkali noble-gas ions LiAr(+), LiKr(+), NaAr(+), and KAr(+) and the alkaline-earth noble-gas ion MgAr(+) to contrast the difference in binding energies between the simple and transition-metal noble-gas ions. The binding energies increase with increasing polarizability of the noble-gas ions, as expected for a charge-induced dipole bonding mechanism. It is found that the spectroscopic constants of the X 1Sigma(+) states of the alkali noble-gas ions are well described at the self-consistent field level. In contrast, the binding energies of the transition-metal noble-gas ions are substantially increased by electron correlation.

Noble gas partitioning behavior in the Sleipner Vest hydrocarbon field

NASA Astrophysics Data System (ADS)

Barry, P. H.; Lawson, M.; Warr, O.; Mabry, J.; Byrne, D. J.; Meurer, W. P.; Ballentine, C. J.

2015-12-01

Noble gases are chemically inert and variably soluble in crustal fluids. They are primarily introduced into hydrocarbon reservoirs through exchange with formation waters, and can be used to assess migration pathways, mechanisms and reservoir storage. Of particular interest is the role groundwater plays in hydrocarbon transport, which is reflected in hydrocarbon-water volume ratios. We present compositional, stable isotope and noble gas isotope and abundance data from the Sleipner Vest field, in the Norwegian North Sea. Sleipner gases are generated from primary cracking of kerogen and the thermal cracking of oil, sourced from type II marine source, with relatively homogeneous maturities and a range in vitrinite reflectance (1.2-1.7%). Gases are hosted in the lower shoreface sandstones of the Jurassic Hugin formation, which is sealed by the Jurassic Upper Draupne and Heather formations. Gases are composed of N2 (0.6-0.9%), CO2 (5.4-15.3%) and hydrocarbons (69-80%). Helium isotopes (3He/4He) are radiogenic and range from 0.065 to 0.116 RA, showing a small mantle contribution, consistent with Ne isotopes (20Ne/22Ne from 9.70-9.91; 21Ne/22Ne from 0.0290-0.0344) and Ar isotopes (40Ar/36Ar from 315-489). 20Ne/36Ar, 84Kr/36Ar and 132Xe/36Ar values are systematically higher relative to air saturated water ratios. These data are discussed within the framework of several conceptual models: i) Total gas-stripping model, which defines the minimum volume of water to have interacted with the hydrocarbon phase; ii) Equilibrium model, assuming simple equilibration between groundwater and hydrocarbon phase at reservoir P,T and salinity; and iii) Open and closed system gas-stripping models. Using Ne-Ar, we estimate gas-water ratios for the Sleipner system of 0.02-0.09, which compare with geologic gas-water estimates of ~0.24, and suggest more groundwater interaction than a static system estimate. Kr and Xe show evidence for an additional source or process involving oil or sediments.

Computational investigation of noble gas adsorption and separation by nanoporous materials.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Allendorf, Mark D.; Sanders, Joseph C.; Greathouse, Jeffery A.

2008-10-01

Molecular simulations are used to assess the ability of metal-organic framework (MOF) materials to store and separate noble gases. Specifically, grand canonical Monte Carlo simulation techniques are used to predict noble gas adsorption isotherms at room temperature. Experimental trends of noble gas inflation curves of a Zn-based material (IRMOF-1) are matched by the simulation results. The simulations also predict that IRMOF-1 selectively adsorbs Xe atoms in Xe/Kr and Xe/Ar mixtures at total feed gas pressures of 1 bar (14.7 psia) and 10 bar (147 psia). Finally, simulations of a copper-based MOF (Cu-BTC) predict this material's ability to selectively adsorb Xemore » and Kr atoms when present in trace amounts in atmospheric air samples. These preliminary results suggest that Cu-BTC may be an ideal candidate for the pre-concentration of noble gases from air samples. Additional simulations and experiments are needed to determine the saturation limit of Cu-BTC for xenon, and whether any krypton atoms would remain in the Cu-BTC pores upon saturation.« less

Recent Experimental Advances to Determine (noble) Gases in Waters

NASA Astrophysics Data System (ADS)

Kipfer, R.; Brennwald, M. S.; Huxol, S.; Mächler, L.; Maden, C.; Vogel, N.; Tomonaga, Y.

2013-12-01

In aquatic systems noble gases, radon, and bio-geochemically conservative transient trace gases (SF6, CFCs) are frequently applied to determine water residence times and to reconstruct past environmental and climatic conditions. Recent experimental breakthroughs now enable ● to apply the well-established concepts of terrestrial noble gas geochemistry in waters to the minute water amounts stored in sediment pore space and in fluid inclusions (A), ● to determine gas exchange processes on the bio-geochemical relevant time scales of minutes - hours (B), and ● to separate diffusive and advective gas transport in soil air (C). A. Noble-gas analysis in water samples (< 1 g) facilitates determining the solute transport in the pore space and identifying the origin of bio- and geogenic fluids in (un) consolidated sediments [1]. Advanced techniques that combine crushing and sieving speleothem samples in ultra-high-vacuum to a specific grain size allow to separate air and water-bearing fluid inclusions and thus enables noble-gas-based reconstruction of environmental conditions from water masses as small as 1mg [2]. B. The coupling of noble gas analysis with approaches of gas chromatography permits combined analysis of noble gases and other gases species (e.g., SF6, CFCs, O2, N2) from a single water sample. The new method substantially improves ground water dating by SF6 and CFCs as excess air is quantified from the same sample and hence can adequately be corrected for [3]. Portable membrane-inlet mass spectrometers enable the quasi-continuous and real-time analysis of noble gases and other dissolved gases directly in the field, allowing, for instance, quantification of O2 turnover rates on small time scales [4]. C. New technical developments perfect 222Rn analysis in water by the synchronous the determination of the short-lived 220Rn. The combined 220,222Rn analysis sheds light on the emanation behaviour of radon by identifying soil water content to be the crucial

Isotopic and noble gas geochemistry in geothermal research

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kennedy, B.M.; DePaolo, D.J.

1997-12-31

The objective of this program is to provide, through isotopic analyses of fluids, fluid inclusions, and rocks and minerals coupled with improved methods for geochemical data analysis, needed information regarding sources of geothermal heat and fluids, the spatial distribution of fluid types, subsurface flow, water-rock reaction paths and rates, and the temporal evolution of geothermal systems. Isotopic studies of geothermal fluids have previously been limited to the light stable isotopes of H, C, and O. However, other isotopic systems such as the noble gases (He, Ne, Ar, Kr and Xe) and reactive elements (e.g. B, N, S, Sr and Pb)more » are complementary and may even be more important in some geothermal systems. The chemistry and isotopic composition of a fluid moving through the crust will change in space and time in response to varying chemical and physical parameters or by mixing with additional fluids. The chemically inert noble gases often see through these variations, making them excellent tracers for heat and fluid sources. Whereas, the isotopic compositions of reactive elements are useful tools in characterizing water-rock interaction and modeling the movement of fluids through a geothermal reservoir.« less

The noble gases: how their electronegativity and hardness determines their chemistry.

PubMed

Furtado, Jonathan; De Proft, Frank; Geerlings, Paul

2015-02-26

The establishment of an internally consistent scale of noble gas electronegativities is a long-standing problem. In the present study, the problem is attacked via the Mulliken definition, which in recent years gained widespread use to its natural appearance in the context of conceptual density functional theory. Basic ingredients of this scale are the electron affinity and the ionization potential. Whereas the latter can be computed routinely, the instability of the anion makes the judicious choice of computational technique for evaluating electron affinities much more tricky. We opted for Puiatti's approach, extrapolating the energy of high ε solvent stabilized anions to the ε = 1 (gas phase) case. The results give negative electron affinity values, monotonically increasing (except for helium which is an outlier in most of the story) to almost zero at eka-radon in agreement with high level calculations. The stability of the B3LYP results is successfully tested both via improving the level of theory (CCSD(T)) and expanding the basis set. Combined with the ionization energies (in good agreement with experiment), an electronegativity scale is obtained displaying (1) a monotonic decrease of χ when going down the periodic table, (2) top values not for the noble gases but for the halogens, as opposed to most (extrapolation) procedures of existing scales, invariably placing the noble gases on top, and (3) noble gases having electronegativities close to the chalcogens. In the accompanying hardness scale (hardly, if ever, discussed in the literature) the noble gases turn out to be by far the farthest the hardest elements, again with a continuous decrease with increasing Z. Combining χ value of the halogens and the noble gases the Ng(δ+)F(δ-) bond polarity emerging from ab initio calculations naturally emerges. In conclusion, the chemistry of the noble gases is for a large part determined by their extreme hardness, equivalent to a high resistance to change in its

Detectability of Noble Gases in Jovian Atmospheres Utilizing Dimer Spectral Structures

NASA Astrophysics Data System (ADS)

Kim, S. J.; Min, Y.; Kim, Y.; Lee, Y.; Trafton, L.; Miller, S.; McKellar, A. R. W.

1997-07-01

The detection of jovian hydrogen-hydrogen dimers through the clear telluric 2-micron window (Kim et al. 1995; Trafton et al. 1997) suggests possibility to detect noble gases in the form of dimer with hydrogen in jovian atmospheres. Since noble gases do not have spectral structures in the infrared, it has been difficult to derive their abundances in the atmospheres of jovian planets. If there is a significant component of noble gases other than helium in the jovian atmospheres, it might be detected through its dimer spectrum with hydrogen molecule. The relatively sharp spectral structures of hydrogen-argon and hydrogen-neon dimers compared with those of hydrogen-hydrogen dimers are useful for the detection, if adequate S/N is obtained. However, these dimer structures should be much weaker than the nearby hydrogen-hydrogen features because noble gases are expected to be minor constituents of these atmospheres. We will discuss the detectability of these dimers based on laboratory measurements (McKellar, 1994; 1996), and current technology of infrared observations.

Comparison of various stopping gases for 3He-based position sensitive neutron detectors

NASA Astrophysics Data System (ADS)

Doumas, A.; Smith, G. C.

2012-05-01

A range of solid state, scintillator and gas based detectors are being developed for use at the next generation of high flux neutron facilities. Since gas detectors are expected to continue to play a key role in future specific thermal neutron experiments, a comparison of the performance characteristics of prospective stopping gases is beneficial. Gas detectors typically utilize the reaction 3He(n,p)t to detect thermal neutrons; the 3He gas is used in a mixture containing a particular stopping gas in order to maintain relatively short ranges for the proton and triton pair emitted from the n-3He reaction. Common stopping gases include hydrocarbons (e.g. propane), carbon tetrafluoride, and noble gases such as argon and xenon. For this study, we utilized the Monte Carlo simulation code "Stopping and Range of Ions in Matter" to analyze the expected behavior of argon, xenon, carbon dioxide, difluoroethane and octafluoropropane as stopping gases for thermal neutron detectors. We also compare these findings to our previously analyzed performance of propane, butane and carbon tetrafluoride. A discussion of these gases includes their behavior in terms of proton and triton range, ionization distribution and straggle.

MASCOT: a new mass-spectrometer facility dedicated to the analysis of cosmogenic noble gases (3He and 21Ne) from terrestrial samples (Institute of Geological Sciences - University of Bern, Switzerland).

NASA Astrophysics Data System (ADS)

Delunel, Romain; Enderli, Patrick; Jenni, Hans-Erich; Leya, Ingo; Schlunegger, Fritz

2017-04-01

In the past years, terrestrial cosmogenic nuclides have been successfully used for dating exposure history of landforms and measuring erosional processes on Earth's surface. In this context, quantifications of landscape change have mainly been accomplished through the use of radioactive cosmogenic nuclides such as 10Be and 26Al, but their application has generally been restricted to Quaternary time scales because of their relatively short half-lives. The results are 10Be and 26Al concentrations that are below the detection limit of available accelerator mass spectrometers if the samples have a Late Miocene or even a Pliocene age. Contrariwise, cosmogenic noble gases such as 3He and 21Ne do not experience any radioactive decay through time, which places these isotopes in an unbeatable position for measuring paleo-denudation rates preserved in detrital material even if the ages of these deposits are up to 10 Ma and even older. These isotopes are thus keys for assessing the interplays between tectonic, climate and surface processes involved in the long-term evolution of mountain belts. Here we report the technical specifications of a noble gas analytical system that we have developed and set up at the Institute of Geological Sciences of the University of Bern, Switzerland, with the motivations to get dates and rates of erosion processes from the measurement of cosmogenic noble gases (3He and 21Ne) concentrations from terrestrial samples. This new facility, hosted at the Institute of Geological Sciences of the University of Bern, combines a MAP215-50 mass spectrometer fitted with a new high-sensitivity channel electron multiplier with an all-metal extraction and purification line. This later system thus comprises: (i) a double vacuum resistance furnace loaded by a 22-samples carrousel, (ii) three in-vacuo crushers (iii) an ultra high vacuum pumping system (<10-8 mbar) composed of turbo-molecular, ion-getter pumps and backed by a scroll pump, (iv) the line itself made

A generic biokinetic model for noble gases with application to radon.

PubMed

Leggett, Rich; Marsh, James; Gregoratto, Demetrio; Blanchardon, Eric

2013-06-01

To facilitate the estimation of radiation doses from intake of radionuclides, the International Commission on Radiological Protection (ICRP) publishes dose coefficients (dose per unit intake) based on reference biokinetic and dosimetric models. The ICRP generally has not provided biokinetic models or dose coefficients for intake of noble gases, but plans to provide such information for (222)Rn and other important radioisotopes of noble gases in a forthcoming series of reports on occupational intake of radionuclides (OIR). This paper proposes a generic biokinetic model framework for noble gases and develops parameter values for radon. The framework is tailored to applications in radiation protection and is consistent with a physiologically based biokinetic modelling scheme adopted for the OIR series. Parameter values for a noble gas are based largely on a blood flow model and physical laws governing transfer of a non-reactive and soluble gas between materials. Model predictions for radon are shown to be consistent with results of controlled studies of its biokinetics in human subjects.

Exotic species with explicit noble metal-noble gas-noble metal linkages.

PubMed

Moreno, Norberto; Restrepo, Albeiro; Hadad, C Z

2018-02-14

We present a study of the isoelectronic Pt 2 Ng 2 F 4 and [Au 2 Ng 2 F 4 ] 2+ species with noble gas atoms (Ng = Kr, Xe, Rn) acting as links bridging the two noble metal atoms. The stability of the species is investigated using several thermodynamic, kinetic and reactivity indicators. The results are compared against [AuXe 4 ] 2+ , which is thermodynamically unstable in the gas phase but is stabilized in the solid state to the point that it has been experimentally detected as [AuXe 4 ](Sb 2 F 11 ) 2 (S. Seidel and K. Seppelt, Science, 2000, 290, 117-118). Our results indicate that improving upon [AuXe 4 ] 2+ , these exotic combinations between the a priori non-reactive noble metals and noble gases lead to metastable species, and, therefore, they have the possibility of existing in the solid state under adequate conditions. Our calculations include accurate energies and geometries at both the CCSD/SDDALL and MP2/SDDALL levels. We offer a detailed description of the nature of the bonding interactions using orbital and density-based analyses. The computational evidence suggests partially covalent and ionic interactions as the stabilization factors.

Noble Gas Signatures in Antrim Shale Gas in the Michigan Basin - Assessing Compositional Variability and Transport Processes

NASA Astrophysics Data System (ADS)

Wen, T.; Castro, M. C.; Ellis, B. R.; Hall, C. M.; Lohmann, K. C.; Bouvier, L.

2014-12-01

Recent studies in the Michigan Basin looked at the atmospheric and terrigenic noble gas signatures of deep brines to place constraints on the past thermal history of the basin and to assess the extent of vertical transport processes within this sedimentary system. In this contribution, we present noble gas data of shale gas samples from the Antrim shale formation in the Michigan Basin. The Antrim shale was one of the first economic shale-gas plays in the U.S. and has been actively developed since the 1980's. This study pioneers the use of noble gases in subsurface shale gas in the Michigan Basin to clarify the nature of vertical transport processes within the sedimentary sequence and to assess potential variability of noble gas signatures in shales. Antrim Shale gas samples were analyzed for all stable noble gases (He, Ne, Ar, Kr, Xe) from samples collected at depths between 300 and 500m. Preliminary results show R/Ra values (where R and Ra are the measured and atmospheric 3He/4He ratios, respectively) varying from 0.022 to 0.21. Although most samples fall within typical crustal R/Ra range values (~0.02-0.05), a few samples point to the presence of a mantle He component with higher R/Ra ratios. Samples with higher R/Ra values also display higher 20Ne/22Ne ratios, up to 10.4, and further point to the presence of mantle 20Ne. The presence of crustally produced nucleogenic 21Ne and radiogenic 40Ar is also apparent with 21Ne/22Ne ratios up to 0.033 and 40Ar/36Ar ratios up to 312. The presence of crustally produced 4He, 21Ne and 40Ar is not spatially homogeneous within the Antrim shale. Areas of higher crustal 4He production appear distinct to those of crustally produced 21Ne and 40Ar and are possibly related the presence of different production levels within the shale with varying concentrations of parent elements.

Submarine Alkalic Lavas Around the Hawaiian Hotspot; Plume and Non-Plume Signatures Determined by Noble Gases

NASA Astrophysics Data System (ADS)

Hanyu, T.; Clague, D. A.; Kaneoka, I.; Dunai, T. J.; Davies, G. R.

2004-12-01

Noble gas isotopic ratios were determined for submarine alkalic volcanic rocks distributed around the Hawaiian islands to constrain the origin of such alkalic volcanism. Samples were collected by dredging or using submersibles from the Kauai Channel between Oahu and Kauai, north of Molokai, northwest of Niihau, Southwest Oahu, South Arch and North Arch volcanic fields. Sites located downstream from the center of the hotspot have 3He/4He ratios close to MORB at about 8 Ra, demonstrating that the magmas erupted at these sites had minimum contribution of volatiles from a mantle plume. In contrast, the South Arch, located upstream of the hotspot on the Hawaiian Arch, has 3He/4He ratios between 17 and 21 Ra, indicating a strong plume influence. Differences in noble gas isotopic characteristics between alkalic volcanism downstream and upstream of the hotspot imply that upstream volcanism contains incipient melts from an upwelling mantle plume, having primitive 3He/4He. In combination with lithophile element isotopic data, we conclude that the most likely source of the upstream magmatism is depleted asthenospheric mantle that has been metasomatised by incipient melt from a mantle plume. After major melt extraction from the mantle plume during production of magmas for the shield stage, the plume material is highly depleted in noble gases and moderately depleted in lithophile elements. Partial melting of the depleted mantle impregnated by melts derived from this volatile depleted plume source may explain the isotopic characteristics of the downstream alkalic magmatism.

Light Noble Gas Abundances in the Solar Wind Trapped by Chondritic Metal

NASA Astrophysics Data System (ADS)

Murer, Ch.; Bauer, H.; Wieler, R.

1995-09-01

The heavy solar noble gases Ar-Xe are retained elementally unfractionated relative to the incoming solar corpuscular radiation in lunar soils, as is shown by the flat profiles of Ar/Kr and Kr/Xe throughout closed system stepped etch extractions [1, 2]. In contrast, He/Ar and Ne/Ar reach present-day solar wind (SW) values only towards the end of the runs, indicating that the well known fractionating losses of solar He and Ne from lunar samples affect the shallowly sited SW component but not the more deeply implanted SEP (solar energetic particles). Rather flat He/Ar and Ne/Ar profiles were previously observed in stepped etchings of metallic Fe-Ni from solar-gas-rich meteorites [3-5], suggesting that Fe-Ni retains unfractionated He, Ne, and Ar from SW and SEP. Most runs showed some variation in elemental ratios, possibly due to i) experiment-induced fractionation, ii) the different penetration depths of the various gases [4], or iii) variable elemental abundances in SW and SEP. The results of a repeat run on a Fe-Ni separate from the H chondrite Fayetteville are shown in Fig. 1. The ^20Ne/^36Ar ratio is essentially flat and most values fall in the range of 48.5 +/- 7 of the modern SW [6]. The low values in the last three steps are presumably due to fractionated solar noble gases released from silicate impurities by copper-chloride in these final about 10 day extractions, since the lowest value is close to that in bulk samples. We thus cannot confirm a real variation of Ne/Ar with grain depth. The He/Ar pattern is similar to Ne/Ar except that the values of individual steps scatter considerably more. Flat profiles as in Fig. 1 strongly suggest that the average ratios deduced from meteoritic Fe-Ni (in some cases slightly corrected for e. g. contributions from silicates) yield good estimates of the relative light noble gas abundances in SW and SEP trapped by chondritic regoliths. Table 1 shows best values deduced from three chondrites (two runs each). These values differ

Fluid clathrate system for continuous removal of heavy noble gases from mixtures of lighter gases

DOEpatents

Gross, K.C.; Markun, F.; Zawadzki, M.T.

1998-04-28

An apparatus and method are disclosed for separation of heavy noble gas in a gas volume. An apparatus and method have been devised which includes a reservoir containing an oil exhibiting a clathrate effect for heavy noble gases with a reservoir input port and the reservoir is designed to enable the input gas volume to bubble through the oil with the heavy noble gas being absorbed by the oil exhibiting a clathrate effect. The gas having reduced amounts of heavy noble gas is output from the oil reservoir, and the oil having absorbed heavy noble gas can be treated by mechanical agitation and/or heating to desorb the heavy noble gas for analysis and/or containment and allow recycling of the oil to the reservoir. 6 figs.

Fluid clathrate system for continuous removal of heavy noble gases from mixtures of lighter gases

DOEpatents

Gross, Kenneth C.; Markun, Francis; Zawadzki, Mary T.

1998-01-01

An apparatus and method for separation of heavy noble gas in a gas volume. An apparatus and method have been devised which includes a reservoir containing an oil exhibiting a clathrate effect for heavy noble gases with a reservoir input port and the reservoir is designed to enable the input gas volume to bubble through the oil with the heavy noble gas being absorbed by the oil exhibiting a clathrate effect. The gas having reduced amounts of heavy noble gas is output from the oil reservoir, and the oil having absorbed heavy noble gas can be treated by mechanical agitation and/or heating to desorb the heavy noble gas for analysis and/or containment and allow recycling of the oil to the reservoir.

Metal-organic frameworks for adsorption and separation of noble gases

DOEpatents

Allendorf, Mark D.; Greathouse, Jeffery A.; Staiger, Chad

2017-05-30

A method including exposing a gas mixture comprising a noble gas to a metal organic framework (MOF), including an organic electron donor and an adsorbent bed operable to adsorb a noble gas from a mixture of gases, the adsorbent bed including a metal organic framework (MOF) including an organic electron donor.

Enhancement of NMR and MRI in the presence of hyperpolarized noble gases

DOEpatents

Pines, Alexander; Budinger, Thomas; Navon, Gil; Song, Yi-Qiao; Appelt, Stephan; Bifone, Angelo; Taylor, Rebecca; Goodson, Boyd; Seydoux, Roberto; Room, Toomas; Pietrass, Tanja

2004-11-16

The present invention relates generally to nuclear magnetic resonance (NMR) techniques for both spectroscopy and imaging. More particularly, the present invention relates to methods in which hyperpolarized noble gases (e.g., Xe and He) are used to enhance and improve NMR and MRI. Additionally, the hyperpolarized gas solutions of the invention are useful both in vitro and in vivo to study the dynamics or structure of a system. When used with biological systems, either in vivo or in vitro, it is within the scope of the invention to target the hyperpolarized gas and deliver it to specific regions within the system.

Probing the interaction of noble gases with pristine and nitrogen-doped graphene through Raman spectroscopy

NASA Astrophysics Data System (ADS)

Cunha, Renato; Perea-López, Néstor; Elías, Ana Laura; Fujisawa, Kazunori; Carozo, Victor; Feng, Simin; Lv, Ruitao; dos Santos, Maria Cristina; Terrones, Mauricio; Araujo, Paulo T.

2018-05-01

The interactions of adsorbates with graphene have received increasing attention due to its importance in the development of applications involving graphene-based coatings. Here, we present a study of the adsorption of noble gases on pristine and nitrogen-doped graphene. Single-layer graphene samples were synthesized by chemical vapor deposition (CVD) and transferred to transmission electron microscopy (TEM) grids. Several noble gases were allowed to adsorb on the suspended graphene substrate at very low temperatures. Raman spectra show distinct frequency blue shifts in both the 2D and G bands, which are induced by gas adsorption onto high quality single layer graphene (1LG). These shifts, which we associate with compressive biaxial strain in the graphene layers induced by the noble gases, are negligible for nitrogen-doped graphene. Additionally, a thermal depinning transition, which is related to the desorption of a noble gas layer from the graphene surface at low temperatures (ranging from 20 to 35 K), was also observed at different transition temperatures for different noble gases. These transition temperatures were found to be 25 K for argon and 35 K for xenon. Moreover, we were able to obtain values for the compressive biaxial strain in graphene induced by the adsorbed layer of noble gases, using Raman spectroscopy. Ab initio calculations confirmed the correlation between the noble gas-induced strain and the changes in the Raman features observed.

Highly Concentrated Nebular Noble Gases in Porous Nanocarbon Separates from the Saratov (L4) Meteorite

NASA Astrophysics Data System (ADS)

Amari, Sachiko; Matsuda, Jun-ichi; Stroud, Rhonda M.; Chisholm, Matthew F.

2013-11-01

The majority of heavy noble gases (Ar, Kr, and Xe) in primitive meteorites are stored in a poorly understood phase called Q. Although Q is thought to be carbonaceous, the full identity of the phase has remained elusive for almost four decades. In order to better characterize phase Q and, in turn, the early solar nebula, we separated carbon-rich fractions from the Saratov (L4) meteorite. We chose this meteorite because Q is most resistant in thermal alteration among carbonaceous noble gas carriers in meteorites and we hoped that, in this highly metamorphosed meteorite, Q would be present but not diamond: these two phases are very difficult to separate from each other. One of the fractions, AJ, has the highest 132Xe concentration of 2.1 × 10-6 cm3 STP g-1, exceeding any Q-rich fractions that have yet been analyzed. Transmission electron microscopy studies of the fraction AJ and a less Q-rich fraction AI indicate that they both are primarily porous carbon that consists of domains with short-range graphene orders, with variable packing in three dimensions, but no long-range graphitic order. The relative abundance of Xe and C atoms (6:109) in the separates indicates that individual noble gas atoms are associated with only a minor component of the porous carbon, possibly one or more specific arrangements of the nanoparticulate graphene.

Energy-Transfer Kinetics for Xe (6p[1/2]0) Atoms in Kr, Ar, Ne, and He.

PubMed

He, Shan; Liu, Dong; Li, Xueyang; Chu, Junzhi; Guo, Jingwei; Liu, Jinbo; Hu, Shu; Sang, Fengting; Jin, Yuqi

2018-06-11

The kinetic processes for the Xe (6p[1/2] 0 ) atoms in Kr, Ar, Ne, and He buffer gases were studied. We found that Kr, Ar, and Ne atoms can be used to switch the amplified spontaneous emission (ASE) channel from 3408 nm (6p[1/2] 0 -6s'[1/2] 1 ) to 3680 nm (5d[1/2] 1 -6p[1/2] 1 ), while Xe and He atoms do not show such a phenomenon. This ASE channel switch is mainly ascribed to the fast transfer of 6p[1/2] 0 → 5d[1/2] 1 . On the basis of the rate equations for two-state coupling (energy-transfer processes between the two states are very rapid), the reason why the ASE channel switch effect normally coincides with a double exponential decay of the spontaneous emission at 828 nm (6p[1/2] 0 -6s[3/2] 1 ) is explained. The actual situations in Xe, Ar, Ne, and He follow this rule. However, the strictly single exponential decay of the spontaneous emission at 828 nm and strong ASE channel switch effect simultaneously emerge in Kr. This indicates that the transfer of 6p[1/2] 0 → 5d[1/2] 1 in Kr does not occur via two-state coupling, but via two steps of near-resonance collision through the 5s[3/2] 2 (Kr) state as the intermediate state (6p[1/2] 0 → 5s[3/2] 2 (Kr) → 5d[1/2] 1 ). In addition, we found Xe (6p[1/2] 0 ) atoms strongly tend to reach the 6p[3/2] 2 , 6p[3/2] 1 , and 6p[5/2] 2 states through the 5s[3/2] 2 (Kr) state as the intermediate state in Kr. The 5s[3/2] 2 (Kr) state plays a very important role in the energy-transfer kinetics for the Xe (6p[1/2] 0 ) atoms. Kr is probably an excellent buffer gas for laser systems based on Xe.

The contribution of hydrothermally altered ocean crust to the mantle halogen and noble gas cycles

NASA Astrophysics Data System (ADS)

Chavrit, Déborah; Burgess, Ray; Sumino, Hirochika; Teagle, Damon A. H.; Droop, Giles; Shimizu, Aya; Ballentine, Chris J.

2016-06-01

Recent studies suggest that seawater-derived noble gases and halogens are recycled into the deep mantle by the subduction of oceanic crust. To understand the processes controlling the availability of halogens and noble gases for subduction, we determined the noble gas elemental and isotopic ratios and halogen (Cl, Br, I) concentrations in 28 igneous samples from the altered oceanic crust (AOC) from 5 ODP sites in the Eastern and Western Pacific Ocean. Crushing followed by heating experiments enabled determination of noble gases and halogens in fluid inclusions and mineral phases respectively. Except for He and Ar, Ne, Kr and Xe isotopic ratios were all air-like suggesting that primary MORB signatures have been completely overprinted by air and/or seawater interaction. In contrast, 3He/4He ratios obtained by crushing indicate that a mantle helium component is still preserved, and 40Ar/36Ar values are affected by radiogenic decay in the mineral phases. The 130Xe/36Ar and 84Kr/36Ar ratios are respectively up to 15 times and 5 times higher than those of seawater and the highest ratios are found in samples affected by low temperature alteration (shallower than 800-900 m sub-basement). We consider three possible processes: (i) adsorption onto the clays present in the samples; (ii) fluid inclusions with a marine pore fluid composition; and (iii) fractionation of seawater through phase separation caused by boiling. Ninety percent of the Cl, Br and I were released during the heating experiments, showing that halogens are dominantly held in mineral phases prior to subduction. I/Cl ratios vary by 4 orders of magnitude, from 3 × 10-6 to 2 × 10-2. The mean Br/Cl ratio is 30% lower than in MORB and seawater. I/Cl ratios lower than MORB values are attributed to Cl-rich amphibole formation caused by hydrothermal alteration at depths greater than 800-900 m sub-basement together with different extents of I loss during low and high temperature alteration. At shallower depths, I

Noble gases identify the mechanisms of fugitive gas contamination in drinking-water wells overlying the Marcellus and Barnett Shales

PubMed Central

Darrah, Thomas H.; Vengosh, Avner; Jackson, Robert B.; Warner, Nathaniel R.; Poreda, Robert J.

2014-01-01

Horizontal drilling and hydraulic fracturing have enhanced energy production but raised concerns about drinking-water contamination and other environmental impacts. Identifying the sources and mechanisms of contamination can help improve the environmental and economic sustainability of shale-gas extraction. We analyzed 113 and 20 samples from drinking-water wells overlying the Marcellus and Barnett Shales, respectively, examining hydrocarbon abundance and isotopic compositions (e.g., C2H6/CH4, δ13C-CH4) and providing, to our knowledge, the first comprehensive analyses of noble gases and their isotopes (e.g., 4He, 20Ne, 36Ar) in groundwater near shale-gas wells. We addressed two questions. (i) Are elevated levels of hydrocarbon gases in drinking-water aquifers near gas wells natural or anthropogenic? (ii) If fugitive gas contamination exists, what mechanisms cause it? Against a backdrop of naturally occurring salt- and gas-rich groundwater, we identified eight discrete clusters of fugitive gas contamination, seven in Pennsylvania and one in Texas that showed increased contamination through time. Where fugitive gas contamination occurred, the relative proportions of thermogenic hydrocarbon gas (e.g., CH4, 4He) were significantly higher (P < 0.01) and the proportions of atmospheric gases (air-saturated water; e.g., N2, 36Ar) were significantly lower (P < 0.01) relative to background groundwater. Noble gas isotope and hydrocarbon data link four contamination clusters to gas leakage from intermediate-depth strata through failures of annulus cement, three to target production gases that seem to implicate faulty production casings, and one to an underground gas well failure. Noble gas data appear to rule out gas contamination by upward migration from depth through overlying geological strata triggered by horizontal drilling or hydraulic fracturing. PMID:25225410

Noble gases identify the mechanisms of fugitive gas contamination in drinking-water wells overlying the Marcellus and Barnett Shales.

PubMed

Darrah, Thomas H; Vengosh, Avner; Jackson, Robert B; Warner, Nathaniel R; Poreda, Robert J

2014-09-30

Horizontal drilling and hydraulic fracturing have enhanced energy production but raised concerns about drinking-water contamination and other environmental impacts. Identifying the sources and mechanisms of contamination can help improve the environmental and economic sustainability of shale-gas extraction. We analyzed 113 and 20 samples from drinking-water wells overlying the Marcellus and Barnett Shales, respectively, examining hydrocarbon abundance and isotopic compositions (e.g., C2H6/CH4, δ(13)C-CH4) and providing, to our knowledge, the first comprehensive analyses of noble gases and their isotopes (e.g., (4)He, (20)Ne, (36)Ar) in groundwater near shale-gas wells. We addressed two questions. (i) Are elevated levels of hydrocarbon gases in drinking-water aquifers near gas wells natural or anthropogenic? (ii) If fugitive gas contamination exists, what mechanisms cause it? Against a backdrop of naturally occurring salt- and gas-rich groundwater, we identified eight discrete clusters of fugitive gas contamination, seven in Pennsylvania and one in Texas that showed increased contamination through time. Where fugitive gas contamination occurred, the relative proportions of thermogenic hydrocarbon gas (e.g., CH4, (4)He) were significantly higher (P < 0.01) and the proportions of atmospheric gases (air-saturated water; e.g., N2, (36)Ar) were significantly lower (P < 0.01) relative to background groundwater. Noble gas isotope and hydrocarbon data link four contamination clusters to gas leakage from intermediate-depth strata through failures of annulus cement, three to target production gases that seem to implicate faulty production casings, and one to an underground gas well failure. Noble gas data appear to rule out gas contamination by upward migration from depth through overlying geological strata triggered by horizontal drilling or hydraulic fracturing.

The solvation radius of silicate melts based on the solubility of noble gases and scaled particle theory.

PubMed

Ottonello, Giulio; Richet, Pascal

2014-01-28

The existing solubility data on noble gases in high-temperature silicate melts have been analyzed in terms of Scaling Particle Theory coupled with an ab initio assessment of the electronic, dispersive, and repulsive energy terms based on the Polarized Continuum Model (PCM). After a preliminary analysis of the role of the contracted Gaussian basis sets and theory level in reproducing appropriate static dipole polarizabilities in a vacuum, we have shown that the procedure returns Henry's law constants consistent with the values experimentally observed in water and benzene at T = 25 °C and P = 1 bar for the first four elements of the series. The static dielectric constant (ɛ) of the investigated silicate melts and its optical counterpart (ɛ(∞)) were then resolved through the application of a modified form of the Clausius-Mossotti relation. Argon has been adopted as a probe to depict its high-T solubility in melts through an appropriate choice of the solvent diameter σs, along the guidelines already used in the past for simple media such as water or benzene. The σs obtained was consistent with a simple functional form based on the molecular volume of the solvent. The solubility calculations were then extended to He, Ne, and Kr, whose dispersive and repulsive coefficients are available from theory and we have shown that their ab initio Henry's constants at high T reproduce the observed increase with the static polarizability of the series element with reasonable accuracy. At room temperature (T = 25 °C) the calculated Henry's constants of He, Ne, Ar, and Kr in the various silicate media predict higher solubilities than simple extrapolations (i.e., Arrhenius plots) based on high-T experiments and give rise to smooth trends not appreciably affected by the static polarizabilities of the solutes. The present investigation opens new perspectives on a wider application of PCM theory which can be extended to materials of great industrial interest at the core of

Noble gases as cardioprotectants – translatability and mechanism

PubMed Central

Smit, Kirsten F; Weber, Nina C; Hollmann, Markus W; Preckel, Benedikt

2015-01-01

Several noble gases, although classified as inert substances, exert a tissue-protective effect in different experimental models when applied before organ ischaemia as an early or late preconditioning stimulus, after ischaemia as a post-conditioning stimulus or when given in combination before, during and/or after ischaemia. A wide range of organs can be protected by these inert substances, in particular cardiac and neuronal tissue. In this review we summarize the data on noble gas-induced cardioprotection, focusing on the underlying protective mechanisms. We will also look at translatability of experimental data to the clinical situation. PMID:25363501

Understanding the interaction of injected CO2 and reservoir fluids in the Cranfield enhanced oil recovery (EOR) field (MS, USA) by non-radiogenic noble gas isotopes

NASA Astrophysics Data System (ADS)

Gyore, Domokos; Stuart, Finlay; Gilfillan, Stuart

2016-04-01

Identifying the mechanism by which the injected CO2 is stored in underground reservoirs is a key challenge for carbon sequestration. Developing tracing tools that are universally deployable will increase confidence that CO2 remains safely stored. CO2 has been injected into the Cranfield enhanced oil recovery (EOR) field (MS, USA) since 2008 and significant amount of CO2 has remained (stored) in the reservoir. Noble gases (He, Ne, Ar, Kr, Xe) are present as minor natural components in the injected CO2. He, Ne and Ar previously have been shown to be powerful tracers of the CO2 injected in the field (Györe et al., 2015). It also has been implied that interaction with the formation water might have been responsible for the observed CO2 loss. Here we will present work, which examines the role of reservoir fluids as a CO2 sink by examining non-radiogenic noble gas isotopes (20Ne, 36Ar, 84Kr, 132Xe). Gas samples from injection and production wells were taken 18 and 45 months after the start of injection. We will show that the fractionation of noble gases relative to Ar is consistent with the different degrees of CO2 - fluid interaction in the individual samples. The early injection samples indicate that the CO2 injected is in contact with the formation water. The spatial distribution of the data reveal significant heterogeneity in the reservoir with some wells exhibiting a relatively free flow path, where little formation water is contacted. Significantly, in the samples, where CO2 loss has been previously identified show active and ongoing contact. Data from the later stage of the injection shows that the CO2 - oil interaction has became more important than the CO2 - formation water interaction in controlling the noble gas fingerprint. This potentially provides a means to estimate the oil displacement efficiency. This dataset is a demonstration that noble gases can resolve CO2 storage mechanisms and its interaction with the reservoir fluids with high resolution

Hydration of the Atlantis Massif: Halogen, Noble Gas and In-Situ δ18O Constraints

NASA Astrophysics Data System (ADS)

Williams, M. J.; Kendrick, M. A.; Rubatto, D.

2017-12-01

A combination of halogen (Cl, Br, I), noble gases (He, Ne, Ar, Kr and Xe) and in situ oxygen isotope analysis have been utilized to investigate the fluid-mobile element record of hydration and alteration processes at the Atlantis Massif (30°N on the Mid-Atlantic Ridge). The sample suite investigated includes serpentinite, talc-amphibole ± chlorite schist and hydrated gabbro recovered by seafloor drilling undertaken at sites on a transect across the Atlantis Massif during IODP Expedition 357. Serpentine mesh and veins analysed in-situ by SHRIMP SI exhibit δ18O from 6‰ down to ≈0‰, suggesting serpentinization temperatures of 150 to >280°C and water/rock ratios >5. Differences of 1.5-2.5‰ are observed between adjacent generations of serpentine, but the δ18O range is similar at each investigated drilling site. Halogen and noble gas abundances in serpentinites, talc-amphibole schist and hydrated gabbro have been measured by noble gas mass spectrometry of both irradiated and non-irradiated samples. Serpentinites contain low abundances of halogens and noble gases (e.g. 70-430 ppm Cl, 4.7-12.2 x 10-14 mol/g 36Ar) relative to other seafloor serpentinites. The samples have systematically different Br/Cl and I/Cl ratios related to their mineralogy. Serpentinites retain mantle-like Br/Cl with a wide variation in I/Cl that stretches toward seawater values. Talc-amphibole schists exhibit depletion of Br and I relative to Cl with increasing Cl abundances, suggesting tremolite exerts strong control on halogen abundance ratios. Serpentinites show no evidence of interaction with halogen-rich sedimentary pore fluids. Iodine abundances are variable across serpentinites, and are decoupled from Br and Cl; iodine enrichment (up to 530 ppb) is observed within relatively oxidised and clay-bearing samples. Serpentinized harzburgites exhibit distinct depletion of Kr and Xe relative to atmospheric 36Ar in seawater. Oxygen isotope compositions and low abundances of both halogens

Noble Gases in the Chelyabinsk Meteorites

NASA Technical Reports Server (NTRS)

Haba, Makiko K.; Sumino, Hirochika; Nagao, Keisuke; Mikouchi, Takashi; Komatsu, Mutsumi; Zolensky, Michael E.

2014-01-01

The Chelyabinsk meteorite fell in Russia on February 15, 2013 and was classified as LL5 chondrite. The diameter before it entered the atmosphere has been estimated to be about 20 m [1]. Up to now, numerous fragments weighing much greater than 100 kg in total have been collected. In this study, all noble gases were measured for 13 fragments to investigate the exposure history of the Chelyabinsk meteorite and the thermal history of its parent asteroid.

Highly concentrated nebular noble gases in porous nanocarbon separates from the Saratov (L4) meteorite

DOE Office of Scientific and Technical Information (OSTI.GOV)

Amari, Sachiko; Matsuda, Jun-ichi; Stroud, Rhonda M.

2013-11-20

The majority of heavy noble gases (Ar, Kr, and Xe) in primitive meteorites are stored in a poorly understood phase called Q. Although Q is thought to be carbonaceous, the full identity of the phase has remained elusive for almost four decades. In order to better characterize phase Q and, in turn, the early solar nebula, we separated carbon-rich fractions from the Saratov (L4) meteorite. We chose this meteorite because Q is most resistant in thermal alteration among carbonaceous noble gas carriers in meteorites and we hoped that, in this highly metamorphosed meteorite, Q would be present but not diamond:more » these two phases are very difficult to separate from each other. One of the fractions, AJ, has the highest {sup 132}Xe concentration of 2.1 × 10{sup –6} cm{sup 3} STP g{sup –1}, exceeding any Q-rich fractions that have yet been analyzed. Transmission electron microscopy studies of the fraction AJ and a less Q-rich fraction AI indicate that they both are primarily porous carbon that consists of domains with short-range graphene orders, with variable packing in three dimensions, but no long-range graphitic order. The relative abundance of Xe and C atoms (6:10{sup 9}) in the separates indicates that individual noble gas atoms are associated with only a minor component of the porous carbon, possibly one or more specific arrangements of the nanoparticulate graphene.« less

Above-threshold ionization of noble gases in elliptically polarized fields: Effects of atomic polarization on photoelectron angular distributions

NASA Astrophysics Data System (ADS)

Wang, YanLan; Yu, ShaoGang; Lai, XuanYang; Liu, XiaoJun; Chen, Jing

2017-06-01

We theoretically investigate the atomic polarization effect on photoelectron angular distributions (PADs) in above-threshold ionization of noble gases with elliptically polarized laser fields at wavelength of 800 nm, ellipticity of 0.25, and intensity of 1.5 ×1014W/cm2 . Simulations based on a semiclassical model that includes both the ionic Coulomb potential and the atomic polarization effect show surprisingly little difference between PADs for Ar, Kr, and Xe, which is in good agreement with recent experimental observations. Our calculations reveal that the atomic polarization effect increases the distance of the tunnel exit point of the photoelectron to the parent ion and weakens the strength of the interaction between the parent ion and the photoelectron on its subsequent classical propagation. As a result, the forward-scattering electrons which contribute to the main lobes in PADs are substantially suppressed. Our results indicate that the insensitivity of PADs for Ar, Kr, and Xe may be closely related to the influence of the atomic polarization effect on the photoelectron dynamics in the strong laser field.

Noble Gases in the Hamlet Meteorite (LL4)

NASA Astrophysics Data System (ADS)

Amari, S.; Sabe, Y.; Shiraishi, T.; Matsuda, J.

2014-09-01

We analyzed noble gases in a bulk sample and an HF-HCl residue of Hamlet (LL4). The Xe composition of the residue shows that no diamond is contained in the residue. The 20Ne/22Ne ratio of Hamlet Ne-Q has been determined to be 11.0 ± 0.5.

Investigation of Lung Structure-Function Relationships Using Hyperpolarized Noble Gases

NASA Astrophysics Data System (ADS)

Thomen, Robert P.

Magnetic Resonance Imaging (MRI) is an application of the nuclear magnetic resonance (NMR) phenomenon to non-invasively generate 3D tomographic images. MRI is an emerging modality for the lung, but it suffers from low sensitivity due to inherent low tissue density and short T(*/2) . Hyperpolarization is a process by which the nuclear contribution to NMR signal is greatly enhanced to more than 100,000 times that of samples in thermal equilibrium. The noble gases 3He and 129Xe are most often hyperpolarized by transfer of light angular momentum through the electron of a vaporized alkali metal to the noble gas nucleus (called Spin Exchange Optical Pumping). The enhancement in NMR signal is so great that the gas itself can be imaged via MRI, and because noble gases are chemically inert, they can be safely inhaled by a subject, and the gas distribution within the interior of the lung can be imaged. The mechanics of respiration is an elegant physical process by which air is is brought into the distal airspaces of the lungs for oxygen/carbon dioxide gas exchange with blood. Therefore proper description of lung function is intricately related to its physical structure , and the basic mechanical operation of healthy lungs -- from pressure driven airflow, to alveolar airspace gas kinetics, to gas exchange by blood/gas concentration gradients, to elastic contraction of parenchymal tissue -- is a process decidedly governed by the laws of physics. This dissertation will describe experiments investigating the relationship of lung structure and function using hyperpolarized (HP) noble gas MRI. In particular HP gases will be applied to the study of several pulmonary diseases each of which demonstrates unique structure-function abnormalities: asthma, cystic fibrosis, and chronic obstructive pulmonary disease. Successful implementation of an HP gas acquisition protocol for pulmonary studies is an involved and stratified undertaking which requires a solid theoretical foundation in NMR

Laser-polarized noble gases: a powerful probe for biology, medicine, and subatomic physics

NASA Astrophysics Data System (ADS)

Cates, Gordon

2010-03-01

For over a decade, laser-polarized noble gases such as ^3He and ^129Xe have proven useful for a wide range of scientific inquiries. These include investigations of pulmonary disease using the polarized gas as a signal source for magnetic resonance imaging (MRI), measurements of various aspects of nucleon structure, and tests of fundamental symmetries. Early efforts were often limited by expensive and bulky laser systems, but ongoing advancements in solid-state lasers have enabled increasingly large volumes of polarized gas to be produced with steadily improved polarization. Equally important have been advances in the fundamental understanding of spin exchange. This has led, for example, to the introduction of hybrid mixtures of alkali metals that can increase the efficiency of spin exchange by an order of magnitude. As a consequence of these advances, the figure of merit for polarized nuclear targets has increased by roughly three orders of magnitude in comparison to early accelerator-based experiments. And in MRI applications, it has become possible to pursue increasingly sophisticated imaging protocols that provide a wide range of diagnostic information. Even the earliest noble-gas MR images of the gas space of the human lung provided unprecedented resolution. More recent work includes the use of diffusion-sensitizing pulse sequences to study lung microstructure, and tagging techniques that enable the visualization (in real-time MRI movies) of gas flow during breathing. The range of applications of laser-polarized noble gases is continuing to grow, and it is notable that with an improved understanding of the underlying physics, it is quite likely that the capabilities of this useful technology will expand for some time to come.

Fullerenes: An extraterrestrial carbon carrier phase for noble gases

PubMed Central

Becker, Luann; Poreda, Robert J.; Bunch, Ted E.

2000-01-01

In this work, we report on the discovery of naturally occurring fullerenes (C60 to C400) in the Allende and Murchison meteorites and some sediment samples from the 65 million-year-old Cretaceous/Tertiary boundary layer (KTB). Unlike the other pure forms of carbon (diamond and graphite), fullerenes are extractable in an organic solvent (e.g., toluene or 1,2,4-trichlorobenzene). The recognition of this unique property led to the detection and isolation of the higher fullerenes in the Kratschmer/Huffmann arc evaporated graphite soot and in the carbon material in the meteorite and impact deposits. By further exploiting the unique ability of the fullerene cage structure to encapsulate and retain noble gases, we have determined that both the Allende and Murchison fullerenes and the KTB fullerenes contain trapped noble gases with ratios that can only be described as extraterrestrial in origin. PMID:10725367

Primordial domains in the depleted upper mantle identified by noble gases in MORBs

NASA Astrophysics Data System (ADS)

Tucker, J.; Mukhopadhyay, S.; Langmuir, C. H.; Hamelin, C.; Fuentes, J.

2017-12-01

The distribution of noble gas isotopic compositions in the mantle provides important constraints on the large-scale mantle evolution, as noble gases can trace the interaction between degassed, or processed, mantle domains and undegassed, or primitive, mantle domains. Data from the radiogenic He, Ne, Ar and Xe isotopic systems have shown that plume-related lavas sample relatively undegassed mantle domains, and the recent identification of isotopic anomalies in the short-lived I-Xe and Hf-W isotopic systems in plume-related lavas further suggests that these domains may be ancient, dating back to Earth's accretion. However, little is known about the potential variability of the heavy noble gas systems and the distribution of undegassed domains in the ambient upper mantle not influenced by plumes. Here, we present new high-precision He, Ne, Ar, and Xe isotopic data for a series of MORBs from a depleted section of the subtropical north Mid-Atlantic Ridge, distant from any known plume influence. Some samples have extremely low (unradiogenic) 4He/3He, 21Ne/22Ne, 40Ar/36Ar, and 129Xe/130Xe ratios, including some of the lowest values ever determined for MORBs. Such unradiogenic compositions are reminiscent of OIBs and plume-influenced E-MORBs, suggesting the presence of a relatively undegassed or primitive reservoir in the source of these depleted MORBs. The He, Ne, and Ar isotopic systems are sensitive to the long-term degassing history, suggesting that this domain in the MORB source is ancient. The 129Xe/130Xe ratio is sensitive to degassing only during the first 100 Ma of Earth history, suggesting that some of the isotopic character of these samples has been preserved since Earth's accretion. Together, these observations suggest that primordial or undegassed material is not only sampled in plumes-related lavas, but also normal, depleted MORBs. Along with data from E-MORBs in the southern EPR (Kurz et al., 2005), southern MAR (Sarda et al., 2000), and equatorial MAR

Noble gases and the early history of the Earth: Inappropriate paradigms and assumptions inhibit research and communication

NASA Technical Reports Server (NTRS)

Huss, G. R.; Alexander, E. C., Jr.

1985-01-01

The development of models as tracers of nobel gases through the Earth's evolution is discussed. A new set of paradigms embodying present knowledge was developed. Several important areas for future research are: (1) measurement of the elemental and isotopic compositions of the five noble gases in a large number of terrestrial materials, thus better defining the composition and distribution of terrestrial noble gases; (2) determinations of relative diffusive behavior, chemical behavior, and the distribution between solid and melt of noble gases under mantle conditions are urgently needed; (3) disequilibrium behavior in the nebula needs investigation, and the behavior of plasmas and possible cryotrapping on cold nebular solids are considered.

The MSFC Noble Gas Research Laboratory (MNGRL): A NASA Investigator Facility

NASA Technical Reports Server (NTRS)

Cohen, Barbara

2016-01-01

Noble-gas isotopes are a well-established technique for providing detailed temperature-time histories of rocks and meteorites. We have established the MSFC Noble Gas Research Laboratory (MNGRL) at Marshall Space Flight Center to serve as a NASA investigator facility in the wake of the closure of the JSC laboratory formerly run by Don Bogard. The MNGRL lab was constructed to be able to measure all the noble gases, particularly Ar-Ar and I-Xe radioactive dating to find the formation age of rocks and meteorites, and Ar/Kr/Ne cosmic-ray exposure ages to understand when the meteorites were launched from their parent planets.

Noble gases in submarine pillow basalt glasses from Loihi and Kilauea, Hawaii: A solar component in the Earth

USGS Publications Warehouse

Honda, M.; McDougall, I.; Patterson, D.B.; Doulgeris, A.; Clague, D.A.

1993-01-01

Noble gas elemental and isotopic abundances have been analysed in twenty-two samples of basaltic glass dredged from the submarine flanks of two currently active Hawaiian volcanoes, Loihi Seamount and Kilauea. Neon isotopic ratios are enriched in 20Ne and 21Ne by as much as 16% with respect to atmospheric ratios. All the Hawaiian basalt glass samples show relatively high 3He 4He ratios. The high 20Ne 22Ne values in some of the Hawaiian samples, together with correlations between neon and helium systematics, suggest the presence of a solar component in the source regions of the Hawaiian mantle plume. The solar hypothesis for the Earth's primordial noble gas composition can account for helium and neon isotopic ratios observed in basaltic glasses from both plume and spreading systems, in fluids in continental hydrothermal systems, in CO2 well gases, and in ancient diamonds. These results provide new insights into the origin and evolution of the Earth's atmosphere. ?? 1993.

Tracing enhanced oil recovery signatures in casing gases from the Lost Hills oil field using noble gases

USGS Publications Warehouse

Barry, Peter H.; Kulongoski, Justin; Landon, Matthew K.; Tyne, R.L.; Gillespie, Janice; Stephens, Michael; Hillegonds, D.J.; Byrne, D.J.; Ballentine, C.J.

2018-01-01

Enhanced oil recovery (EOR) and hydraulic fracturing practices are commonly used methods to improve hydrocarbon extraction efficiency; however the environmental impacts of such practices remain poorly understood. EOR is particularly prevalent in oil fields throughout California where water resources are in high demand and disposal of high volumes of produced water may affect groundwater quality. Consequently, it is essential to better understand the fate of injected (EOR) fluids in California and other subsurface petroleum systems, as well as any potential effect on nearby aquifer systems. Noble gases can be used as tracers to understand hydrocarbon generation, migration, and storage conditions, as well as the relative proportions of oil and water present in the subsurface. In addition, a noble gas signature diagnostic of injected (EOR) fluids can be readily identified. We report noble gas isotope and concentration data in casing gases from oil production wells in the Lost Hills oil field, northwest of Bakersfield, California, and injectate gas data from the Fruitvale oil field, located within the city of Bakersfield. Casing and injectate gas data are used to: 1) establish pristine hydrocarbon noble-gas signatures and the processes controlling noble gas distributions, 2) characterize the noble gas signature of injectate fluids, 3) trace injectate fluids in the subsurface, and 4) construct a model to estimate EOR efficiency. Noble gas results range from pristine to significantly modified by EOR, and can be best explained using a solubility exchange model between oil and connate/formation fluids, followed by gas exsolution upon production. This model is sensitive to oil-water interaction during hydrocarbon expulsion, migration, and storage at reservoir conditions, as well as any subsequent modification by EOR.

Groundwater studies using isotopes and noble gases as a tracer: Review and prospect

NASA Astrophysics Data System (ADS)

Kazahaya, Kohei; Yasuhara, Masaya; Takahashi, Hiroshi A.; Morikawa, Noritoshi; Ohwada, Michiko; Tosaki, Yuki; Asai, Kazuyoshi

Environmental tracers become a common tool for the groundwater study and a number of methods have been presented in order to understand groundwater flow processes, water budget, origins, chemical reaction processes and retention time. Tracers often used are selected and reviewed for their various methods and advantages as follows; 1) stable 18O, D in water, 2) stable 13C and radioactive 14C in DIC, 3) noble gases such as He, Ne, Ar, Kr, Xe and their isotopes, 4) radioactive 36Cl in dissolved chloride and some heavier isotopes, and 5) inert gaseous species such as CFCs. If they are less reactive species, they likely preserve information at the time of recharge or their origin. Use of D, 18O and the d-value of water is the powerful tool to determine the recharge area because recharged meteoric water have their inherent isotopic ratios correlated with the recharge elevation, distance from the coast, or the local topography. Carbon-bearing species are more reactive though, use of stable isotopes of DIC leads to identify its origin and helps to analyze the chemical reaction between minerals and water or gas addition processes during the groundwater flow in aquifers. Radioactive 14C has been used to estimate groundwater age however special attention should be paid for, i.e., the origin of DIC, before applying the method. Noble gas tracers are the useful species to presume recharge temperature from their concentrations in water using their temperature dependence of solubilities. Radiogenic 4He concentration can be used for the very long-term groundwater dating since the 4He is produced in the crust and is accumulated in the deep aquifers, if the local accumulation rate of 4He is known. Radioactive 36Cl has been used to determine the age of very old saline waters up to million years. This isotope will also be convenient for the dating of very younger waters, by the use of bomb-produced 36Cl resulted from surface nuclear experiments near the seawater in the 1950s

Efficient conversion of 3He(n,tp) and 10B(n, α7Li) reaction energies into far-ultraviolet radiation by noble gas excimers

NASA Astrophysics Data System (ADS)

Hughes, Patrick P.; Coplan, Michael A.; Thompson, Alan K.; Vest, Robert E.; Clark, Charles W.

2011-03-01

Previous work showed that the 3He(n , tp) reaction in a cell of 3He at atmospheric pressure generated tens of far-ultraviolet (FUV) photons per reacted neutron. Here we report amplification of that signal by factors of 1000 when noble gases are added to the cell. Calibrated filter-detector measurements show that this large signal is due to noble-gas excimer emissions, and that the nuclear reaction energy is converted to FUV radiation with efficiencies of up to 30 % . Our results have been placed on an absolute scale through calibrations at the NIST SURF III Synchrotron and Center for Neutron Research. We have also seen large neutron-induced FUV signals when the 3He gas in our system is replaced with a 10B film target; an experiment on substituting 3He with BF3 is underway. Our results suggest possibilities for high-efficiency, non-3He neutron detectors as an alternative to existing proportional counters.

The spectrum of density fluctuations of noble gases probed by THz neutron and x-ray spectroscopy

DOE PAGES

Cunsolo, Alessandro

2016-02-26

Approximately 50 years of inelastic scattering studies of noble gases are reviewed to illustrate the main advances achieved in the understanding of the THz dynamics of simple systems. The gradual departure of the spectral shape from the hydrodynamic regime is discussed with an emphasis on the phenomenology of fast (sub- ps) relaxation processes. This review shows that relaxation phenomena in noble gases have an essentially collisional origin, which is also revealed by the parallelism between their characteristic timescale and the interatomic collision time. In addition, recent THz spectroscopy results on noble gases at extreme thermodynamic conditions are discussed to illustratemore » the need for a revision of our current understanding of the supercritical phase.« less

Incorporation of Solar Noble Gases from a Nebula-Derived Atmosphere During Magma Ocean Cooling

NASA Technical Reports Server (NTRS)

Woolum, D. S.; Cassen, P.; Wasserburg, G. J.; Porcelli, D.; DeVincenzi, Donald (Technical Monitor)

1998-01-01

The presence of solar noble gases in the deep interior of the Earth is inferred from the Ne isotopic compositions of MORB (Mid-ocean Ridge Basalts) and OIB (Oceanic Island Basalt); Ar data may also consistent with a solar component in the deep mantle. Models of the transport and distribution of noble gases in the earth's mantle allow for the presence of solar Ar/Ne and Xe/Ne ratios and permit the calculation of lower mantle noble gas concentrations. These mantle data and models also indicate that the Earth suffered early (0.7 to 2 x 10(exp 8) yr) and large (greater than 99 percent) losses of noble gases from the interior, a result previously concluded for atmospheric Xe. We have pursued the suggestion that solar noble gases were incorporated in the forming Earth from a massive, nebula-derived atmosphere which promoted large-scale melting, so that gases from this atmosphere dissolved in the magma ocean and were mixed downward. Models of a primitive atmosphere captured from the solar nebula and supported by accretion luminosity indicate that pressures at the Earth's surface were adequate (and largely more than the required 100 Atm) to dissolve sufficient gases. We have calculated the coupled evolution of the magma ocean and the overlying atmosphere under conditions corresponding to the cessation (or severe attenuation) of the sustaining accretion luminosity, prior to the complete removal of the solar nebula. Such a condition was likely to obtain, for instance, when most of the unaccumulated mass resided in large bodies which were only sporadically accreted. The luminosity supporting the atmosphere is then that provided by the cooling Earth, consideration of which sets a lower limit to the time required to solidify the mantle and terminate the incorporation of atmospheric gases within it. In our initial calculations, we have fixed the nebula temperature at To = 300K, a value likely to be appropriate for nebular temperatures at lAU in the early planet-building epoch

Noble Gas signatures of Enhanced Oil Recovery

NASA Astrophysics Data System (ADS)

Barry, P. H.; Kulongoski, J. T.; Tyne, R. L.; Hillegonds, D.; Byrne, D. J.; Landon, M. K.; Ballentine, C. J.

2017-12-01

Noble gases are powerful tracers of fluids from various oil and gas production activities in hydrocarbon reservoirs and nearby groundwater. Non-radiogenic noble gases are introduced into undisturbed oil and natural gas reservoirs through exchange with formation waters [1-3]. Reservoirs with extensive hydraulic fracturing, injection for enhanced oil recovery (EOR), and/or waste disposal also show evidence for a component of noble gases introduced from air [4]. Isotopic and elemental ratios of noble gases can be used to 1) assess the migration history of the injected and formation fluids, and 2) determine the extent of exchange between multiphase fluids in different reservoirs. We present noble gas isotope and abundance data from casing, separator and injectate gases of the Lost Hills and Fruitvale oil fields in the San Joaquin basin, California. Samples were collected as part of the California State Water Resource Control Board's Oil and Gas Regional Groundwater Monitoring Program. Lost Hills (n=7) and Fruitvale (n=2) gases are geochemically distinct and duplicate samples are highly reproducible. Lost Hills casing gas samples were collected from areas where EOR and hydraulic fracturing has occurred in the past several years, and from areas where EOR is absent. The Fruitvale samples were collected from a re-injection port. All samples are radiogenic in their He isotopes, typical of a crustal environment, and show enrichments in heavy noble gases, resulting from preferential adsorption on sediments. Fruitvale samples reflect air-like surface conditions, with higher air-derived noble gas concentrations. Lost Hills gases show a gradation from pristine crustal signatures - indicative of closed-system exchange with formation fluids - to strongly air-contaminated signatures in the EOR region. Pristine samples can be used to determine the extent of hydrocarbon exchange with fluids, whereas samples with excess air can be used to quantify the extent of EOR. Determining noble

Trapping Ne, Ar, Kr, and Xe in Si2O3 smokes

NASA Technical Reports Server (NTRS)

Nuth, Joseph A., III; Donn, Bertram; Olinger, Chad; Garrison, Dan; Hohenberg, Charles

1988-01-01

Simple Si2O3 smokes have been condensed at both low (less than 750 K) and high (greater than 1000 K) temperature at 35 torr H2 pressure in the presence of 0, 10, 100, and 1000 microns of a noble gas mixture containing Ne, Ar, Kr, and Xe. In general, both Ne and Ar are quite loosely bound in the smokes (6.0 x 10 to the -8th and 2.6 x 10 to the -4th ccSTP/g, respectively), and are degassed at temperatures below 1200 K. Both Kr and Xe are somewhat more strongly bound at concentrations of 1.0 x 10 to the -7th and 8.2 x 10 to the -8th ccSTP/g, respectively, and in addition show a double release with a second component at a temperature of about 1875 K. With the exception that Si2O3 smokes appear to show a particular affinity for argon, possibly due to an anomalous absorption of atmospheric argon, none of the other noble gases are found in sufficient concentration to explain the gases observed in meteorites as primary circumstellar condensates. However, this data in conjunction with observations of Honda et al. (1979) do seem to show a degree of dependence between noble gas retention and chemical composition.

Solubilities of nitrogen and noble gases in basalt melt

NASA Technical Reports Server (NTRS)

Miyazaki, A.; Hiyagon, H.; Sugiura, N.

1994-01-01

Nitrogen and noble gases are important tracers in geochemistry and chosmochemistry. Compared to noble gases, however, physicochemical properties of nitrogen, such as solubility in melt or melt/silicate partition, are not well known. Solubility of nitrogen in basalt melt depends on redox condition of the atmosphere. For example, solubility of nitrogen in E chondrite melt under reducing conditions is as high as 2 mol percent at 1500 C, suggesting that nitrogen is chemically dissolved in silicate melts, i.e., being dissolved as free anions or replacing oxygen sites in silicate network. However, the solubility and the dissolution mechanism of nitrogen under oxidizing conditions are not well investigated. To obtain nitrogen solubility in silicate melts under various redox conditions and to understand its mechanism, we are conducting experiments by using (15)N(15)N-labeled nitrogen gas. This makes it easy to distinguish dissolved nitrogen from later contamination of atmospheric nitrogen, and hence enables us to measure the nitrogen solubility accurately. As a preliminary experiment, we have measured solubility of nitrogen in basalt melt under the atmospheric oxygen pressure.

Intermolecular dissociation energies of dispersively bound complexes of aromatics with noble gases and nitrogen

NASA Astrophysics Data System (ADS)

Knochenmuss, Richard; Sinha, Rajeev K.; Leutwyler, Samuel

2018-04-01

We measured accurate intermolecular dissociation energies D0 of the supersonic jet-cooled complexes of 1-naphthol (1NpOH) with the noble gases Ne, Ar, Kr, and Xe and with N2, using the stimulated-emission pumping resonant two-photon ionization method. The ground-state values D0(S0) for the 1NpOHṡS complexes with S= Ar, Kr, Xe, and N2 were bracketed to be within ±3.5%; they are 5.67 ± 0.05 kJ/mol for S = Ar, 7.34 ± 0.07 kJ/mol for S = Kr, 10.8 ± 0.28 kJ/mol for S = Xe, 6.67 ± 0.08 kJ/mol for isomer 1 of the 1NpOHṡN2 complex, and 6.62 ± 0.22 kJ/mol for the corresponding isomer 2. For S = Ne, the upper limit is D0 < 3.36 kJ/mol. The dissociation energies increase by 1%-5% upon S0 → S1 excitation of the complexes. Three dispersion-corrected density functional theory (DFT-D) methods (B97-D3, B3LYP-D3, and ωB97X-D) predict that the most stable form of these complexes involves dispersive binding to the naphthalene "face." A more weakly bound edge isomer is predicted in which the S moiety is H-bonded to the OH group of 1NpOH; however, no edge isomers were observed experimentally. The B97-D3 calculated dissociation energies D0(S0) of the face complexes with Ar, Kr, and N2 agree with the experimental values within <5%, but the D0(S0) for Xe is 12% too low. The B3LYP-D3 and ωB97X-D calculated D0(S0) values exhibit larger deviations to both larger and smaller dissociation energies. For comparison to 1-naphthol, we calculated the D0(S0) of the carbazole complexes with S = Ne, Ar, Kr, Xe, and N2 using the same DFT-D methods. The respective experimental values have been previously determined to be within <2%. Again, the B97-D3 results are in the best overall agreement with experiment.

Noble gases in submarine pillow basalt glasses from Loihi and Kilauea, Hawaii: A solar component in the Earth

DOE Office of Scientific and Technical Information (OSTI.GOV)

Honda, M.; McDougall, I.; Patterson, D.B.

1993-02-01

Noble gas elemental and isotopic abundances have been analysed in twenty-two samples of basaltic glass dredged from the submarine flanks of two currently active Hawaiian volcanoes, Loihi Seamount and Kilauea. Neon isotopic ratios are enriched in [sup 20]Ne and [sup 21]Ne by as much as 16% with respect to atmospheric ratios. All the Hawaiian basalt glass samples show relatively high [sup 3]He/[sup 4]He ratios. The high [sup 20]Ne/[sup 22]Ne values in some of the Hawaiian samples, together with correlations between neon and helium systematics, suggest the presence of a solar component in the source regions of the Hawaiian mantle plume.more » The solar hypothesis for the Earth's primordial noble gas composition can account for helium and neon isotopic ratios observed in basaltic glasses from both plume and spreading systems, in fluids in continental hydrothermal systems, in CO[sub 2] well gases, and in ancient diamonds. These results provide new insights into the origin and evolution of the Earth's atmosphere.« less

Ab initio theory of noble gas atoms in bcc transition metals

DOE PAGES

Jiang, Chao; Zhang, Yongfeng; Gao, Yipeng; ...

2018-01-01

Systematic ab initio calculations based on density functional theory have been performed to gain fundamental understanding of the interactions between noble gas atoms (He, Ne, Ar and Kr) and bcc transition metals in groups 5B (V, Nb and Ta), 6B (Cr, Mo and W) and 8B (Fe).

Observations of mass fractionation of noble gases in synthetic methane hydrate

USGS Publications Warehouse

Hunt, Andrew G.; Pohlman, John; Stern, Laura A.; Ruppel, Carolyn D.; Moscati, Richard J.; Landis, Gary P.; Pinkston, John C.

2011-01-01

As a consequence of contemporary or longer term (since 15 ka) climate warming, gas hydrates in some settings are presently dissociating and releasing methane and other gases to the oceanatmosphere system. A key challenge in assessing the susceptibility of gas hydrates to warming climate is the lack of a technique able to distinguish between methane recently released from gas hydrates and methane emitted from leaky thermogenic reservoirs, shallow sublake and subseafloor sediments, coalbeds, and other sources. Carbon and deuterium stable isotopic data provide only a first-order characterization of methane sources, while gas hydrate can sequester any type of methane. Here, we investigate the possibility of exploiting the pattern of noble gas fractionation within the gas hydrate lattice to fingerprint methane released from gas hydrates. Starting with synthetic gas hydrate formed under careful laboratory conditions, we document complex noble gas fractionation patterns in the gases liberated during dissociation and explore the effects of aging and storage (e.g., in liquid nitrogen), as well as sampling and preservation procedures. The laboratory results confirm a unique noble gas fractionation pattern for gas hydrates, one that shows promise in evaluating modern natural gas seeps for a signature associated with gas hydrate dissociation.

Regularities And Irregularities Of The Stark Parameters For Single Ionized Noble Gases

NASA Astrophysics Data System (ADS)

Peláez, R. J.; Djurovic, S.; Cirišan, M.; Aparicio, J. A.; Mar S.

2010-07-01

Spectroscopy of ionized noble gases has a great importance for the laboratory and astrophysical plasmas. Generally, spectra of inert gases are important for many physics areas, for example laser physics, fusion diagnostics, photoelectron spectroscopy, collision physics, astrophysics etc. Stark halfwidths as well as shifts of spectral lines are usually employed for plasma diagnostic purposes. For example atomic data of argon krypton and xenon will be useful for the spectral diagnostic of ITER. In addition, the software used for stellar atmosphere simulation like TMAP, and SMART require a large amount of atomic and spectroscopic data. Availability of these parameters will be useful for a further development of stellar atmosphere and evolution models. Stark parameters data of spectral lines can also be useful for verification of theoretical calculations and investigation of regularities and systematic trends of these parameters within a multiplet, supermultiplet or transition array. In the last years, different trends and regularities of Stark parameters (halwidths and shifts of spectral lines) have been analyzed. The conditions related with atomic structure of the element as well as plasma conditions are responsible for regular or irregular behaviors of the Stark parameters. The absence of very close perturbing levels makes Ne II as a good candidate for analysis of the regularities. Other two considered elements Kr II and Xe II with complex spectra present strong perturbations and in some cases an irregularities in Stark parameters appear. In this work we analyze the influence of the perturbations to Stark parameters within the multiplets.

Bremsstrahlung of nitrogen and noble gases in single-bubble sonoluminescence

NASA Astrophysics Data System (ADS)

Xu, Ning; Wang, Long; Hu, Xiwei

2000-03-01

A hydrodynamic model, discussing neutral gases as well as plasmas, is applied to simulate single-bubble sonoluminescence. In this model, thermal conduction and various inelastic impact processes such as dissociation, ionization, and recombination are considered. Bremsstrahlung is assumed as the mechanism of the picosecond light pulse in sonoluminescence. Diatomic nitrogen and noble gas bubbles are studied. The results show that the sonoluminescing bubbles are completely optically thin for bremsstrahlung. The calculated spectra agree with previous observations, and can explain the observed differences in spectra of different gases.

Understanding and modulating the high-energy properties of noble-gas hydrides from their long-bonding: an NBO/NRT investigation on HNgCO+/CS+/OSi+ and HNgCN/NC (Ng = He, Ar, Kr, Xe, Rn) molecules.

PubMed

Zhang, Guiqiu; Song, Junjie; Fu, Lei; Tang, Kongshuang; Su, Yue; Chen, Dezhan

2018-04-18

The noble-gas hydrides, HNgX (X is an electronegative atom or fragment), represent potential high-energy materials because their two-body decomposition process, HNgX → Ng + HX, is strongly exoergic. Our previous studies have shown that each member of the HNgX (X = halogen atom or CN/NC fragment) molecules is composed of three leading resonance structures: two ω-bonding structures (H-Ng+ :X- and H:- Ng+-X) and one long-bonding structure (H∧X). The last one paints a novel [small sigma, Greek, circumflex]-type long-bonding picture. The present study focuses on the relationship between this novel bonding motif and the unusual energetic properties. We chose HNgCO+/CS+/OSi+/CN/NC, with the formula HNgAB (Ng = He, Ar, Kr, Xe, Rn; AB = CO+/CS+/OSi+/CN/NC) as the research system. We first investigated the bonding of HNgCO+ and its analogous HNgCS+/OSi+ species using NBO/NRT methods, and quantitatively compared the bonding with that in HNgCN/NC molecules. NBO/NRT results showed that each of the HNgCO+/CS+/OSi+ molecules could be better represented as a resonance hybrid of ω-bonding and long-bonding structures, but the long-bonding is much weaker than that in HNgCN/NC molecules. Furthermore, we introduced the long-bonding concept into the rationalization of the high-energy properties, and found a good correlation between the highly exothermic two-body dissociation channel and the long-bond order, bH-A. We also found that the long-bond order is highly tunable for these noble-gas hydrides due to its dependence on the nature of the electronegative AB fragments or the central noble-gas atoms, Ng. On the basis of these results, we could optimize the energetic properties by changing the long-bonding motif of our studied molecules. Overall, this study shows that the long-bonding model provides an easy way to rationalize and modulate the unusual energy properties of noble-gas hydrides, and that it is helpful to predict some noble-gas hydrides as potential energetic materials.

On the origin of (4)He and (40)Ar in natural gold

NASA Technical Reports Server (NTRS)

Eugster, O.; Hofmann, B.; Niedermann, S.; Thalmann, CH.

1993-01-01

In a first report on our investigations of noble gases in native gold we demonstrated that placer gold contains an excess of radiogenic (4)He and (40)Ar relative to the concentrations expected from in situ decay of U, Th, and K, respectively, during the geologic age of about 30 Ma of the samples. We also showed that the U/Th-(4)He age of 36 Ma of vein-type gold from the Southern Alps agrees with its K-Ar formation age derived from associated muscovite and biotite. We now studied the question of the origin of the (4)He and (40)Ar excesses of placer gold. We conclude that gold contains two components of noble gases, a low-temperature component from fluid inclusions or phases which release noble gases at less than 800 C and a high-temperature component released when gold melts (1064 C). In some samples extremely high U and K concentrations or an unreasonably high formation age would be required to explain the observed (4)He abundances. Thus, trapped (4)He and (40)Ar must be present in gold.

Applicability of Monte-Carlo Simulation to Equipment Design of Radioactive Noble Gas Monitor

NASA Astrophysics Data System (ADS)

Sakai, Hirotaka; Hattori, Kanako; Umemura, Norihiro

In the nuclear facilities, radioactive noble gas is continuously monitored by using the radioactive noble gas monitor with beta-sensitive plastic scintillation radiation detector. The detection efficiency of the monitor is generally calibrated by using a calibration loop and standard radioactive noble gases such as 85Kr. In this study, the applicability of PHITS to the equipment design of the radioactive noble gas monitor was evaluated by comparing the calculated results to the test results obtained by actual calibration loop tests to simplify the radiation monitor design evaluation. It was confirmed that the calculated results were well matched to the test results of the monitor after the modeling. In addition, the key parameters for equipment design, such as thickness of detector window or depth of the sampler, were also specified and evaluated.

Noble gases, nitrogen, and methane from the deep interior to the atmosphere of Titan

NASA Astrophysics Data System (ADS)

Glein, Christopher R.

2015-04-01

Titan's thick N2-CH4 atmosphere is unlike any in the Solar System, and its origin has been shrouded in mystery for over half a century. Here, I perform a detailed analysis of chemical and isotopic data from the Cassini-Huygens mission to develop the hypothesis that Titan's (non-photochemical) atmospheric gases came from deep within. It is suggested that Titan's CH4, N2, and noble gases originated in a rocky core buried inside the giant satellite, and hydrothermal and cryovolcanic processes were critical to the creation of Titan's atmosphere. Mass balance and chemical equilibrium calculations demonstrate that all aspects of this hypothesis can be considered geochemically plausible with respect to contemporary observational, experimental, and theoretical knowledge. Specifically, I show that a rocky core with a bulk noble gas content similar to that in CI carbonaceous meteorites would contain sufficient 36Ar and 22Ne to explain their reported abundances. I also show that Henry's law constants for noble gases in relevant condensed phases can be correlated with the size of their atoms, which leads to expected mixing ratios for 84Kr (∼0.2 ppbv) and 132Xe (∼0.01 ppbv) that can explain why these species have yet to be detected (Huygens upper limit <10 ppbv). The outgassing of volatiles into Titan's atmosphere may be restricted by the stability of clathrate hydrates in Titan's interior. The noble gas geochemistry also provides significant new insights into the origin of N2 and CH4 on Titan, as I find that Ar and N2, and Kr and CH4 should exhibit similar phase partitioning behavior on Titan. One implication is that over 95% of Titan's N2 may still reside in the interior. Another key result is that the upper limit from the Huygens GC-MS on the Kr/CH4 ratio in Titan's atmosphere is far too low to be consistent with accretion of primordial CH4 clathrate, which motivates me to consider endogenic production of CH4 from CO2 as a result of geochemical reactions between liquid

Adsorption of Dissolved Gases (CH4, CO2, H2, Noble Gases) by Water-Saturated Smectite Clay Minerals

NASA Astrophysics Data System (ADS)

Bourg, I. C.; Gadikota, G.; Dazas, B.

2016-12-01

Adsorption of dissolved gases by water-saturated clay minerals plays important roles in a range of fields. For example, gas adsorption in on clay minerals may significantly impact the formation of CH4 hydrates in fine-grained sediments, the behavior of CH4 in shale, CO2 leakage across caprocks of geologic CO2 sequestration sites, H2 leakage across engineered clay barriers of high-level radioactive waste repositories, and noble gas geochemistry reconstructions of hydrocarbon migration in the subsurface. Despite its importance, the adsorption of gases on clay minerals remains poorly understood. For example, some studies have suggested that clay surfaces promote the formation of CH4 hydrates, whereas others indicate that clay surfaces inhibit the formation of CH4 hydrates. Here, we present molecular dynamics (MD) simulations of the adsorption of a range of gases (CH4, CO2, H2, noble gases) on clay mineral surfaces. Our results indicate that the affinity of dissolved gases for clay mineral surfaces has a non-monotone dependence on the hydrated radius of the gas molecules. This non-monotone dependence arises from a combination of two effects: the polar nature of certain gas molecules (in particular, CO2) and the templating of interfacial water structure by the clay basal surface, which results in the presence of interfacial water "cages" of optimal size for intermediate-size gas molecules (such as Ne or Ar).

Advancing Physically-Based Flow Simulations of Alluvial Systems Through Atmospheric Noble Gases and the Novel 37Ar Tracer Method

NASA Astrophysics Data System (ADS)

Schilling, Oliver S.; Gerber, Christoph; Partington, Daniel J.; Purtschert, Roland; Brennwald, Matthias S.; Kipfer, Rolf; Hunkeler, Daniel; Brunner, Philip

2017-12-01

To provide a sound understanding of the sources, pathways, and residence times of groundwater water in alluvial river-aquifer systems, a combined multitracer and modeling experiment was carried out in an important alluvial drinking water wellfield in Switzerland. 222Rn, 3H/3He, atmospheric noble gases, and the novel 37Ar-method were used to quantify residence times and mixing ratios of water from different sources. With a half-life of 35.1 days, 37Ar allowed to successfully close a critical observational time gap between 222Rn and 3H/3He for residence times of weeks to months. Covering the entire range of residence times of groundwater in alluvial systems revealed that, to quantify the fractions of water from different sources in such systems, atmospheric noble gases and helium isotopes are tracers suited for end-member mixing analysis. A comparison between the tracer-based mixing ratios and mixing ratios simulated with a fully-integrated, physically-based flow model showed that models, which are only calibrated against hydraulic heads, cannot reliably reproduce mixing ratios or residence times of alluvial river-aquifer systems. However, the tracer-based mixing ratios allowed the identification of an appropriate flow model parametrization. Consequently, for alluvial systems, we recommend the combination of multitracer studies that cover all relevant residence times with fully-coupled, physically-based flow modeling to better characterize the complex interactions of river-aquifer systems.

Primordial and cosmogenic noble gases in the Sutter's Mill CM chondrite

NASA Astrophysics Data System (ADS)

Okazaki, Ryuji; Nagao, Keisuke

2017-04-01

The Sutter's Mill (SM) CM chondrite fell in California in 2012. The CM chondrite group is one of the most primitive, consisting of unequilibrated minerals, but some of them have experienced complex processes occurring on their parent body, such as aqueous alteration, thermal metamorphism, brecciation, and solar wind implantation. We have determined noble gas concentrations and isotopic compositions for SM samples using a stepped heating gas extraction method, in addition to mineralogical observation of the specimens. The primordial noble gas abundances, especially the P3 component trapped in presolar diamonds, confirm the classification of SM as a CM chondrite. The mineralogical features of SM indicate that it experienced mild thermal alteration after aqueous alteration. The heating temperature is estimated to be <350 °C based on the release profile of primordial 36Ar. The presence of a Ni-rich Fe-Ni metal suggests that a minor part of SM has experienced heating at >500 °C. The variation in the heating temperature of thermal alteration is consistent with the texture as a breccia. The heterogeneous distribution of solar wind noble gases is also consistent with it. The cosmic-ray exposure (CRE) age for SM is calculated to be 0.059 ± 0.023 Myr based on cosmogenic 21Ne by considering trapped noble gases as solar wind, the terrestrial atmosphere, P1 (or Q), P3, A2, and G components. The CRE age lies at the shorter end of the CRE age distribution of the CM chondrite group.

Experimental Constraints on He, Ne, and Ar Solubility in Serpentinite

NASA Astrophysics Data System (ADS)

Krantz, J. A.; Parman, S. W.; Kelley, S. P.; Smye, A.; Jackson, C.; Cooper, R. F.

2015-12-01

Experiments have been performed to constrain the solubility of He, Ne, and Ar in natural samples of antigorite from three locations. Geochemical analyses of exhumed subduction zone material [1] and well gases [2] indicate that noble gases are recycled from the surface of the earth into the mantle. The mechanism by which uncharged atoms can be bound to a mineral and subsequently recycled remains unclear, but recent experimental work suggests that ring structures in silicate minerals are ideal sites for noble gases [3]. Serpentine contains such ring structures and is abundant in subducting slabs, providing significant potential for control of the recycling of noble gases. Experiments were performed in a cold seal pressure vessel at 350°C using a mix of equal parts He, Ne, and Ar as the pressure media (Brown University, USA). Pressures varied from 0.15 to 1.13 kbar total pressure and durations varied from 20 to 188 hours. Samples were analyzed by UV laser ablation, noble gas mass spectrometry (Open University, UK). He and Ne reached equilibrium during the experiments and both exhibit Henrian behavior. Data from the cleanest sample reduces the error by approximately an order of magnitude over previous work [3] and confirms that He is significantly more soluble (HCHe=6.05x10-10 mol/g/bar) than Ne (HCNe=5.12x10-12 mol/g/bar) in antigorite. Preliminary data from the cleanest sample suggests that Ar is more soluble than both He and Ne (HCAr=1.94x10-10 mol/g/bar). This provides a mechanism for fractionation of noble gases during recycling. 1. Kendrick, M.A., Scambelluri, M., Honda, M., Phillips, D., Nature Geoscience, 4, 807-812, 2011 2. Holland, G., and Ballentine, C.J., Nature, 441, 186-191, 2006 3. Jackson, C.R.M., Parman, S.W., Kelley, S.P., Cooper, R.F., GCA, 159, 1-15, 2015

Noble gases in diamonds - Occurrences of solarlike helium and neon

NASA Technical Reports Server (NTRS)

Honda, M.; Reynolds, J. H.; Roedder, E.; Epstein, S.

1987-01-01

Seventeen diamond samples from diverse locations were analyzed for the contents of He, Ar, Kr, and Xe, and of their isotopes, using a Reynolds (1956) type glass mass spectrometer. The results disclosed a large spread in the He-3/He-4 ratios, ranging from values below atmospheric to close to the solar ratio. In particular, solarlike He-3/He-4 ratios were seen for an Australian colorless diamond composite and an Arkansas diamond, which also displayed solarlike neon isotopic ratios. Wide variation was also observed in the He-4/Ar-40 ratios, suggesting a complex history for the source regions and the diamond crystallization processes.

Dating and tracing groundwater resources in central Québec with noble gases, 14C and water chemistry

NASA Astrophysics Data System (ADS)

Vautour, G.; Pinti, D. L.; Castro, M. C.; Barbecot, F.; Larocque, M.; Hall, C. M.

2011-12-01

Canada water supply is derived mainly from lakes and rivers while groundwater accounts for less than 30% of the demand. Climatic and anthropogenic stress is endangering this natural resource. This study is part of a Quebec-funded program to characterize groundwater resources from major basins to ensure adequate water quality and management. The Bécancour River catchment area, 200 km NE of Montréal, is studied for this purpose. The region extends from the Appalachian Mts. down to the St. Lawrence River. Water chemistry shows the occurrence of Ca,Na-HCO3, Ca-HCO3, Na-HCO3 and NaCl waters, mainly recharged in the Appalachians and flowing to the St. Lawrence River. Aquifers are also recharged locally through Quaternary sandy deposits throughout the plain. Main aquifers are found both in unconfined and confined Quaternary sands intercalated with clays, and also locally in fractured Ordovician carbonates. To identify groundwater flow paths and to estimate water residence times, a multi-isotopic study involving noble gases, 14C and U, Th isotopes was initiated. Noble gas preliminary results were obtained on two transects, one along the downward flow path and the second perpendicular to the first, along a deeper sinclinorium with NaCl waters (TDS =170-705 mg/L). The 3He/4He ratios versus 4He/20Ne clearly points to mixing between three water bodies. The first has been recharged very recently displaying a near-atmospheric ratio of 0.79 Ra (Ra=atmospheric 3He/4He ratio of 1.386 x 10-6) and a 4He/20Ne of 0.2 close to the Air Saturated Water value, i.e. the ratio of atmospheric He and Ne dissolved in groundwater. The second water body is slightly older and shows the occurrence of tritiogenic 3He (3Hetri) excesses up to 1.07x10-13 ccSTP/g. These waters are found along the transect parallel to the main flow path. Using a local tritium decay curve and measured 3Hetri, an age of 19-20 years is suggested. The third water body contains large amounts of radiogenic 4He produced by U

Howardite Noble Gases as Indicators of Asteroid Surface Processing

NASA Technical Reports Server (NTRS)

Cartwright, J. A.; Mittlefehldt, D. W.; Herrin, J. S.; Ott, U.

2011-01-01

The HED (Howardite, Eucrite and Diogenite) group meteorites likely or iginate from the Asteroid 4 Vesta - one of two asteroid targets of NA SA's Dawn mission. Whilst Howardites are polymict breccias of eucriti c and diogenitic material that often contain "regolithic" petrologica l features, neither their exact regolithic nature nor their formation processes are well defined. As the Solar Wind (SW) noble gas compon ent is implanted onto surfaces of solar system bodies, noble gas anal yses of Howardites provides a key indicator of regolithic origin. In addition to SW, previous work by suggested that restricted Ni (300-12 00 micro g/g) and Al2O3 (8-9 wt%) contents may indicate an ancient we ll-mixed regolith. Our research combines petrological, compositional and noble gas analyses to help improve understanding of asteroid reg olith formation processes, which will play an intergral part in the i nterpretation of Dawn mission data. Following compositional and petrological analyses, we developed a regolith grading scheme for our sampl e set of 30 Howardites and polymict Eucrites. In order to test the r egolith indicators suggested by, our 8 selected samples exhibited a r ange of Ni, Al2O3 contents and regolithic grades. Noble gas analyses were performed using furnace stepheating on our MAP 215-50 noble gas mass spectrometer. Of our 8 howardites, only 3 showed evidence of SW noble gases (e.g approaching Ne-20/Ne-22 approximately equals 13.75, Ne-21/Ne-22 approximately equals 0.033). As these samples display low regolithic grades and a range of Ni and Al2O3 contents, so far we are unable to find any correlation between these indicators and "regolit hic" origin. These results have a number of implications for both Ho wardite and Vesta formation, and may suggest complex surface stratigr aphies and surface-gardening processes.

Theoretical investigation of HNgNH{sub 3}{sup +} ions (Ng = He, Ne, Ar, Kr, and Xe)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Kunqi; Sheng, Li, E-mail: shengli@hit.edu.cn

2015-04-14

The equilibrium geometries, harmonic frequencies, and dissociation energies of HNgNH{sub 3}{sup +} ions (Ng = He, Ne, Ar, Kr, and Xe) were investigated using the following method: Becke-3-parameter-Lee-Yang-Parr (B3LYP), Boese-Matrin for Kinetics (BMK), second-order Møller-Plesset perturbation theory (MP2), and coupled-cluster with single and double excitations as well as perturbative inclusion of triples (CCSD(T)). The results indicate that HHeNH{sub 3}{sup +}, HArNH{sub 3}{sup +}, HKrNH{sub 3}{sup +}, and HXeNH{sub 3}{sup +} ions are metastable species that are protected from decomposition by high energy barriers, whereas the HNeNH{sub 3}{sup +} ion is unstable because of its relatively small energy barrier for decomposition.more » The bonding nature of noble-gas atoms in HNgNH{sub 3}{sup +} was also analyzed using the atoms in molecules approach, natural energy decomposition analysis, and natural bond orbital analysis.« less

In vivo MRI Using Laser Polarized Noble Gases.

NASA Astrophysics Data System (ADS)

Cates, G. D.

1996-03-01

A new technique for magnetic resonance imaging (MRI) will be reviewed in which the noble gas nuclei ^3He and ^129Xe are used as the source of signal instead of the protons in water, as is the case in conventional MRI. The noble gas nuclei are polarized by spin exchange with laser optically pumped alkali-metal vapor. The noble gas, which under appropriate conditions can exhibit spin relaxation times of hours to days, can be inhaled, making it possible to obtain images of the gas space of the lungs of unprecedented resolution. In the case of ^129Xe, substantial quantities of gas dissolves into the blood, opening up the prospect of imaging other parts of the body such as the heart and the brain. Recent results will be reviewed, including lung images of both guinea pigs and humans from a Duke/Princeton collaboration, and spectroscopic measurements of ^129Xe that is dissolved in mouse blood, from the Stony Brook group. Other results will be reviewed as available. Attention will be given to the issues involved in producing large quantities of polarized noble gas for imaging, including a discussion of the use of high power diode laser arrays, a technology that has helped this new MRI technique grow quickly to be of potential clinical value. Finally, future prospects for the diagnosis of disease will be discussed.

Noble gases as tracers of the origin and evolution of the Martian atmosphere and the degassing history of the planet

NASA Technical Reports Server (NTRS)

Swindle, T. D.

1988-01-01

Noble gas analysis of Martian samples can provide answers to a number of crucial questions. Some of the most obvious benefits will be in Martian chronology, using techniques that have been applied to lunar samples. However, these are by no means the only relevant noble gas studies possible. Since Mars has a substantial atmosphere, noble gases can be used to study the origin and evolution of that atmosphere, including the degassing history of the planet. This type of study can provide constraints on: (1) the total noble gas inventory of the planet, (2) the number of noble gas reservoirs existing, and (3) the exchange of gases between these reservoirs. How to achieve these goals are examined.

New methods for measuring atmospheric heavy noble gas isotope and elemental ratios in ice core samples.

PubMed

Bereiter, Bernhard; Kawamura, Kenji; Severinghaus, Jeffrey P

2018-05-30

The global ocean constitutes the largest heat buffer in the global climate system, but little is known about its past changes. The isotopic and elemental ratios of heavy noble gases (krypton and xenon), together with argon and nitrogen in trapped air from ice cores, can be used to reconstruct past mean ocean temperatures (MOTs). Here we introduce two successively developed methods to measure these parameters with a sufficient precision to provide new constraints on past changes in MOT. The air from an 800-g ice sample - containing roughly 80 mL STP air - is extracted and processed to be analyzed on two independent dual-inlet isotope ratio mass spectrometers. The primary isotope ratios (δ 15 N, δ 40 Ar and δ 86 Kr values) are obtained with precisions in the range of 1 per meg (0.001‰) per mass unit. The three elemental ratio values δKr/N 2 , δXe/N 2 and δXe/Kr are obtained using sequential (non-simultaneous) peak-jumping, reaching precisions in the range of 0.1-0.3‰. The latest version of the method achieves a 30% to 50% better precision on the elemental ratios and a twofold better sample throughput than the previous one. The method development uncovered an unexpected source of artefactual gas fractionation in a closed system that is caused by adiabatic cooling and warming of gases (termed adiabatic fractionation) - a potential source of measurement artifacts in other methods. The precisions of the three elemental ratios δKr/N 2 , δXe/N 2 and δXe/Kr - which all contain the same MOT information - suggest smaller uncertainties for reconstructed MOTs (±0.3-0.1°C) than previous studies have attained. Due to different sensitivities of the noble gases to changes in MOT, δXe/N 2 provides the best constraints on the MOT under the given precisions followed by δXe/Kr, and δKr/N 2 ; however, using all of them helps to detect methodological artifacts and issues with ice quality. Copyright © 2018 John Wiley & Sons, Ltd.

Noble gas Records of Early Evolution of the Earth

NASA Astrophysics Data System (ADS)

Ozima, M.; Podoesk, F. A.

2001-12-01

Comparison between atmospheric noble gases (except for He) and solar (or meteoritic) noble gases clearly suggests that the Earth should have much more Xe than is present in air, and thus that up to about 90 percent of terrestrial Xe is missing from the Earth (1). In this report, we discuss implications of these observations on I-Pu chronology of the Earth and on the origin of terrestrial He3. Whetherill (2) first noted that an estimated I129/I127 ratio (3x10-6) in the proto-Earth was about two orders of magnitude smaller than values commonly observed in meteorites (10-4), and pointed out the possibility that Earth formation postdated meteorites by about 100Ma. Ozima and Podosek (1999) came to a similar conclusion on the basis of I129/I127-Pu244/U238 systematics (1). In this report, we reexamine I-Pu systematics with new data for crustal I content (295 ppb for a bulk crust, (3)). With imposition of an estimated value of 86 percent missing Xe as a constraint on terrestrial Xe inventory, we conclude that the best estimate for a formation age of the Earth is about 28Ma after the initial condensation of the solar nebula (at 4.57Ga). The formation age thus estimated is significantly later than the generally assumed age of meteorites. We also argue from the I-Pu systematics that the missing Xe became missing place about 120Ma after Earth formation. Assuming that the Earth is mostly degassed, the I-Pu formation age of the Earth can be reasonably assumed to represent a whole Earth event. Therefore, we interpret that the I-Pu age of the Earth represents the time when the Earth started to retain noble gases. More specifically, this may correspond to the time when the proto-Earth attained a sufficient size to exert the necessary gravitational force. A giant impact could be another possibility, but it remains to be seen whether or not a giant impact could quantitatively remove heavier noble gases from the Earth. It is interesting to speculate that missing Xe was sequestered in

Ground-Water Temperature, Noble Gas, and Carbon Isotope Data from the Espanola Basin, New Mexico

USGS Publications Warehouse

Manning, Andrew H.

2009-01-01

Ground-water samples were collected from 56 locations throughout the Espanola Basin and analyzed for general chemistry (major ions and trace elements), carbon isotopes (delta 13C and 14C activity) in dissolved inorganic carbon, noble gases (He, Ne, Ar, Kr, Xe, and 3He/4He ratio), and tritium. Temperature profiles were measured at six locations in the southeastern part of the basin. Temperature profiles suggest that ground water generally becomes warmer with distance from the mountains and that most ground-water flow occurs at depths 50 years old, consistent with the 14C ages. Terrigenic He (Heterr) concentrations in ground water are high (log Delta Heterr of 2 to 5) throughout much of the basin. High Heterr concentrations are probably caused by in situ production in the Tesuque Formation from locally high concentrations of U-bearing minerals (Northeast zone only), or by upward diffusive/advective transport of crustal- and mantle-sourced He possibly enhanced by basement piercing faults, or by both. The 3He/4He ratio of Heterr (Rterr) is commonly high (Rterr/Ra of 0.3-2.0, where Ra is the 3He/4He ratio in air) suggesting that Espanola Basin ground water commonly contains mantle-sourced He. The 3He/4He ratio of Heterr is generally the highest in the western and southern parts of the basin, closest to the western border fault system and the Quaternary to Miocene volcanics of the Jemez Mountains and Cerros del Rio.

The Noble Gas Fingerprint in a UK Unconventional Gas Reservoir

NASA Astrophysics Data System (ADS)

McKavney, Rory; Gilfillan, Stuart; Györe, Domokos; Stuart, Fin

2016-04-01

In the last decade, there has been an unprecedented expansion in the development of unconventional hydrocarbon resources. Concerns have arisen about the effect of this new industry on groundwater quality, particularly focussing on hydraulic fracturing, the technique used to increase the permeability of the targeted tight shale formations. Methane contamination of groundwater has been documented in areas of gas production1 but conclusively linking this to fugitive emissions from unconventional hydrocarbon production has been controversial2. A lack of baseline measurements taken before drilling, and the equivocal interpretation of geochemical data hamper the determination of possible contamination. Common techniques for "fingerprinting" gas from discrete sources rely on gas composition and isotopic ratios of elements within hydrocarbons (e.g. δ13CCH4), but the original signatures can be masked by biological and gas transport processes. The noble gases (He, Ne, Ar, Kr, Xe) are inert and controlled only by their physical properties. They exist in trace quantities in natural gases and are sourced from 3 isotopically distinct environments (atmosphere, crust and mantle)3. They are decoupled from the biosphere, and provide a separate toolbox to investigate the numerous sources and migration pathways of natural gases, and have found recent utility in the CCS4 and unconventional gas5 industries. Here we present a brief overview of noble gas data obtained from a new coal bed methane (CBM) field, Central Scotland. We show that the high concentration of helium is an ideal fingerprint for tracing fugitive gas migration to a shallow groundwater. The wells show variation in the noble gas signatures that can be attributed to differences in formation water pumping from the coal seams as the field has been explored for future commercial development. Dewatering the seams alters the gas/water ratio and the degree to which noble gases degas from the formation water. Additionally the

Nuclear magnetic resonance of laser-polarized noble gases in molecules, materials and organisms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Goodson, Boyd McLean

1999-12-01

Conventional nuclear magnetic resonance (NMR) spectroscopy and magnetic resonance imaging (MRI) are fundamentally challenged by the insensitivity that stems from the ordinarily low spin polarization achievable in even the strongest NMR magnets. However, by transferring angular momentum from laser light to electronic and nuclear spins, optical pumping methods can increase the nuclear spin polarization of noble gases by several orders of magnitude, thereby greatly enhancing their NMR sensitivity. This dissertation is primarily concerned with the principles and practice of optically pumped nuclear magnetic resonance (OPNMR). The enormous sensitivity enhancement afforded by optical pumping noble gases can be exploited to permitmore » a variety of novel NMR experiments across many disciplines. Many such experiments are reviewed, including the void-space imaging of organisms and materials, NMR and MRI of living tissues, probing structure and dynamics of molecules in solution and on surfaces, and zero-field NMR and MRI.« less

The Noble Gas Record of Gas-Water Phase Interaction in the Tight-Gas-Sand Reservoirs of the Rocky Mountains

NASA Astrophysics Data System (ADS)

Ballentine, C. J.; Zhou, Z.; Harris, N. B.

2015-12-01

The mass of hydrocarbons that have migrated through tight-gas-sandstone systems before the permeability reduces to trap the hydrocarbon gases provides critical information in the hydrocarbon potential analysis of a basin. The noble gas content (Ne, Ar, Kr, Xe) of the groundwater has a unique isotopic and elemental composition. As gas migrates through the water column, the groundwater-derived noble gases partition into the hydrocarbon phase. Determination of the noble gases in the produced hydrocarbon phase then provides a record of the type of interaction (simple phase equilibrium or open system Rayleigh fractionation). The tight-gas-sand reservoirs of the Rocky Mountains represent one of the most significant gas resources in the United States. The producing reservoirs are generally developed in low permeability (averaging <0.1mD) Upper Cretaceous fluvial to marginal marine sandstones and commonly form isolated overpressured reservoir bodies encased in even lower permeability muddy sediments. We present noble gas data from producing fields in the Greater Green River Basin, Wyoming; the the Piceance Basin, Colorado; and in the Uinta Basin, Utah. The data is consistent from all three basins. We show how in each basin the noble gases record open system gas migration through a water column at maximum basin burial. The data within an open system model indicates that the gas now in-place represents the last ~10% of hydrocarbon gas to have passed through the water column, most likely prior to permeability closedown.

Chromatographic separation of radioactive noble gases from xenon

NASA Astrophysics Data System (ADS)

Akerib, D. S.; Araújo, H. M.; Bai, X.; Bailey, A. J.; Balajthy, J.; Beltrame, P.; Bernard, E. P.; Bernstein, A.; Biesiadzinski, T. P.; Boulton, E. M.; Bramante, R.; Cahn, S. B.; Carmona-Benitez, M. C.; Chan, C.; Chiller, A. A.; Chiller, C.; Coffey, T.; Currie, A.; Cutter, J. E.; Davison, T. J. R.; Dobi, A.; Dobson, J. E. Y.; Druszkiewicz, E.; Edwards, B. N.; Faham, C. H.; Fiorucci, S.; Gaitskell, R. J.; Gehman, V. M.; Ghag, C.; Gibson, K. R.; Gilchriese, M. G. D.; Hall, C. R.; Hanhardt, M.; Haselschwardt, S. J.; Hertel, S. A.; Hogan, D. P.; Horn, M.; Huang, D. Q.; Ignarra, C. M.; Ihm, M.; Jacobsen, R. G.; Ji, W.; Kamdin, K.; Kazkaz, K.; Khaitan, D.; Knoche, R.; Larsen, N. A.; Lee, C.; Lenardo, B. G.; Lesko, K. T.; Lindote, A.; Lopes, M. I.; Manalaysay, A.; Mannino, R. L.; Marzioni, M. F.; McKinsey, D. N.; Mei, D.-M.; Mock, J.; Moongweluwan, M.; Morad, J. A.; Murphy, A. St. J.; Nehrkorn, C.; Nelson, H. N.; Neves, F.; O'Sullivan, K.; Oliver-Mallory, K. C.; Palladino, K. J.; Pease, E. K.; Pech, K.; Phelps, P.; Reichhart, L.; Rhyne, C.; Shaw, S.; Shutt, T. A.; Silva, C.; Solovov, V. N.; Sorensen, P.; Stephenson, S.; Sumner, T. J.; Szydagis, M.; Taylor, D. J.; Taylor, W.; Tennyson, B. P.; Terman, P. A.; Tiedt, D. R.; To, W. H.; Tripathi, M.; Tvrznikova, L.; Uvarov, S.; Verbus, J. R.; Webb, R. C.; White, J. T.; Whitis, T. J.; Witherell, M. S.; Wolfs, F. L. H.; Yazdani, K.; Young, S. K.; Zhang, C.

2018-01-01

The Large Underground Xenon (LUX) experiment operates at the Sanford Underground Research Facility to detect nuclear recoils from the hypothetical Weakly Interacting Massive Particles (WIMPs) on a liquid xenon target. Liquid xenon typically contains trace amounts of the noble radioactive isotopes 85Kr and 39Ar that are not removed by the in situ gas purification system. The decays of these isotopes at concentrations typical of research-grade xenon would be a dominant background for a WIMP search experiment. To remove these impurities from the liquid xenon, a chromatographic separation system based on adsorption on activated charcoal was built. 400 kg of xenon was processed, reducing the average concentration of krypton from 130 ppb to 3.5 ppt as measured by a cold-trap assisted mass spectroscopy system. A 50 kg batch spiked to 0.001 g/g of krypton was processed twice and reduced to an upper limit of 0.2 ppt.

Chromatographic separation of radioactive noble gases from xenon

DOE PAGES

Akerib, DS; Araújo, HM; Bai, X; ...

2017-10-31

The Large Underground Xenon (LUX) experiment operates at the Sanford Underground Research Facility to detect nuclear recoils from the hypothetical Weakly Interacting Massive Particles (WIMPs) on a liquid xenon target. Liquid xenon typically contains trace amounts of the noble radioactive isotopesmore » $$^{85}$$Kr and $$^{39}$$Ar that are not removed by the in situ gas purification system. The decays of these isotopes at concentrations typical of research-grade xenon would be a dominant background for a WIMP search exmperiment. To remove these impurities from the liquid xenon, a chromatographic separation system based on adsorption on activated charcoal was built. 400 kg of xenon was processed, reducing the average concentration of krypton from 130 ppb to 3.5 ppt as measured by a cold-trap assisted mass spectroscopy system. A 50 kg batch spiked to 0.001 g/g of krypton was processed twice and reduced to an upper limit of 0.2 ppt.« less

Optical Pumping Spin Exchange 3He Gas Cells for Magnetic Resonance Imaging

NASA Astrophysics Data System (ADS)

Kim, W.; Stepanyan, S. S.; Kim, A.; Jung, Y.; Woo, S.; Yurov, M.; Jang, J.

2009-08-01

We present a device for spin-exchange optical pumping system to produce large quantities of polarized noble gases for Magnetic Resonance Imaging (MRI). A method and design of apparatus for pumping the polarization of noble gases is described. The method and apparatus enable production, storage and usage of hyperpolarized noble gases for different purposes, including Magnetic Resonance Imaging of human and animal subjects. Magnetic imaging agents breathed into lungs can be observed by the radio waves of the MRI scanner and report back physical and functional information about lung's health and desease. The technique known as spin exchange optical pumping is used. Nuclear magnetic resonance is implemented to measure the polarization of hyperpolarized gas. The cells prepared and sealed under high vacuum after handling Alkali metals into the cell and filling with the 3He-N2 mixture. The cells could be refilled. The 3He reaches around 50% polarization in 5-15 hours.

LaRC results on nuclear pumped noble gas lasers

NASA Technical Reports Server (NTRS)

Deyoung, R. J.

1979-01-01

The recent experiment and theoretical results obtained for noble gas nuclear laser systems are presented. It is shown that the noble gas lasers are among the easiest systems to pump by nuclear excitation and as a result, all of the noble gases except He have lased under nuclear excitation. The noble gas systems are not ideal for high-power applications but they do give valuable insight into the operation and pumping mechanisms associated with nuclear lasers. At present, the Ar-Xe system is the best noble gas candidate for (U-235)F6 pumping. It appears that the quenching of Ar-Xe lasing is a result of the fluorine and not the uranium or fission fragments themselves. Thus, to achieve lasing with UF6, a fluorine compatible system must be found.

Charge state distribution of 86Kr in hydrogen and helium gas charge strippers at 2.7 MeV /nucleon

NASA Astrophysics Data System (ADS)

Kuboki, H.; Okuno, H.; Hasebe, H.; Fukunishi, N.; Ikezawa, E.; Imao, H.; Kamigaito, O.; Kase, M.

2014-12-01

The charge state distributions of krypton (86Kr) with an energy of 2.7 MeV /nucleon were measured using hydrogen (H2 ) and helium (He) gas charge strippers. A differential pumping system was constructed to confine H2 and He gases to a thickness sufficient for the charge state distributions to attain equilibrium. The mean charge states of 86Kr in H2 and He gases attained equilibrium at 25.1 and 23.2, respectively, whereas the mean charge state in N2 gas at equilibrium was estimated to be less than 20. The charge distributions are successfully reproduced by the cross sections of ionization and electron capture processes optimized by a fitting procedure.

Anomalous trapping of noble gases during sample crushing

NASA Astrophysics Data System (ADS)

Cox, S. E.; Miller, H.; Farley, K. A.; Hofmann, F.

2017-12-01

Fine-grained mineral samples are commonly analyzed for noble gas composition. Many coarse minerals contain inclusions that require that the samples be crushed and purified before analysis. Other samples are crushed because fine-grained samples may be degassed at lower temperature. And many rocks lack coarse mineral grains entirely. Protin et al. (2016) showed that crushed fine-grained olivine absorbs He from the atmosphere and retains it under heating to at least 900 degrees. We show that the act of crushing itself is responsible for the vast majority of this trapping. Samples crushed in the presence of pure He retain 25 times as much He as samples crushed in vacuum and immediately exposed to pure helium. We tested several ways to mitigate this problem, including acid leaching and crushing under a liquid. We find that crushing samples under water is the simplest, most effective way to avoid contamination with He during crushing. This approach resulted in no significant contamination of crushed fine-grained olivine, even when the submerged crushing was conducted under a headspace of pure He. Protin, M. (2016), et al. GCA 179, 76-88.

A Philippinite with an Unusually Large Bubble: Gas Pressure and Noble Gas Composition

NASA Astrophysics Data System (ADS)

Matsuda, J.; Maruoka, T.; Pinti, D. L.; Koeberl, C.

1995-09-01

. Part of the extracted gas was kept for total gas analysis, while the remainder has been purified for the noble gas measurements. Total amounts and isotopic ratios of all noble gases were measured. The amounts of Ar, Kr, and Xe close to the blank level, while those of He and Ne were about 3 to 4 orders of magnitude larger than the blank. The ^20Ne/^36Ar ratio in the bubble gas is more than 4 orders of magnitude higher than the atmospheric value, which is similar to the pattern previously observed in tektites [2,3,5]. The isotopic ratios of Ar, Kr and Xe were, within uncertainties, similar to those of the terrestrial atmosphere. However, the Ne isotopic ratios were significantly different from atmospheric values, and differ from the results reported in previous studies [2,5]. The Ne isotope data seem to lie on the mass fractionation line from the atmosphere in a ^20Ne/^22Ne vs. ^21Ne/^22Ne three isotope plot, suggesting that the Ne in the bubble has diffused in from the atmosphere. However, it is generally believed that the isotopic fractionation during a steady state is very small, and the observed Ne values are higher than those calculated from simple mass fractionation [6]. The high isotopic fractionation is likely to be associated with the non-equilibrium conditions prevailing during tektite formation. Acknowledgments: We are grateful to D. Heinlein for bringing the precious sample to our attention and for allowing its analysis. References: [1] Jessberger E. K. and Gentner W. (1972) EPSL, 14, 221-225. [2] Matsubara K. and Matsuda J. (1991) Meteoritics, 26, 217-220. [3] Matsuda J. et al. (1993) Meteoritics, 28, 586-599. [4] Maruoka T. and Matsuda J. (1995) J. Mass Spectrom. Soc. Jpn., 43, 1-8. [5] Hennecke et al. (1975) JGR, 80, 2931-2934. [6] Kaneoka I., EPSL, 48, 284-292.

Atmospheric noble gases in Mid-Ocean Ridge Basalts: Identification of atmospheric contamination processes

NASA Astrophysics Data System (ADS)

Roubinet, Claire; Moreira, Manuel A.

2018-02-01

Noble gases in oceanic basalts always show the presence in variable proportions of a component having elemental and isotopic compositions that are similar to those of the atmosphere and distinct from the mantle composition. Although this component could be mantle-derived (e.g. subduction of air or seawater-derived noble gases trapped in altered oceanic crust and sediments), it is most often suggested that this air component is added after sample collection and probably during storage at ambient air, although the mechanism remains unknown. In an attempt to reduce this atmospheric component observed in MORBs, four experimental protocols have been followed in this study. These protocols are based on the hypothesis that air can be removed from the samples, as it appears to be sheltered in distinct vesicles compared to those filled with mantle gases. All of the protocols involve a glove box filled with nitrogen, and in certain cases, the samples are stored under primary vacuum (lower than 10-2 mbar) to pump air out or, alternatively, under high pressure of N2 to expel atmospheric noble gases. In all protocols, three components are observed: atmospheric, fractionated atmospheric and magmatic. The fractionated air component seems to be derived from the non-vitreous part of the pillow-lava, which has cooled more slowly. This component is enriched in Ne relative to Ar, reflecting a diffusive process. This contaminant has already been observed in other studies and thus seems to be relatively common. Although it is less visible, unfractionated air has also been detected in some crushing steps, which tends to indicate that despite the experiments, air is still present in the vesicles. This result is surprising, since studies have demonstrated that atmospheric contamination could be limited if samples were stored under nitrogen quickly after their recovery from the seafloor. Thus, the failure of the protocols could be explained by the insufficient duration of these protocols or

Laser microprobe analyses of noble gas isotopes and halogens in fluid inclusions: Analyses of microstandards and synthetic inclusions in quartz

USGS Publications Warehouse

Böhlke, J.K.; Irwin, J.J.

1992-01-01

Ar, Kr, Xe, Cl, Br, I, and K abundances and isotopic compositions have been measured in microscopic fluid inclusions in minerals by noble gas mass spectrometry following neutron irradiation and laser extraction. The laser microprobe noble gas mass spectrometric (LMNGMS) technique was quantified by use of microstandards, including air-filled capillary tubes, synthetic basalt glass grains, standard hornblende grains, and synthetic fluid inclusions in quartz. Common natural concentrations of halogens (Cl, Br, and I) and noble gases (Ar and Kr) in trapped groundwaters and hydrothermal fluids can be analyzed simultaneously by LMNGMS in as little as 10−11 L of inclusion fluid, with accuracy and precision to within 5–10% for element and isotope ratios. Multicomponent element and isotope correlations indicate contaminants or persistent reservoirs of excess Xe and/or unfractionated air in some synthetic and natural fluid inclusion samples. LMNGMS analyses of natural fluid inclusions using the methods and calibrations reported here may be used to obtain unique information on sources of fluids, sources of fluid salinity, mixing, boiling (or unmixing), and water-rock interactions in ancient fluid flow systems.

Silicon PIN diode based electron-gamma coincidence detector system for Noble Gases monitoring.

PubMed

Khrustalev, K; Popov, V Yu; Popov, Yu S

2017-08-01

We present a new second generation SiPIN based electron-photon coincidence detector system developed by Lares Ltd. for use in the Noble Gas measurement systems of the International Monitoring System and the On-site Inspection verification regimes of the Comprehensive Nuclear-Test Ban Treaty (CTBT). The SiPIN provide superior energy resolution for electrons. Our work describes the improvements made in the second generation detector cells and the potential use of such detector systems for other applications such as In-Situ Kr-85 measurements for non-proliferation purposes. Copyright © 2017 Elsevier Ltd. All rights reserved.

Using noble gases and 87Sr/86Sr to constrain heat sources and fluid evolution at the Los Azufres Geothermal Field, Mexico

NASA Astrophysics Data System (ADS)

Wen, T.; Pinti, D. L.; Castro, M. C.; Lopez Hernandez, A.; Hall, C. M.; Shouakar-Stash, O.; Sandoval-Medina, F.

2017-12-01

Geothermal wells and hot springs were sampled for noble gases' volume fraction and isotopic measurements and 87Sr/86Sr in the Los Azufres Geothermal Field (LAGF), Mexico, to understand the evolution of fluid circulation following three decades of exploitation and re-injection of used brines. The LAGF, divided into the Southern Production Zone (SPZ) and the Northern Production Zone (NPZ), is hosted in a Miocene to Pliocene andesitic volcanic complex covered by Quaternary rhyolitic-dacitic units. Air contamination corrected 3He/4He ratios (Rc) normalized to the atmospheric ratio (Ra=1.384 x 10-6), show a median value of 6.58 indicating a dominant mantle helium component. Contributions of crustal helium up to 53% and 18% are observed in NPZ and SPZ, respectively. Observations based on Rc/Ra and 87Sr/86Sr ratios points to the mixing of three magmatic sources supplying mantle helium to the LAGF: (1) a pure mantle He (Rc/Ra = 8) and Sr (87Sr/86Sr = 0.7035) source; (2) a pure mantle helium (Rc/Ra = 8) with some radiogenic Sr (87Sr/86Sr = 0.7049) source possibly resulting from Quaternary rhyolitic volcanism; and (3) a fossil mantle He component (Rc/Ra = 3.8) with some radiogenic Sr (87Sr/86Sr = 0.7038), corresponding possibly to the Miocene andesite reservoir. Intrusions within the last 50 kyrs from sources (1) and (2) are likely responsible for the addition of mantle volatiles and heat to the hydrothermal system of Los Azufres. He and Ar isotopes indicate that heat flow is transported by both convection and conduction. Atmospheric noble gas elemental ratios suggest that geothermal wells located closer to the western re-injection zone are beginning to be dominated by re-injection of used brines (injectate). The area affected by boiling in LAGF has further extended to the north and west since the last noble gas sampling campaign in 2009.

Biomedical Investigations with Laser-Polarized Noble Gas Magnetic Resonance

NASA Technical Reports Server (NTRS)

Walsworth, Ronald L.

2003-01-01

We pursued advanced technology development of laser-polarized noble gas nuclear magnetic resonance (NMR) as a novel biomedical imaging tool for ground-based and eventually space-based application. This new multidisciplinary technology enables high-resolution gas-space magnetic resonance imaging (MRI)-e.g., of lung ventilation-as well as studies of tissue perfusion. In addition, laser-polarized noble gases (3He and 129Xe) do not require a large magnetic field for sensitive detection, opening the door to practical MRI at very low magnetic fields with an open, lightweight, and low-power device. We pursued two technology development specific aims: (1) development of low-field (less than 0.01 T) noble gas MRI of humans; and (2) development of functional MRI of the lung using laser-polarized noble gas and related techniques.

Rapid processing of 85Kr/Kr ratios using Atom Trap Trace Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zappala, J. C.; Bailey, K.; Mueller, P.

In this paper, we report a methodology for measuring 85Kr/Kr isotopic abundances using Atom Trap Trace Analysis (ATTA) that increases sample measurement throughput by over an order of magnitude to six samples per 24 h. The noble gas isotope 85Kr (half-life = 10.7 years) is a useful tracer for young groundwater in the age range of 5–50 years. ATTA, an efficient and selective laser-based atom counting method, has recently been applied to 85Kr/Kr isotopic abundance measurements, requiring 5–10 μL of krypton gas at STP extracted from 50 to 100 L of water. Previously, a single such measurement required 48 h.more » In conclusion, our new method demonstrates that we can measure 85Kr/Kr ratios with 3–5% relative uncertainty every 4 h, on average, with the same sample requirements.« less

Rapid processing of 85Kr/Kr ratios using Atom Trap Trace Analysis

DOE PAGES

Zappala, J. C.; Bailey, K.; Mueller, P.; ...

2017-03-11

In this paper, we report a methodology for measuring 85Kr/Kr isotopic abundances using Atom Trap Trace Analysis (ATTA) that increases sample measurement throughput by over an order of magnitude to six samples per 24 h. The noble gas isotope 85Kr (half-life = 10.7 years) is a useful tracer for young groundwater in the age range of 5–50 years. ATTA, an efficient and selective laser-based atom counting method, has recently been applied to 85Kr/Kr isotopic abundance measurements, requiring 5–10 μL of krypton gas at STP extracted from 50 to 100 L of water. Previously, a single such measurement required 48 h.more » In conclusion, our new method demonstrates that we can measure 85Kr/Kr ratios with 3–5% relative uncertainty every 4 h, on average, with the same sample requirements.« less

Subsurface dynamics of reactive and inert gases in the context of noble gases as environmental tracers in groundwater hydrology

NASA Astrophysics Data System (ADS)

Mayer, Simon; Jenner, Florian; Aeschbach, Werner

2017-04-01

Applications of inert gases in groundwater hydrology require a profound understanding of underlying biogeochemical processes. Some of these processes are, however, not well understood and therefore require further investigation. This is the first study simultaneously investigating soil air and groundwater in the context of noble gas tracer applications, accounting for seasonal effects in different climate regions. The sampled data confirm a general reliability of common assumptions proposed in the literature. In particular, a solubility-controlled description of excess air formation and of groundwater degassing can be confirmed. This study identifies certain effects which need to be taken into account to reliably evaluate noble gas patterns. First, long-term samplings suggest a permanent temperature-driven equilibration of shallow groundwater with entrapped air bubbles, even some years after recharge. Second, minor groundwater degassing is found to challenge existing excess air model approaches, depending on the amount and the fractionation of excess air. Third, soil air composition data of this study imply a potential bias of noble gas temperatures by up to about 2℃ due to microbial oxygen depletion and a reduced sum value of O2+CO2. This effect causes systematically lower noble gas temperatures in tropical groundwater samples and in shallow mid-latitude groundwater samples after strong recharge during the warm season. However, a general bias of noble gas temperatures in mid-latitudes is probably prevented by a predominant recharge during the cold season, accompanied by nearly atmospheric noble gas mixing ratios in the soil air. Findings of this study provide a remarkable contribution to the reliability of noble gas tracer applications in hydrology, in particular with regard to paleoclimate reconstructions and an understanding of subsurface gas dynamics.

Tracing ancient hydrogeological fracture network age and compartmentalisation using noble gases

NASA Astrophysics Data System (ADS)

Warr, Oliver; Sherwood Lollar, Barbara; Fellowes, Jonathan; Sutcliffe, Chelsea N.; McDermott, Jill M.; Holland, Greg; Mabry, Jennifer C.; Ballentine, Christopher J.

2018-02-01

We show that fluid volumes residing within the Precambrian crystalline basement account for ca 30% of the total groundwater inventory of the Earth (> 30 million km3). The residence times and scientific importance of this groundwater are only now receiving attention with ancient fracture fluids identified in Canada and South Africa showing: (1) microbial life which has existed in isolation for millions of years; (2) significant hydrogen and hydrocarbon production via water-rock reactions; and (3) preserving noble gas components from the early atmosphere. Noble gas (He, Ne, Ar, Kr, Xe) abundance and isotopic compositions provide the primary evidence for fluid mean residence time (MRT). Here we extend the noble gas data from the Kidd Creek Mine in Timmins Ontario Canada, a volcanogenic massive sulfide (VMS) deposit formed at 2.7 Ga, in which fracture fluids with MRTs of 1.1-1.7 Ga were identified at 2.4 km depth (Holland et al., 2013); to fracture fluids at 2.9 km depth. We compare here the Kidd Creek Mine study with noble gas compositions determined in fracture fluids taken from two mines (Mine 1 & Mine 2) at 1.7 and 1.4 km depth below surface in the Sudbury Basin formed by a meteorite impact at 1.849 Ga. The 2.9 km samples at Kidd Creek Mine show the highest radiogenic isotopic ratios observed to date in free fluids (e.g. 21Ne/22Ne = 0.6 and 40Ar/36Ar = 102,000) and have MRTs of 1.0-2.2 Ga. In contrast, resampled 2.4 km fluids indicated a less ancient MRT (0.2-0.6 Ga) compared with the previous study (1.1-1.7 Ga). This is consistent with a change in the age distribution of fluids feeding the fractures as they drain, with a decreasing proportion of the most ancient end-member fluids. 129Xe/136Xe ratios for these fluids confirm that boreholes at 2.4 km versus 2.9 km are sourced from hydrogeologically distinct systems. In contrast, results for the Sudbury mines have MRTs of 0.2-0.6 and 0.2-0.9 Ga for Mines 1 and 2 respectively. While still old compared to almost all

On Noble Gas Processing in the Solar Accretion Disk

NASA Astrophysics Data System (ADS)

Pepin, R. O.

2003-04-01

generate fractionated Xe, Kr, Ar and Ne compositions in the residual atmosphere that closely match observed meteoritic isotopic distributions, and Q-gas elemental ratios are approximated by adsorption of fractionated gases on planetesimal surface grains using plausible values of relative Henry Law constants. Additional requirements for adsorption of sufficient absolute amounts of Q-gases on carrier grains, and their subsequent ejection to space, mixing in the nebula, and dispersal into meteorite bodies, are examined in the context of current models for body sizes and dynamical evolution in an early mass-rich asteroid belt (Chambers and Wetherill, 2001). Despite its ability to replicate isotopic compositions, uncertainties about the environments in which the blowoff model can successfully operate suggest that there is, as yet, no entirely satisfactory understanding of how the Q-component noble gases might have evolved from solar-like precursor compositions.

Carbon atom and cluster sputtering under low-energy noble gas plasma bombardment

NASA Astrophysics Data System (ADS)

Oyarzabal, E.; Doerner, R. P.; Shimada, M.; Tynan, G. R.

2008-08-01

Exit-angle resolved carbon atom and cluster (C2 and C3) sputtering yields are measured during different noble gas (Xe, Kr, Ar, Ne, and He) ion bombardments from a plasma, for low incident energies (75-225 eV). A quadrupole mass spectrometer (QMS) is used to detect the fraction of sputtered neutrals that is ionized in the plasma and to obtain the angular distribution by changing the angle between the target normal and the QMS aperture. A one-dimensional Monte Carlo code is used to simulate the interaction of the plasma and the sputtered particles in the region between the sample and the QMS. The effective elastic scattering cross sections of C, C2, and C3 with the different bombarding gas neutrals are obtained by varying the distance between the sample and the QMS and by performing a best fit of the simulation results to the experimental results. The total sputtering yield (C+C2+C3) for each bombarding gas is obtained from weight-loss measurements and the sputtering yield for C, C2, and C3 is then calculated from the integration of the measured angular distribution, taking into account the scattering and ionization of the sputtered particles between the sample and the QMS. We observe undercosine angular distributions of the sputtered atoms and clusters for all the studied bombarding gases and a clear decrease of the atom to cluster (C2 and C3) sputtering ratio as the incident ion mass increases, changing from a carbon atom preferential erosion for the lower incident ion masses (He, Ne, and Ar) to a cluster preferential erosion for the higher incident ion masses (Kr and Xe).

Noble gas models of mantle structure and reservoir mass transfer

NASA Astrophysics Data System (ADS)

Harrison, Darrell; Ballentine, Chris J.

Noble gas observations from different mantle samples have provided some of the key observational data used to develop and support the geochemical "layered" mantle model. This model has dominated our conceptual understanding of mantle structure and evolution for the last quarter of a century. Refinement in seismic tomography and numerical models of mantle convection have clearly shown that geochemical layering, at least at the 670 km phase change in the mantle, is no longer tenable. Recent adaptations of the mantle-layering model that more successfully reconcile whole-mantle convection with the simplest data have two common features: (i) the requirement for the noble gases in the convecting mantle to be sourced, or "fluxed", by a deep long-lived volatile-rich mantle reservoir; and (ii) the requirement for the deep mantle reservoirs to be seismically invisible. The fluxing requirement is derived from the low mid-ocean ridge basalt (MORB)-source mantle 3He concentration, in turn calculated from the present day 3He flux from mid-ocean ridges into the oceans (T½ ˜ 1,000 yr) and the ocean crust generation rate (T½ ˜ 108 yr). Because of these very different residence times we consider the 3He concentration constraint to be weak. Furthermore, data show 3He/22Ne ratios derived from different mantle reservoirs to be distinct and require additional complexities to be added to any model advocating fluxing of the convecting mantle from a volatile-rich mantle reservoir. Recent work also shows that the convecting mantle 20Ne/22Ne isotopic composition is derived from an implanted meteoritic source and is distinct from at least one plume source system. If Ne isotope heterogeneity between convecting mantle and plume source mantle is confirmed, this result then excludes all mantle fluxing models. While isotopic heterogeneity requires further quantification, it has been shown that higher 3He concentrations in the convecting mantle, by a factor of 3.5, remove the need for the noble

Size versus polarizability in protein-ligand interactions: binding of noble gases within engineered cavities in phage T4 lysozyme.

PubMed

Quillin, M L; Breyer, W A; Griswold, I J; Matthews, B W

2000-09-29

To investigate the relative importance of size and polarizability in ligand binding within proteins, we have determined the crystal structures of pseudo wild-type and cavity-containing mutant phage T4 lysozymes in the presence of argon, krypton, and xenon. These proteins provide a representative sample of predominantly apolar cavities of varying size and shape. Even though the volumes of these cavities range up to the equivalent of five xenon atoms, the noble gases bind preferentially at highly localized sites that appear to be defined by constrictions in the walls of the cavities, coupled with the relatively large radii of the noble gases. The cavities within pseudo wild-type and L121A lysozymes each bind only a single atom of noble gas, while the cavities within mutants L133A and F153A have two independent binding sites, and the L99A cavity has three interacting sites. The binding of noble gases within two double mutants was studied to characterize the additivity of binding at such sites. In general, when a cavity in a protein is created by a "large-to-small" substitution, the surrounding residues relax somewhat to reduce the volume of the cavity. The binding of xenon and, to a lesser degree, krypton and argon, tend to expand the volume of the cavity and to return it closer to what it would have been had no relaxation occurred. In nearly all cases, the extent of binding of the noble gases follows the trend xenon>krypton>argon. Pressure titrations of the L99A mutant have confirmed that the crystallographic occupancies accurately reflect fractional saturation of the binding sites. The trend in noble gas affinity can be understood in terms of the effects of size and polarizability on the intermolecular potential. The plasticity of the protein matrix permits repulsion due to increased ligand size to be more than compensated for by attraction due to increased ligand polarizability. These results have implications for the mechanism of general anesthesia, the migration

3c/4e [small sigma, Greek, circumflex]-type long-bonding competes with ω-bonding in noble-gas hydrides HNgY (Ng = He, Ne, Ar, Kr, Xe, Rn; Y = F, Cl, Br, I): a NBO/NRT perspective.

PubMed

Zhang, Guiqiu; Li, Hong; Weinhold, Frank; Chen, Dezhan

2016-03-21

Noble-gas hydrides HNgY are frequently described as a single ionic form (H-Ng)(+)Y(-). We apply natural bond orbital (NBO) and natural resonance theory (NRT) analyses to a series of noble-gas hydrides HNgY (Ng = He, Ne, Ar, Kr, Xe, Rn; Y = F, Cl, Br, I) to gain quantitative insight into the resonance bonding of these hypervalent molecules. We find that each of the studied species should be better represented as a resonance hybrid of three leading resonance structures, namely, H-Ng(+ -):Y (I), H:(- +)Ng-Y (II), and H^Y (III), in which the "ω-bonded" structures I and II arise from the complementary donor-acceptor interactions nY → σ*HNg and nH → σ*NgY, while the "long-bond" ([small sigma, Greek, circumflex]-type) structure III arises from the nNg → [small sigma, Greek, circumflex]*HY/[small sigma, Greek, circumflex]HY interaction. The bonding for all of the studied molecules can be well described in terms of the continuously variable resonance weightings of 3c/4e ω-bonding and [small sigma, Greek, circumflex]-type long-bonding motifs. Furthermore, we find that the calculated bond orders satisfy a generalized form of "conservation of bond order" that incorporates both ω-bonding and long-bonding contributions [viz., (bHNg + bNgY) + bHY = bω-bonding + blong-bonding = 1]. Such "conservation" throughout the title series implies a competitive relationship between ω-bonding and [small sigma, Greek, circumflex]-type long-bonding, whose variations are found to depend in a chemically reasonable manner on the electronegativity of Y and the outer valence-shell character of the central Ng atom. The calculated bond orders are also found to exhibit chemically reasonable correlations with bond lengths, vibrational frequencies, and bond dissociation energies, in accord with Badger's rule and related empirical relationships. Overall, the results provide electronic principles and chemical insight that may prove useful in the rational design of noble-gas hydrides of

Noble Gas Signatures in Groundwater and Rainwater on the Island of Maui, Hawaii - Developing a New Noble Gas Application in Fractured, Volcanic Systems

NASA Astrophysics Data System (ADS)

Castro, M. C.; Niu, Y.; Warrier, R. B.; Hall, C. M.; Gingerich, S. B.; Scholl, M. A.; Bouvier, L.

2014-12-01

Recent work in the Galapagos Islands suggests that noble gas temperatures (NGTs) in fractured groundwater systems reflect the temperature of the ground surface at the time of infiltration rather than the mean annual air temperature (MAAT) value as commonly assumed in sedimentary systems where NGTs are typically used as indicators of past climate. This suggests that noble gases in fractured areas may record seasonality, and thus, provide information about timing of recharge in addition to location. Calculation of NGTs assumes that rain-derived recharge at the water table is in equilibrium with ground air. Lack of noble gas equilibration with respect to surface conditions, however, was observed in high-altitude springs in the Galapagos Islands and in a rainwater pilot study in Michigan, supporting the NGT seasonality hypothesis. Developing this new NGT application will lead to a better understanding of fractured groundwater flow systems and will contribute to improved water resource management plans. This study, carried out on Maui, Hawaii, is meant to test these hypotheses while improving knowledge of this island's groundwater flow system where limited hydrologic data are available. Here, we present the first results of noble gas analyses from samples collected in springs, groundwater wells and rainwater on northeast Maui. Results show that like most Michigan rainwater samples, rainwater from Maui is in disequilibrium with surface conditions and follows a mass-dependent pattern. Spring samples follow a similar pattern to that of rainwater and suggest that spring water originates directly from rainfall. These findings further support the hypothesis of NGT seasonality. However, while the atmospheric composition of noble gases points to direct supply from rainfall to spring aquifer systems, a direct connection between spring water and deeper aquifer levels or the mantle is apparent from He isotopic ratios which display an almost pure He mantle component in some springs.

Shock Compression of Liquid Noble Gases to Multi-Mbar Pressures

NASA Astrophysics Data System (ADS)

Root, Seth

2011-10-01

The high pressure - high temperature behavior of noble gases is of considerable interest because of their use in z-pinch liners for fusion studies and for understanding astrophysical and planetary evolution. However, our understanding of the equation of state (EOS) of the noble gases at extreme conditions is limited. A prime example of this is the liquid xenon Hugoniot. Previous EOS models rapidly diverged on the Hugoniot above 1 Mbar because of differences in the treatment of the electronic contribution to the free energy. Similar divergences are observed for krypton EOS. Combining shock compression experiments and density functional theory (DFT) simulations, we can determine the thermo-physical behavior of matter under extreme conditions. The experimental and DFT results have been instrumental to recent developments in planetary astrophysics and inertial confinement fusion. Shock compression experiments are performed using Sandia's Z-Accelerator to determine the Hugoniot of liquid xenon and krypton in the Mbar regime. Under strong pressure, krypton and xenon undergo an insulator to metal transition. In the metallic state, the shock front becomes reflective allowing for a direct measurement of the sample's shock velocity using laser interferometry. The Hugoniot state is determined using a Monte Carlo analysis method that accounts for systematic error in the standards and for correlations. DFT simulations at these extreme conditions show good agreement with the experimental data - demonstrating the attention to detail required for dealing with elements with relativistic core states and d-state electrons. The results from shock compression experiments and DFT simulations are presented for liquid xenon to 840 GPa and for liquid krypton to 800 GPa, decidedly increasing the range of known behavior of both gases. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Company

Assessing the use of 3H-3He dating to determine the subsurface transit time of cave drip waters.

PubMed

Kluge, Tobias; Wieser, Martin; Aeschbach-Hertig, Werner

2010-09-01

(3)H-(3)He measurements constitute a well-established method for the determination of the residence time of young groundwater. However, this method has rarely been applied to karstified aquifers and in particular to drip water in caves, despite the importance of the information which may be obtained. Besides the determination of transfer times of climate signals from the atmosphere through the epikarst to speleothems as climate archives, (3)H-(3)He together with Ne, Ar, Kr, Xe data may also help to give new insights into the local hydrogeology, e.g. the possible existence of a perched aquifer above a cave. In order to check the applicability of (3)H-(3)He dating to cave drips, we collected drip water samples from three adjacent caves in northwestern Germany during several campaigns. The noble gas data were evaluated by inverse modelling to obtain recharge temperature and excess air, supporting the calculation of the tritiogenic (3)He and hence the (3)H-(3)He age. Although atmospheric noble gases were often found to be close to equilibrium with the cave atmosphere, several drip water samples yielded an elevated (3)He/(4)He ratio, providing evidence for the accumulation of (3)He from the decay of (3)H. No significant contribution of radiogenic (4)He was found, corresponding to the low residence times mostly in the range of one to three years. Despite complications during sampling, conditions of a perched aquifer could be confirmed by replicate samples at one drip site. Here, the excess air indicator ΔNe was about 10 %, comparable to typical values found in aquifers in mid-latitudes. The mean (3)H-(3)He age of 2.1 years at this site presumably refers to the residence time in the perched aquifer and is lower than the entire transit time of 3.4 years estimated from the tritium data.

Prediction of neutral noble gas insertion compounds with heavier pnictides: FNgY (Ng = Kr and Xe; Y = As, Sb and Bi).

PubMed

Ghosh, Ayan; Manna, Debashree; Ghanty, Tapan K

2016-04-28

A novel class of interesting insertion compounds obtained through the insertion of a noble gas atom into the heavier pnictides have been explored by various ab initio quantum chemical techniques. Recently, the first neutral noble gas insertion compounds, FXeY (Y = P, N), were theoretically predicted to be stable; the triplet state was found to be the most stable state, with a high triplet-singlet energy gap, by our group. In this study, we investigated another noble gas inserted compound, FNgY (Ng = Kr and Xe; Y = As, Sb and Bi), with a triplet ground state. Density functional theory (DFT), second order Møller-Plesset perturbation theory (MP2), coupled-cluster theory (CCSD(T)) and multi-reference configuration interaction (MRCI) based techniques have been utilized to investigate the structures, stabilities, harmonic vibrational frequencies, charge distributions and topological properties of these compounds. These predicted species, FNgY (Ng = Kr and Xe; Y = As, Sb and Bi) are found to be energetically stable with respect to all the probable 2-body and 3-body dissociation pathways, except for the 2-body channel leading to the global minimum products (FY + Ng). Nevertheless, the finite barrier height corresponding to the saddle points of the compounds connected to their respective global minima products indicates that these compounds are kinetically stable. The structural parameters, energetics, and charge distribution results as well as atoms-in-molecules (AIM) analysis suggest that these predicted molecules can be best represented as F(-)[(3)NgY](+). Thus, all the aforementioned computed results clearly indicate that it may be possible to experimentally prepare the most stable triplet state of FNgY molecules under cryogenic conditions through a matrix isolation technique.

Revealing the magmas degassing below closed-conduit active volcanoes: noble gases in volcanic rocks versus fumarolic fluids at Vulcano (Aeolian Islands, Italy)

NASA Astrophysics Data System (ADS)

Mandarano, Michela; Paonita, Antonio; Martelli, Mauro; Viccaro, Marco; Nicotra, Eugenio; Millar, Ian L.

2016-04-01

With the aim to constrain the nature of magma currently feeding the fumarolic field of Vulcano, we measured the elemental and isotopic compositions of noble gases (He, Ne, and Ar) in olivine- and clinopyroxene-hosted fluid inclusions in high-K calcalcaline-shoshonitic and shoshonitic-potassic series so as to cover the entire volcanological history of Vulcano Island (Italy). The major and trace-element concentrations and the Sr- and Pb-isotope compositions for whole rocks were integrated with data obtained from the fluid inclusions. 3He/4He in fluid inclusions is within the range of 3.30 and 5.94 R/Ra, being lower than the value for the deep magmatic source expected for Vulcano Island (6.0-6.2 R/Ra). 3He/4He of the magmatic source is almost constant throughout the volcanic record of Vulcano. Integration of the He- and Sr-isotope systematics leads to the conclusion that a decrease in the He-isotope ratio of the rocks is mainly due to the assimilation of 10-25% of a crustal component similar to the Calabrian basement. 3He/4He shows a negative correlation with Sr isotopes except for the last-emitted Vulcanello latites (Punta del Roveto), which have high He- and Sr-isotope ratios. This anomaly has been attributed to a flushing process by fluids coming from the deepest reservoirs. Indeed, an input of deep magmatic volatiles with high 3He/4He values increases the He-isotope ratio without changing 87Sr/86Sr. A comparison of the He isotope ratios between fluid inclusions and fumarolic gases showed that only the basalts of La Sommata and the latites of Vulcanello have comparable values. Taking into account that the latites of Vulcanello relate to one of the most-recent eruptions at Vulcano (in the 17th century), we infer that that the most probable magma which actually feeds the fumarolic emissions is a latitic body ponding at about 3-3.5 km of depth and flushed by fluids coming from a deeper and basic magma.

Noble-gas-rich separates from the Allende meteorite

NASA Technical Reports Server (NTRS)

Ott, U.; Mack, R.; Chang, S.

1981-01-01

Predominantly carbonaceous HF/HCl-resistant residues from the Allende meteorite are studied. Samples are characterized by SEM/EDXA, X-ray diffraction, INAA, C, S, H, N, and noble gas analyses. Isotopic data for carbon show variations no greater than 5%, while isotopic data from noble gases confirm previously established systematics. Noble gas abundances correlate with those of C and N, and concomitant partial loss of C and normal trapped gas occur during treatments with oxidizing acids. HF/HCl demineralization of bulk meteorite results in similar fractional losses of C and trapped noble gases, which leads to the conclusion that various macromolecular carbonaceous substances serve as the main host phase for normal trapped noble gases and anomalous gases in acid-resistant residues, and as the carrier of the major part of trapped noble gases lost during HF/HCl demineralization. Limits on the possible abundances of dense mineralic host phases in the residues are obtained, and considerations of the nucleogenetic origin for CCF-XE indicate that carbonaceous host phases and various forms of organic matter in carbonaceous meteorites may have a presolar origin.

Exploring the deep, ancient hydrogeosphere within Precambrian crystalline rocks using noble gases

NASA Astrophysics Data System (ADS)

Warr, O.; Sherwood Lollar, B.; Fellowes, J.; Sutcliffe, C. N.; McDermott, J. M.; Holland, G.; Mabry, J.; Ballentine, C. J.

2016-12-01

Serpentinization is a key long-term water-rock interaction occurring within isolated fractures in Precambrian crystalline rocks and is a significant source of global H2 production. Highly saline fracture fluids, containing in-situ produced dissolved gases (e.g. percent level He, abiogenic CH4 and mM H2), have revealed microbial ecosystems isolated from the surface photosphere for millions of years. Noble gases can provide crucial physical and temporal constraints on these serpentinizing and life-supporting environments via radiogenic-derived fluid residence times, while also providing evidence of isolation. New noble gas data is presented here from four locations on the Canadian Shield. Kidd Creek Mine in Ontario, where fluids with a mean residence time ≥ 1.1 Ga were identified in 2013, was revisited with resampling of the waters from 2.4 km bls (below land surface), and new samples collected from 2.9 km bls. The study was also expanded to include two mines from Sudbury, Ontario at 1.7 (Mine 1) and 1.4 (Mine 2) km bls. The radiogenic excesses within the fluids were greatest for the 2.9 km Kidd Creek samples and provided an average residence time of 1.6 Ga. Consistent with our hypothesis, the resampling of the 2.4 km fluids (80 months after the original study) reveal significantly reduced residence times (1.1 Ga to 390 Ma) due to stress-induced opening of younger, though nonetheless old, fractures. This is supported by recent sulphur isotope, and 2H & 18O data. Additional hydrogeological constraints are provided by the 129Xe & 136Xe data, which suggest distinct fracture networks feed the 2.4 km, and the 2.9 km systems. Fracture fluids in the Sudbury Basin were targeted to investigate the influence of a later 1.8 Ga bolide impact which formed major fractures in the underlying basement. As hypothesised the fluids in the Sudbury Archean basement are younger than those at Kidd Creek, with mean residence times of 313 and 544 Ma for Mine 1 and 2 respectively. Our

Neutron detection by scintillation of noble-gas excimers

NASA Astrophysics Data System (ADS)

McComb, Jacob Collin

Neutron detection is a technique essential to homeland security, nuclear reactor instrumentation, neutron diffraction science, oil-well logging, particle physics and radiation safety. The current shortage of helium-3, the neutron absorber used in most gas-filled proportional counters, has created a strong incentive to develop alternate methods of neutron detection. Excimer-based neutron detection (END) provides an alternative with many attractive properties. Like proportional counters, END relies on the conversion of a neutron into energetic charged particles, through an exothermic capture reaction with a neutron absorbing nucleus (10B, 6Li, 3He). As charged particles from these reactions lose energy in a surrounding gas, they cause electron excitation and ionization. Whereas most gas-filled detectors collect ionized charge to form a signal, END depends on the formation of diatomic noble-gas excimers (Ar*2, Kr*2,Xe* 2) . Upon decaying, excimers emit far-ultraviolet (FUV) photons, which may be collected by a photomultiplier tube or other photon detector. This phenomenon provides a means of neutron detection with a number of advantages over traditional methods. This thesis investigates excimer scintillation yield from the heavy noble gases following the boron-neutron capture reaction in 10B thin-film targets. Additionally, the thesis examines noble-gas excimer lifetimes with relationship to gas type and gas pressure. Experimental data were collected both at the National Institute of Standards and Technology (NIST) Center for Neutron Research, and on a newly developed neutron beamline at the Maryland University Training Reactor. The components of the experiment were calibrated at NIST and the University of Maryland, using FUV synchrotron radiation, neutron imaging, and foil activation techniques, among others. Computer modeling was employed to simulate charged-particle transport and excimer photon emission within the experimental apparatus. The observed excimer

Opacity and conductivity measurements in noble gases at conditions of planetary and stellar interiors

PubMed Central

McWilliams, R. Stewart; Dalton, D. Allen; Konôpková, Zuzana; Mahmood, Mohammad F.; Goncharov, Alexander F.

2015-01-01

The noble gases are elements of broad importance across science and technology and are primary constituents of planetary and stellar atmospheres, where they segregate into droplets or layers that affect the thermal, chemical, and structural evolution of their host body. We have measured the optical properties of noble gases at relevant high pressures and temperatures in the laser-heated diamond anvil cell, observing insulator-to-conductor transformations in dense helium, neon, argon, and xenon at 4,000–15,000 K and pressures of 15–52 GPa. The thermal activation and frequency dependence of conduction reveal an optical character dominated by electrons of low mobility, as in an amorphous semiconductor or poor metal, rather than free electrons as is often assumed for such wide band gap insulators at high temperatures. White dwarf stars having helium outer atmospheres cool slower and may have different color than if atmospheric opacity were controlled by free electrons. Helium rain in Jupiter and Saturn becomes conducting at conditions well correlated with its increased solubility in metallic hydrogen, whereas a deep layer of insulating neon may inhibit core erosion in Saturn. PMID:26080401

Opacity and conductivity measurements in noble gases at conditions of planetary and stellar interiors

DOE PAGES

McWilliams, R. Stewart; Dalton, D. Allen; Konopkova, Zuzana; ...

2015-06-16

The noble gases are elements of broad importance across science and technology, and are primary constituents of planetary and stellar atmospheres, where they segregate into droplets or layers that affect the thermal, chemical, and structural evolution of their host body. We have measured the optical properties of noble gases at relevant high pressures and temperatures in the laser-heated diamond anvil cell, observing insulator-to-conductor transformations in dense helium, neon, argon, and xenon at 4,000 to 15,000 K and pressures of 15-52 GPa. The thermal activation and frequency-dependence of conduction reveal an optical character dominated by electrons of low mobility, as inmore » an amorphous semiconductor or poor metal, rather than free electrons as is often assumed for such wide band gap insulators at high temperatures. White dwarf stars having helium outer atmospheres cool slower and may have different color than if atmospheric opacity were controlled by free-electrons. As a result, helium rain in Jupiter and Saturn becomes conducting at conditions well correlated with increased solubility in metallic hydrogen, while a deep layer of insulating neon may inhibit core erosion in Saturn.« less

Inert gases in Sea of Fertility regolith

NASA Technical Reports Server (NTRS)

Vinogradov, A. P.; Zadorozhnyy, I. K.

1974-01-01

The content and isotopic composition were studied of inert gases -- He, Ne, Ar, Kr, and Xe -- in samples of lunar regolith returned by the Luna 16 automatic station. The samples were taken from depths of about 12 and 30 cm. The high concentrations of inert gases exceed by several orders their concentrations observed in ordinary stony meteorites. The gases in lunar regolith were a complex mixture of gases of different origins: Solar, cosmogenic, radiogenic, and so on. Solar wind gases predominated, distributed in the thin surficial layer of the regolith grains. The concentrations of these gases in the surficial layer is several cubic centimeters per gram. The isotopic composition of the inert gases of solar origin approaches their composition measured in gas-rich meteorites.

Extraction of Solar Wind Nitrogen and Noble Gases From the Genesis Gold Foil Collector

NASA Astrophysics Data System (ADS)

Schlutter, D. J.; Pepin, R. O.

2005-12-01

The Genesis gold foil is a bulk solar wind collector, integrating fluences from all three of the wind regimes. Pyrolytic extraction of small foil samples at Minnesota yielded He fluences, corrected for backscatter, in good agreement with measurements by on-board spacecraft instruments, and He/Ne elemental ratios close to those implanted in collector foils deployed on the lunar surface during the Apollo missions. Isotopic distributions of He, Ne and Ar are under study. Pyrolysis to temperatures above the gold melting point generates nitrogen blanks large enough to obscure the solar-wind nitrogen component. An alternative technique for nitrogen and noble gas extraction, by room-temperature amalgamation of the gold foil surface, will be discussed. Ne and Ar releases in preliminary tests of this technique on small foil samples were close to 100% of the amounts expected from the high-temperature pyrolysis yields, indicating that amalgamation quantitatively liberates gases from several hundred angstroms deep in the gold, beyond the implantation depth of most of the solar wind. Present work is focused on two problems currently interfering with accurate nitrogen measurements at the required picogram to sub-picogram levels: a higher than expected blank likely due to tiny air bubbles rolled into the gold sheet during fabrication, and the presence of a refractory hydrocarbon film on Genesis collector surfaces (the "brown stain") that, if left in place on the foil, shields the underlying gold from mercury attack. We have found, however, that the film is efficiently removed within tens of seconds by oxygen plasma ashing. Potential nitrogen contaminants introduced during the crash of the sample return canister are inert in amalgamation, and so are not hazards to the measurements.

Photosensitive dopants for liquid noble gases

DOEpatents

Anderson, David F.

1988-01-01

In an ionization type detector for high energy radiation wherein the energy of incident radiation is absorbed through the ionization of a liquid noble gas and resulting free charge is collected to form a signal indicative of the energy of the incident radiation, an improvement comprising doping the liquid noble gas with photosensitive molecules to convert scintillation light due to recombination of ions, to additional free charge.

Biomedical Investigations with Laser-Polarized Noble Gas Magnetic Resonance

NASA Technical Reports Server (NTRS)

Walsworth, Ronald L.

2001-01-01

We are developing laser-polarized noble gas nuclear magnetic resonance (NMR) as a novel biomedical imaging tool for ground-based and eventually space-based application. This emerging multidisciplinary technology enables high-resolution gas-space magnetic resonance imaging (MRI) (e.g., of lung ventilation) as well as studies of tissue perfusion. In addition, laser-polarized noble gases (He-3 and Xe-129) do not require a large magnetic field for sensitive detection, opening the door to practical MRI at very low magnetic fields with an open, lightweight, and low-power device. We are pursuing two specific aims in this research. The first aim is to develop a low-field (< 0.01 T) instrument for noble gas MRI of humans, and the second aim is to develop functional MRI of the lung using laser-polarized Xe-129 and related techniques.

Application of combined 81Kr and 4He chronometers to the dating of old groundwater in a tectonically active region of the North China Plain

NASA Astrophysics Data System (ADS)

Matsumoto, Takuya; Chen, Zongyu; Wei, Wen; Yang, Guo-Min; Hu, Shui-Ming; Zhang, Xiangyang

2018-07-01

Groundwater dating by radio-krypton (81Kr; half-life of about 229,000 years) was applied to the sedimentary basin aquifer of the North China Plain (NCP). Krypton gas extracted from deep groundwater in the Coastal Plain was analyzed for 81Kr/Kr ratios by Atom Trap Trace Analysis, which yielded normalized ratios of 0.05 to 0.20, corresponding to groundwater residence times of 0.5-1 million years. Helium isotope compositions were determined on groundwater samples collected from the Central Plain and the Coastal Plain along a flow path of about 200 km. Helium dissolved in the groundwater samples are a mixture of atmospheric, crustal radiogenic and mantle derived sources. Mantle derived 3He contributes up to 30% of the total, and the area of occurrence coincides with zones of previous magmatic/tectonic activities. By contrast, >90% of 4He is derived from crustal reservoirs and correlates with 81Kr ages. The absolute groundwater ages (81Kr) and radiogenic 4He concentrations permit us to calibrate the 4He flux into the aquifer as well as the vertical diffusion rate of 4He to utilize the radiogenic 4He in groundwater as a quantitative age tracer. Previously, groundwater showed 14C activities near the limit of detection (30-40 k yr), in contrast Kr and radiogenic 4He data reveal progressively older ages from the recharge area to the Coastal Plain, from <20,000 yr to 0.5 to 1 Ma along the flow path of the NCP aquifers.

Mass fractionation of noble gases in synthetic methane hydrate: Implications for naturally occurring gas hydrate dissociation

USGS Publications Warehouse

Hunt, Andrew G.; Stern, Laura; Pohlman, John W.; Ruppel, Carolyn; Moscati, Richard J.; Landis, Gary P.

2013-01-01

As a consequence of contemporary or longer term (since 15 ka) climate warming, gas hydrates in some settings may presently be dissociating and releasing methane and other gases to the ocean-atmosphere system. A key challenge in assessing the impact of dissociating gas hydrates on global atmospheric methane is the lack of a technique able to distinguish between methane recently released from gas hydrates and methane emitted from leaky thermogenic reservoirs, shallow sediments (some newly thawed), coal beds, and other sources. Carbon and deuterium stable isotopic fractionation during methane formation provides a first-order constraint on the processes (microbial or thermogenic) of methane generation. However, because gas hydrate formation and dissociation do not cause significant isotopic fractionation, a stable isotope-based hydrate-source determination is not possible. Here, we investigate patterns of mass-dependent noble gas fractionation within the gas hydrate lattice to fingerprint methane released from gas hydrates. Starting with synthetic gas hydrate formed under laboratory conditions, we document complex noble gas fractionation patterns in the gases liberated during dissociation and explore the effects of aging and storage (e.g., in liquid nitrogen), as well as sampling and preservation procedures. The laboratory results confirm a unique noble gas fractionation pattern for gas hydrates, one that shows promise in evaluating modern natural gas seeps for a signature associated with gas hydrate dissociation.

Volatiles (H, C, N, O, noble gases) in comets as tracers of early solar system events (Invited)

NASA Astrophysics Data System (ADS)

Marty, B.

2013-12-01

Volatiles (H, C, N, O, noble gases) present the largest variations in their relative abundances and, importantly, in their isotopic ratios, among solar system elements. The original composition of the protosolar nebula has been investigated through the measurements of primitive meteorites and of in-situ (e.g. Galileo probe analysis of the Jupiter's atmosphere) and sample-return (Genesis, recovery and analysis of solar wind) missions. The protosolar gas was poor in deuterium, in 15N and in 17,18O. Variations among solar system reservoir reach several hundreds of percents for the D/H and 15N/14N ratios. These variations are possibly : (i) due to interactions between XUV photons of the proto-Sun and the-dust, (ii) result from low temperature ion-molecule reactions, or (iii) constitute an heritage on interstellar volatiles trapped in dust (e.g., organics). Likewise, noble gases are elementally and isotopically (1% per amu for xenon) fractionated with respect to the composition of the solar wind (our best proxy for the protosolar nebula composition). Cometary matter directly measured on coma, or in Stardust material, or in IDPs, seems to present among the largest heterogeneities in their stable isotope compositions but knowledge on their precise compositions of the different phases and species is partial and mosty lacking. Among the several important issues requiring a better knowledge of cometary volatiles are the origin(s) of volatile elements on Earth and Moon, on Mars and on Venus, understanding large scale circulation of matter between hot and frozen zones, and the possibility of interstellar heritage for organics. Critical measurements to be made by the next cometary missions include the value of the D/H ratio in water ice, in NH3 and organics. Nitrogen is particularly interesting as cometary HCN and CN are rich in 15N, but an isotoppe mass balance will require to measure the main host species (N2 ?). Noble gases are excellent tracers of physical processes

On the Noble-Gas Induced Intersystem Crossing for the CUO Molecule: Experimental and Theoretical investigations of CUO(Ng)n (Ng = Ar, Kr, Xe; n = 1, 2, 3, 4) Complexes in Solid Neon

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liang, Binyong; Andrews, Lester S.; Li, Jun

2004-02-09

Uranium atoms excited by laser ablation react with CO in excess neon to produce the novel CUO molecule, which forms distinct Ng complexes (Ng = Ar, Kr, Xe) when the heavier noble gases are added. The CUO(Ng) complexes are identified through CO isotopic and Ng substitution on the neon matrix infrared spectra and by comparison to DFT frequency calculations. The U-C and U-O stretching frequencies of CUO(Ng) complexes are slightly red shifted from frequencies for the 1S+ CUO ground state, which identifies singlet ground state CUO(Ng) complexes. In solid neon the CUO molecule is also a complex CUO(Ne)n, and themore » CUO(Ne)n-1(Ng) complexes are likewise specified. The next singlet CUO(Ne)x(Ng)2 complexes in excess neon follow in like manner. However, the higher CUO(Ne)x(Ng)n complex (n = 3, 4) stretching modes approach pure argon matrix CUO(Ar)n values and isotopic behavior, which are characterized as triplet ground state complexes by DFT frequency calculations. This work suggests that the singlet-triplet crossing occurs with 3 Ar, 3 Kr or 4 Xe and a balance of Ne atoms coordinated to CUO in the neon matrix host.« less

The evolution of Devonian hydrocarbon gases in shallow aquifers of the northern Appalachian Basin: Insights from integrating noble gas and hydrocarbon geochemistry

NASA Astrophysics Data System (ADS)

Darrah, Thomas H.; Jackson, Robert B.; Vengosh, Avner; Warner, Nathaniel R.; Whyte, Colin J.; Walsh, Talor B.; Kondash, Andrew J.; Poreda, Robert J.

2015-12-01

groundwater (P(CH4) = ∼1 atmosphere) and elevated [Cl] and [Ba]. These data suggest that 4He is dominated by an exogenous (i.e., migrated) crustal source for these hydrocarbon gas- and salt-rich fluids. In combination with published inorganic geochemistry (e.g., 87Sr/86Sr, Sr/Ba, Br-/Cl-), new noble gas and hydrocarbon isotopic data (e.g., 20Ne/36Ar, C2+/C1, δ13C-CH4) suggest that a hydrocarbon-rich brine likely migrated from the Marcellus Formation (via primary hydrocarbon migration) as a dual-phase fluid (gas + liquid) and was fractionated by solubility partitioning during fluid migration and emplacement into conventional UD traps (via secondary hydrocarbon migration). Based on the highly fractionated 4He/CH4 data relative to Marcellus and UD production gases, we propose an additional phase of hydrocarbon gas migration where natural gas previously emplaced in UD hydrocarbon traps actively diffuses out into and equilibrates with modern shallow groundwater (via tertiary hydrocarbon migration) following uplift, denudation, and neotectonic fracturing. These data suggest that by integrating noble gas geochemistry with hydrocarbon and dissolved ion chemistry, one can better determine the source and migration processes of natural gas in the Earth's crust, which are two critical factors for understanding the presence of hydrocarbon gases in shallow aquifers.

Experimental studies and model analysis of noble gas fractionation in low-permeability porous media

NASA Astrophysics Data System (ADS)

Ding, Xin; Mack Kennedy, B.; Molins, Sergi; Kneafsey, Timothy; Evans, William C.

2017-05-01

Gas flow through the vadose zone from sources at depth involves fractionation effects that can obscure the nature of transport and even the identity of the source. Transport processes are particularly complex in low permeability media but as shown in this study, can be elucidated by measuring the atmospheric noble gases. A series of laboratory column experiments was conducted to evaluate the movement of noble gas from the atmosphere into soil in the presence of a net efflux of CO2, a process that leads to fractionation of the noble gases from their atmospheric abundance ratios. The column packings were designed to simulate natural sedimentary deposition by interlayering low permeability ceramic plates and high permeability beach sand. Gas samples were collected at different depths at CO2 fluxes high enough to cause extreme fractionation of the noble gases (4He/36Ar > 20 times the air ratio). The experimental noble gas fractionation-depth profiles were in good agreement with those predicted by the dusty gas (DG) model, demonstrating the applicability of the DG model across a broad spectrum of environmental conditions. A governing equation based on the dusty gas model was developed to specifically describe noble gas fractionation at each depth that is controlled by the binary diffusion coefficient, Knudsen diffusion coefficient and the ratio of total advection flux to total flux. Finally, the governing equation was used to derive the noble gas fractionation pattern and illustrate how it is influenced by soil CO2 flux, sedimentary sequence, thickness of each sedimentary layer and each layer's physical parameters. Three potential applications of noble gas fractionation are provided: evaluating soil attributes in the path of gas flow from a source at depth to the atmosphere, testing leakage through low permeability barriers used to isolate buried waste, and tracking biological methanogenesis and methane oxidation associated with hydrocarbon degradation.

Cucurbit[6]uril: A Possible Host for Noble Gas Atoms.

PubMed

Pan, Sudip; Mandal, Subhajit; Chattaraj, Pratim K

2015-08-27

Density functional and ab initio molecular dynamics studies are carried out to investigate the stability of noble gas encapsulated cucurbit[6]uril (CB[6]) systems. Interaction energy, dissociation energy and dissociation enthalpy are calculated to understand the efficacy of CB[6] in encapsulating noble gas atoms. CB[6] could encapsulate up to three Ne atoms having dissociation energy (zero-point energy corrected) in the range of 3.4-4.1 kcal/mol, whereas due to larger size, only one Ar or Kr atom encapsulated analogues would be viable. The dissociation energy value for the second Ar atom is only 1.0 kcal/mol. On the other hand, the same for the second Kr is -0.5 kcal/mol, implying the instability of the system. The noble gas dissociation processes are endothermic in nature, which increases gradually along Ne to Kr. Kr encapsulated analogue is found to be viable at room temperature. However, low temperature is needed for Ne and Ar encapsulated analogues. The temperature-pressure phase diagram highlights the region in which association and dissociation processes of Kr@CB[6] would be favorable. At ambient temperature and pressure, CB[6] may be used as an effective noble gas carrier. Wiberg bond indices, noncovalent interaction indices, electron density, and energy decomposition analyses are used to explore the nature of interaction between noble gas atoms and CB[6]. Dispersion interaction is found to be the most important term in the attraction energy. Ne and Ar atoms in one Ng entrapped analogue are found to stay inside the cavity of CB[6] throughout the simulation at 298 K. However, during simulation Ng2 units in Ng2@CB[6] flip toward the open faces of CB[6]. After 1 ps, one Ne atom of Ne3@CB[6] almost reaches the open face keeping other two Ne atoms inside. At lower temperature (77 K), all the Ng atoms in Ngn@CB[6] remain well inside the cavity of CB[6] throughout the simulation time (1 ps).

A Density Functional Theory Evaluation of Hydrophobic Solvation: Ne, Ar and Kr in a 50-Water Cluster. Implications for the Hydrophobic Effect.

PubMed

Kobko, Nadya; Marianski, Mateusz; Asensio, Amparo; Wieczorek, Robert; Dannenberg, J J

2012-06-15

The physical explanation for the hydrophobic effect has been the subject of disagreement. Physical organic chemists tend to use a explanation related to pressure, while many biochemists prefer an explanation that involves decreased entropy of the aqueous solvent. We present DFT calculations at the B3LYP/6-31G(d,p) and X3LYP/6-31G(d,p) levels on the solvation of three noble gases (Ne, Ar, and Kr) in clusters of 50 waters. Vibrational analyses show no substantial decreases in the vibrational entropies of the waters in any of the three clusters. The observed positive free energies of transfer from the gas phase or from nonpolar solvents to water appear to be due to the work needed to make a suitable hole in the aqueous solvent. We distinguish between hydrophobic solvations (explicitly studied here) and the hydrophobic effect that occurs when a solute (or transition state) can decrease its volume through conformational change (which is not possible for the noble gases).

Dating native gold by noble gas analyses

NASA Technical Reports Server (NTRS)

Niedermann, S.; Eugster, O.; Hofmann, B.; Thalmann, CH.; Reimold, W. U.

1993-01-01

Our recent work on He, Ne, and Ar in Alpine gold samples has demonstrated that gold is extremely retentive for He and could thus, in principle, be used for U/Th-He-4 dating. For vein-type gold from Brusson, Northern Italy, we derived a U/Th-He-4 age of 36 Ma, in agreement with the K-Ar formation age of associated muscovites and biotites. However, in placer gold from the Napf area, Central Switzerland, we observed large excesses of both He-4 and radiogenic Ar-40 (Ar-40 sub rad, defined as Ar-40-295.5-Ar-.36). The gas release systematics indicate two distinct noble gas components, one of which is released below about 800 C and the other one at the melting point of gold (1064 C). We now present results of He and Xe measurements in a 1 g placer gold sample from the river Kruempelgraben, as well as He and Ar data for Brusson vein-type gold and for gold from the Lily Gold Mine, South Africa. We calculate reasonable U/Th-He-4 as well as U-Xe ages based on those gases which are released at approximately 800 C. Probably the low-temperature components represent in-situ-produced radiogenic He and fission Xe, whereas the gases evolving when gold melts have been trapped during gold formation. Therefore, only the low-temperature components are relevant for dating purposes.

Using noble gases to investigate mountain-front recharge

USGS Publications Warehouse

Manning, A.H.; Solomon, D.K.

2003-01-01

Mountain-front recharge is a major component of recharge to inter-mountain basin-fill aquifers. The two components of mountain-front recharge are (1) subsurface inflow from the mountain block (subsurface inflow), and (2) infiltration from perennial and ephemeral streams near the mountain front (stream seepage). The magnitude of subsurface inflow is of central importance in source protection planning for basin-fill aquifers and in some water rights disputes, yet existing estimates carry large uncertainties. Stable isotope ratios can indicate the magnitude of mountain-front recharge relative to other components, but are generally incapable of distinguishing subsurface inflow from stream seepage. Noble gases provide an effective tool for determining the relative significance of subsurface inflow, specifically. Dissolved noble gas concentrations allow for the determination of recharge temperature, which is correlated with recharge elevation. The nature of this correlation cannot be assumed, however, and must be derived for the study area. The method is applied to the Salt Lake Valley Principal Aquifer in northern Utah to demonstrate its utility. Samples from 16 springs and mine tunnels in the adjacent Wasatch Mountains indicate that recharge temperature decreases with elevation at about the same rate as the mean annual air temperature, but is on average about 2??C cooler. Samples from 27 valley production wells yield recharge elevations ranging from the valley elevation (about 1500 m) to mid-mountain elevation (about 2500 m). Only six of the wells have recharge elevations less than 1800 m. Recharge elevations consistently greater than 2000 m in the southeastern part of the basin indicate that subsurface inflow constitutes most of the total recharge in this area. ?? 2003 Published by Elsevier Science B.V.

Experimental/Computational Approach to Accommodation Coefficients and its Application to Noble Gases on Aluminum Surface (Preprint)

DTIC Science & Technology

2009-02-03

computational approach to accommodation coefficients and its application to noble gases on aluminum surface Nathaniel Selden Uruversity of Southern Cahfornia, Los ...8217 ,. 0.’ a~ .......,..,P. • " ,,-0, "p"’U".. ,Po"D.’ 0.’P.... uro . P." FIG. 5: Experimental and computed radiometri~ force for argon (left), xenon

Noble-gas-induced collisional broadening of the 3P12-3P32 transition of sodium measured by the trilevel-echo technique

NASA Astrophysics Data System (ADS)

Mossberg, T. W.; Whittaker, E.; Kachru, R.; Hartmann, S. R.

1980-11-01

A variant of the trilevel-echo effect is observed and utilized to measure the effective cross section for broadening of the 3P12-3P32 transition of sodium by the noble gases. The cross section measured here should be the same as the broadening cross section obtained from a direct measurement of the collisionally broadened 3P12-3P32 transition linewidth (if such a measurement were possible). The new echo, the "inverted-difference-frequency" (IDF) trilevel echo, is well suited to the study of transitions between excited states of the same parity. At 400 K the measured broadening cross sections are He 115(12) Å2, Ne 120(12) Å2, Ar 234(23) Å2, Kr 266(27) Å2, and Xe 311(31) Å2. With He as the perturber, the cross section for broadening of the 3P12-3P32 transition can be calculated from measured depolarization and fine-structure-changing collision cross sections. With the other perturbers, however, collisional phase changes appear to be important. An intuitive diagrammatic technique for the analysis of echoes is applied to the IDF trilevel echo.

Mineralogy and noble gas isotopes of micrometeorites collected from Antarctic snow

NASA Astrophysics Data System (ADS)

Okazaki, Ryuji; Noguchi, Takaaki; Tsujimoto, Shin-ichi; Tobimatsu, Yu; Nakamura, Tomoki; Ebihara, Mitsuru; Itoh, Shoichi; Nagahara, Hiroko; Tachibana, Shogo; Terada, Kentaro; Yabuta, Hikaru

2015-06-01

We have investigated seven micrometeorites (MMs) from Antarctic snow collected in 2003 and 2010 by means of electron microscopy, X-ray diffraction, micro-Raman spectroscopy, transmission electron microscopy (TEM) observation, and noble-gas isotope analysis. Isotopic ratios of He and Ne indicate that the noble gases in these MMs are mostly of solar wind (SW). Based on the release patterns of SW 4He, which should reflect the degree of heating during atmospheric entry, the seven MMs were classified into three types including two least heated, three moderately heated, and two severely heated MMs. The heating degrees are well correlated to their mineralogical features determined by TEM observation. One of the least heated MMs is composed of phyllosilicates, whereas the other consists of anhydrous minerals within which solar flare tracks were observed. The two severely heated MMs show clear evidence of atmospheric heating such as partial melt of the uppermost surface layer in one and abundant patches of dendritic magnetite and Si-rich glass within an olivine grain in the other. It is noteworthy that a moderately heated MM composed of a single crystal of olivine has a 3He/4He ratio of 8.44 × 10-4, which is higher than the SW value of 4.64 × 10-4, but does not show a cosmogenic 21Ne signature such as 20Ne/21Ne/22Ne = 12.83/0.0284/1. The isotopic compositions of He and Ne in this sample cannot be explained by mixing of a galactic cosmic ray (GCR)-produced component and SW gases. The high 3He/4He ratio without cosmogenic 21Ne signature likely indicates the presence of a 3He-enriched component derived from solar energetic particles.

Ab initio theory of noble gas atoms in bcc transition metals.

PubMed

Jiang, Chao; Zhang, Yongfeng; Gao, Yipeng; Gan, Jian

2018-06-18

Systematic ab initio calculations based on density functional theory have been performed to gain fundamental understanding of the interactions between noble gas atoms (He, Ne, Ar and Kr) and bcc transition metals in groups 5B (V, Nb and Ta), 6B (Cr, Mo and W) and 8B (Fe). Our charge density analysis indicates that the strong polarization of nearest-neighbor metal atoms by noble gas interstitials is the electronic origin of their high formation energies. Such polarization becomes more significant with an increasing gas atom size and interstitial charge density in the host bcc metal, which explains the similar trend followed by the unrelaxed formation energies of noble gas interstitials. Upon allowing for local relaxation, nearby metal atoms move farther away from gas interstitials in order to decrease polarization, albeit at the expense of increasing the elastic strain energy. Such atomic relaxation is found to play an important role in governing both the energetics and site preference of noble gas atoms in bcc metals. Our most notable finding is that the fully relaxed formation energies of noble gas interstitials are strongly correlated with the elastic shear modulus of the bcc metal, and the physical origin of this unexpected correlation has been elucidated by our theoretical analysis based on the effective-medium theory. The kinetic behavior of noble gas atoms and their interaction with pre-existing vacancies in bcc transition metals have also been discussed in this work.

Modelling of noble anaesthetic gases and high hydrostatic pressure effects in lipid bilayers

DOE PAGES

Moskovitz, Yevgeny; Yang, Hui

2015-01-08

Our objective was to study molecular processes that might be responsible for inert gas narcosis and high-pressure nervous syndrome. The classical molecular dynamics trajectories (200 ns-long) of dioleoylphosphatidylcholine (DOPC) bilayers simulated by the Berger force field were evaluated for water and the atomic distribution of noble gases around DOPC molecules at a pressure range of 1 - 1000 bar and temperature of 310 Kelvin. Xenon and argon have been tested as model gases for general anesthetics, and neon has been investigated for distortions that are potentially responsible for neurological tremor at hyperbaric conditions. The analysis of stacked radial pair distributionmore » functions of DOPC headgroup atoms revealed the explicit solvation potential of gas molecules, which correlates with their dimensions. The orientational dynamics of water molecules at the biomolecular interface should be considered as an influential factor; while excessive solvation effects appearing in the lumen of membrane-embedded ion channels could be a possible cause of inert gas narcosis. All the noble gases tested exhibit similar patterns of the order parameter for both DOPC acyl chains, which is opposite to the patterns found for the order parameter curve at high hydrostatic pressures in intact bilayers. This finding supports the ‘critical volume’ hypothesis of anesthesia pressure reversal. The irregular lipid headgroup-water boundary observed in DOPC bilayers saturated with neon in the pressure range of 1 - 100 bar could be associated with the possible manifestation of neurological tremor at the atomic scale. The non-immobilizer neon also demonstrated the highest momentum impact on the normal component of the DOPC diffusion coefficient representing monolayers undulations rate, which indicates enhanced diffusivity, rather than atom size, as the key factor.« less

EXTERNAL PHOTOEVAPORATION OF THE SOLAR NEBULA: JUPITER's NOBLE GAS ENRICHMENTS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Monga, Nikhil; Desch, Steven

We present a model explaining the elemental enrichments in Jupiter's atmosphere, particularly the noble gases Ar, Kr, and Xe. While He, Ne, and O are depleted, seven other elements show similar enrichments (∼3 times solar, relative to H). Being volatile, Ar is difficult to fractionate from H{sub 2}. We argue that external photoevaporation by far-ultraviolet (FUV) radiation from nearby massive stars removed H{sub 2}, He, and Ne from the solar nebula, but Ar and other species were retained because photoevaporation occurred at large heliocentric distances where temperatures were cold enough (≲ 30 K) to trap them in amorphous water ice. Asmore » the solar nebula lost H, it became relatively and uniformly enriched in other species. Our model improves on the similar model of Guillot and Hueso. We recognize that cold temperatures alone do not trap volatiles; continuous water vapor production is also necessary. We demonstrate that FUV fluxes that photoevaporated the disk generated sufficient water vapor in regions ≲ 30 K to trap gas-phase species in amorphous water ice in solar proportions. We find more efficient chemical fractionation in the outer disk: whereas the model of Guillot and Hueso predicts a factor of three enrichment when only <2% of the disk mass remains, we find the same enrichments when 30% of the disk mass remains. Finally, we predict the presence of ∼0.1 M {sub ⊕} of water vapor in the outer solar nebula and protoplanetary disks in H II regions.« less

Metal-organic frameworks for Xe/Kr separation

DOEpatents

Ryan, Patrick J.; Farha, Omar K.; Broadbelt, Linda J.; Snurr, Randall Q.; Bae, Youn-Sang

2014-07-22

Metal-organic framework (MOF) materials are provided and are selectively adsorbent to xenon (Xe) over another noble gas such as krypton (Kr) and/or argon (Ar) as a result of having framework voids (pores) sized to this end. MOF materials having pores that are capable of accommodating a Xe atom but have a small enough pore size to receive no more than one Xe atom are desired to preferentially adsorb Xe over Kr in a multi-component (Xe--Kr mixture) adsorption method. The MOF material has 20% or more, preferably 40% or more, of the total pore volume in a pore size range of 0.45-0.75 nm which can selectively adsorb Xe over Kr in a multi-component Xe--Kr mixture over a pressure range of 0.01 to 1.0 MPa.

Metal-organic frameworks for Xe/Kr separation

DOEpatents

Ryan, Patrick J.; Farha, Omar K.; Broadbelt, Linda J.; Snurr, Randall Q.; Bae, Youn-Sang

2013-08-27

Metal-organic framework (MOF) materials are provided and are selectively adsorbent to xenon (Xe) over another noble gas such as krypton (Kr) and/or argon (Ar) as a result of having framework voids (pores) sized to this end. MOF materials having pores that are capable of accommodating a Xe atom but have a small enough pore size to receive no more than one Xe atom are desired to preferentially adsorb Xe over Kr in a multi-component (Xe--Kr mixture) adsorption method. The MOF material has 20% or more, preferably 40% or more, of the total pore volume in a pore size range of 0.45-0.75 nm which can selectively adsorb Xe over Kr in a multi-component Xe--Kr mixture over a pressure range of 0.01 to 1.0 MPa.

Noble gas evidence for the depositional and irradiational history of 60010-60009 core soils

NASA Technical Reports Server (NTRS)

Bogard, D. D.; Hirsch, W. C.

1977-01-01

Isotopic abundances of the noble gases have been determined in grain size separates of eleven soils from different depths in the 60010-60009 double drive tube and in magnetic and plagioclase separates from a few of these soils. Data for the 60010 core are presented here. The entire core was deposited a maximum of approximately 125 m.y. ago as deduced from the Ar-38 cosmic ray exposure age of soil 60009,457. Soils in the topmost 12 cm of the core show loss of cosmogenic He-3 and Ne-21 and gain of trapped solar gases in proportion to the degree of surface reworking by micrometeorites as deduced from FMR data. A variety of compositional and irradiational evidence suggests that soils in the core were formed by mixing of three or more components during or immediately prior to core deposition less than about 125 m.y. ago. Based on cosmogenic noble gases and a variety of other data soils 60009,457 and 60010,3107 are similar (and possibly identical) to two of the end member soils which formed the mixture. More mature soils in the core, however, could not have matured in situ from these two soils because of significant differences in noble gas abundances and chemical composition.

Simulations of noble gases adsorbed on graphene

NASA Astrophysics Data System (ADS)

Maiga, Sidi; Gatica, Silvina

2014-03-01

We present results of Grand Canonical Monte Carlo simulations of adsorption of Kr, Ar and Xe on a suspended graphene sheet. We compute the adsorbate-adsorbate interaction by a Lennard-Jones potential. We adopt a hybrid model for the graphene-adsorbate force; in the hybrid model, the potential interaction with the nearest carbon atoms (within a distance rnn) is computed with an atomistic pair potential Ua; for the atoms at r>rnn, we compute the interaction energy as a continuous integration over a carbon uniform sheet with the density of graphene. For the atomistic potential Ua, we assume the anisotropic LJ potential adapted from the graphite-He interaction proposed by Cole et.al. This interaction includes the anisotropy of the C atoms on graphene, which originates in the anisotropic π-bonds. The adsorption isotherms, energy and structure of the layer are obtained and compared with experimental results. We also compare with the adsorption on graphite and carbon nanotubes. This research was supported by NSF/PRDM (Howard University) and NSF (DMR 1006010).

Development of Laser-Polarized Noble Gas Magnetic Resonance Imaging (MRI) Technology

NASA Technical Reports Server (NTRS)

Walsworth, Ronald L.

2004-01-01

We are developing technology for laser-polarized noble gas nuclear magnetic resonance (NMR), with the aim of enabling it as a novel biomedical imaging tool for ground-based and eventually space-based application. This emerging multidisciplinary technology enables high-resolution gas-space magnetic resonance imaging (MRI)-e.g., of lung ventilation, perfusion, and gas-exchange. In addition, laser-polarized noble gases (3He and 1BXe) do not require a large magnetic field for sensitive NMR detection, opening the door to practical MRI with novel, open-access magnet designs at very low magnetic fields (and hence in confined spaces). We are pursuing two specific aims in this technology development program. The first aim is to develop an open-access, low-field (less than 0.01 T) instrument for MRI studies of human gas inhalation as a function of subject orientation, and the second aim is to develop functional imaging of the lung using laser-polarized He-3 and Xe-129.

Gradient-induced Longitudinal Relaxation of Hyperpolarized Noble Gases in the Fringe Fields of Superconducting Magnets Used for Magnetic Resonance

PubMed Central

Zheng, Wangzhi; Cleveland, Zackary I.; Möller, Harald E.; Driehuys, Bastiaan

2010-01-01

When hyperpolarized noble gases are brought into the bore of a superconducting magnet for magnetic resonance imaging (MRI) or spectroscopy studies, the gases must pass through substantial field gradients, which can cause rapid longitudinal relaxation. In this communication, we present a means of calculating this spatially dependent relaxation rate in the fringe field of typical magnets. We then compare these predictions to experimental measurements of 3He relaxation at various positions near a medium-bore 2-T small animal MRI system. The calculated and measured relaxation rates on the central axis of the magnet agree well and show a maximum 3He relaxation rate of 3.83 × 10−3 s−1 (T1 = 4.4 min) at a distance of 47 cm from the magnet isocenter. We also show that if this magnet were self-shielded, its minimum T1 would drop to 1.2 min. In contrast, a typical self-shielded 1.5-T clinical MRI scanner will induce a minimum on-axis T1 of 12 min. Additionally, we show that the cylindrically symmetric fields of these magnets enable gradient-induced relaxation to be calculated using only knowledge of the on-axis longitudinal field, which can either be measured directly or calculated from a simple field model. Thus, while most MRI magnets employ complex and proprietary current configurations, we show that their fringe fields and the resulting gradient induced relaxation are well approximated by simple solenoid models. Finally, our modeling also demonstrates that relaxation rates can increase by nearly an order of magnitude at radial distances equivalent to the solenoid radius. PMID:21134771

Gradient-induced longitudinal relaxation of hyperpolarized noble gases in the fringe fields of superconducting magnets used for magnetic resonance.

PubMed

Zheng, Wangzhi; Cleveland, Zackary I; Möller, Harald E; Driehuys, Bastiaan

2011-02-01

When hyperpolarized noble gases are brought into the bore of a superconducting magnet for magnetic resonance imaging (MRI) or spectroscopy studies, the gases must pass through substantial field gradients, which can cause rapid longitudinal relaxation. In this communication, we present a means of calculating this spatially dependent relaxation rate in the fringe field of typical magnets. We then compare these predictions to experimental measurements of (3)He relaxation at various positions near a medium-bore 2-T small animal MRI system. The calculated and measured relaxation rates on the central axis of the magnet agree well and show a maximum (3)He relaxation rate of 3.83×10(-3) s(-1) (T(1)=4.4 min) at a distance of 47 cm from the magnet isocenter. We also show that if this magnet were self-shielded, its minimum T(1) would drop to 1.2 min. In contrast, a typical self-shielded 1.5-T clinical MRI scanner will induce a minimum on-axis T(1) of 12 min. Additionally, we show that the cylindrically symmetric fields of these magnets enable gradient-induced relaxation to be calculated using only knowledge of the on-axis longitudinal field, which can either be measured directly or calculated from a simple field model. Thus, while most MRI magnets employ complex and proprietary current configurations, we show that their fringe fields and the resulting gradient-induced relaxation are well approximated by simple solenoid models. Finally, our modeling also demonstrates that relaxation rates can increase by nearly an order of magnitude at radial distances equivalent to the solenoid radius. Copyright © 2010 Elsevier Inc. All rights reserved.

Pressure-dependent refractive indices of gases by THz time-domain spectroscopy.

PubMed

Sang, Bark Hyeon; Jeon, Tea-In

2016-12-12

Noncontact terahertz time-domain spectroscopy was employed to measure pressure-dependent refractive indices of gases such as helium (He), argon (Ar), krypton (Kr), oxygen (O₂), nitrogen (N₂), methane (CH₄), and carbon dioxide (CO₂). The refractive indices of these gases scaled linearly with pressure, for pressures in the 55-3,750 torr range. At the highest pressure, the refractive indices ((n-1) x 10⁶) of He and CO₂ were 170 and 2,390, respectively. The refractive index of CO₂ was 14.1-fold higher than that of He, owing to the stronger polarizability of CO₂. Although the studied gases differed in terms of their molecular structure, their refractive indices were strongly determined by polarizability. The measured refractive indices agreed well with the theoretical calculations.

A Density Functional Theory Evaluation of Hydrophobic Solvation: Ne, Ar and Kr in a 50-Water Cluster. Implications for the Hydrophobic Effect

PubMed Central

Kobko, Nadya; Marianski, Mateusz; Asensio, Amparo; Wieczorek, Robert; Dannenberg, J. J.

2011-01-01

The physical explanation for the hydrophobic effect has been the subject of disagreement. Physical organic chemists tend to use a explanation related to pressure, while many biochemists prefer an explanation that involves decreased entropy of the aqueous solvent. We present DFT calculations at the B3LYP/6-31G(d,p) and X3LYP/6-31G(d,p) levels on the solvation of three noble gases (Ne, Ar, and Kr) in clusters of 50 waters. Vibrational analyses show no substantial decreases in the vibrational entropies of the waters in any of the three clusters. The observed positive free energies of transfer from the gas phase or from nonpolar solvents to water appear to be due to the work needed to make a suitable hole in the aqueous solvent. We distinguish between hydrophobic solvations (explicitly studied here) and the hydrophobic effect that occurs when a solute (or transition state) can decrease its volume through conformational change (which is not possible for the noble gases). PMID:22666658

A Complex Exposure History of the Gold Basin L4-Chondrite Shower from Cosmogenic Radionuclides and Noble Gases

NASA Technical Reports Server (NTRS)

Welten, K. C.; Nishiizumi, K.; Caffee, M. W.; Masarik, J.; Wieler, R.

2001-01-01

Cosmogenic radionuclides and noble gases in samples of the Gold Basin L-chondrite shower indicate a complex exposure history, with a first stage exposure on the parent body, followed by a second stage of approx. 19 Myr in a meteoroid 3-4 m in radius. Additional information is contained in the original extended abstract.

Isotopic separation of He-3/He-4 from solar wind gases evolved from the lunar regolith

NASA Astrophysics Data System (ADS)

Wilkes, William R.; Wittenberg, Layton J.

The potential benefits of He-3 when utilized in a nuclear fusion reactor to provide clean, safe electricity in the 21st century for the world's inhabitants has been documented. Unfortunately, He is scarce on earth. Large quantities of He-3, perhaps a million tons, are embedded in the lunar regolith, presumably implanted by the solar wind together with other elements, notably He-4, H, C, and N. Several studies have suggested processing the lunar regolith and recovering these valuable solar wind gases. Once released, these gases can be separated for use. The separation of helium isotopes is described in this paper. He-3 constitutes only 400 at. ppm of lunar He, too dilute to separate economically by distillation alone. A 'superfluid' separator is being considered to preconcentrate the He-3. The superfluid separator consists of a porous filter in a tube maintained at a temperature of 2.17 K or less. Although the He-4, which is superfluid below 2.17 K, flows readily through the filter, the He is blocked by the filter, and becomes enriched at the feed end. He can be enriched to about 10 percent in such a system. The enriched product from the superfluid separation serves as a feed to a distillation apparatus operating at a pressure of 9 kPa, with a boiler temperature of 2.4 K, and a condenser temperature of 1.6 K. Under constant flow conditions, a 99.9 percent enriched He product can be produced in this apparatus. The heat rejection load of the refrigeration equipment necessary to cool the separation operations would be conducted during the lunar nights.

The Role of Noble Gases in Defining the Mean Residence Times of Fluids within Precambrian Crustal Systems

NASA Astrophysics Data System (ADS)

Warr, O.; Sherwood Lollar, B.; Fellowes, J.; Sutcliffe, C. N.; McDermott, J. M.; Holland, G.; Mabry, J.; Ballentine, C. J.

2015-12-01

Brines rich in N2, H2, CH4 and He hosted within Precambrian crustal rocks are known to sustain microbial life [1]. The geological systems containing these brines have the potential to isolate organisms over planetary timescales and so can provide unique insight into the diversity and evolution of terrestrial life [1-3]. Long considered geological outliers, the prevalence of systems containing these ancient, deep fracture waters is only now being revealed. Recent studies demonstrate the Precambrian crust which accounts for ~70% of total crustal surface area has a global hydrogen production comparable to marine systems [2]. In addition to H2-producing reactions (e.g. radiolysis and serpentinization), a diversity of CH4-producing reactions also occur in these systems through both microbial and water-rock interactions [1, 2]. However, the role these Precambrian systems have in global hydrogen and carbon cycles is poorly understood. For this we need good constraints on the origins, residence times and degree of microbial activity of the fluids within these systems as well as the degree of interaction with external systems. Fortunately, noble gases are ideal for this role [1,3]. Previous noble gas analysis of N2, H2, CH4 and He-rich fluid samples collected at 2.4 km depth from a Cu-Zn mine in Timmins, Ontario, identified isolated fracture fluids with the oldest residence times ever observed (>1.1 Ga) [3]. This study has been significantly expanded now to fluids from an even greater depth (3 km) at Timmins, and from two new mines in the Sudbury Basin. Preliminary data from the deeper Timmins level indicate a new closed system with 136Xe/130Xe ratios 93% above modern air values (20% at 2.4 km) and an early atmosphere 124Xe/130Xe signal approaching the age of the host rock (~2.7 Ga) [4]. In comparison, the Sudbury system indicates exchange with an external source, being highly enriched in helium (30% gas volume) but with a low fissiogenic 136Xe/130Xe excess (10-38% above

Noble Gas Thermometry and Hydrologic Ages: Evidence for Late Holocene Warming in Southwest Texas

NASA Astrophysics Data System (ADS)

Castro, M.; Goblet, P.

2003-12-01

Paleoclimatic reconstruction through the use of noble gases dissolved in groundwater has been the object of numerous studies in recent years. Unlike many other continental temperature proxies, noble gases have the advantage of providing direct information on atmospheric temperatures at the time rainwater penetrated the ground and joined a particular groundwater reservoir. In recent years, new methods for determination of noble gas temperatures have been developed, which provide a high level of accuracy on such temperature estimations. The issue of paleoclimatic reconstruction through noble gases however, is not only one of accurate temperature determination, but also one of accurate water age estimation so that a correct correspondence between noble gas temperatures and groundwater age can be established and proper paleoclimatic reconstruction attempted. The typical approach to estimate groundwater ages has been based on computing water travel times along streamlines from the recharge to the observation point taking into account only advection. This approach is limited because, like any other tracer, the movement of water in porous media is also affected by cinematic dispersion and molecular diffusion. We have therefore undertaken the formulation of hydrologic models that yield significantly better constraints on groundwater ages in the Carrizo aquifer and surrounding formations of south Texas, where noble gas temperatures have already been determined. To account for groundwater mixing we treat age as one would treat a solute concentration. In order to simulate groundwater ages we used a finite element model of groundwater flow that has been validated by 4He and 3He. The finite model spans a 120.6 Km cross-section between altitudes of +220m and -2210 m, and comprises 58,968 elements and 31,949 nodes. Combination of these newly calculated water ages and previously reported noble gas temperatures reveals new aspects of late Pleistocene and Holocene climate in

Global atmospheric monitoring of noble gases: insight into transport processes in the southern hemisphere.

NASA Astrophysics Data System (ADS)

Kusmierczyk-Michulec, J.; Kalinowski, M.; Bourgouin, P.; Schoeppner, M.

2017-12-01

The International Monitoring System (IMS) developed by the Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO) is a global system of monitoring stations, using four complementary technologies: seismic, hydroacoustic, infrasound and radionuclide. Data from all stations, belonging to IMS, are collected and transmitted to the International Data Centre (IDC) in Vienna, Austria. The radionuclide network comprises 80 stations, of which 31 stations are located in the Southern Hemisphere. The aim of radionuclide stations is a global monitoring of radioactive aerosols and radioactive noble gases supported by atmospheric transport modeling (ATM). The air mass trajectory provides a "link" between a radionuclide release and a detection confirmed by radionuclide measurements. One of the important noble gases, monitored on a daily basis, is xenon. It can be produced either during a nuclear explosion with a high fission yield, and thus be considered as an important tracer to prove the nuclear character of an explosion, or be emitted from nuclear power plants (NPPs) or from isotope production facilities (IPFs). On the southern hemisphere the number of IPF is rather limited in comparison to the northern hemisphere. Among the major sources are: the ANSTO facility in Sydney (Australia), CNEA in Ezeiza (Argentina), BaTek/INUKI in Jakarta (Indonesia) and NECSA in Pelindaba (South Africa). This study will demonstrate the examples of seasonal contribution of Xe-133 emissions from major sources as observed at selected IMS stations located in the southern hemisphere. It will show as well examples of the atmospheric transport from the northern to the southern hemisphere, and the influence of strong atmospheric convection.

Laser Interferometric Measurements of the Physical Properties for He, ne Gases and Their Mixture

NASA Astrophysics Data System (ADS)

Abdel-Moniem, N. M.; El-Masry, M. M.; El-Bradie, B.; El-Mekawy, F. M.

2010-04-01

A Mach-Zehner interferometer MZI illuminated with He-Ne Laser 632.8nm is used for measuring the refractive index for He, Ne gases and their mixture HeNe. The measurements are carried out at different pressures and temperatures. The error factors of the refractive index measurements for He, Ne and HeNe gases are equal to ±1.7×10-5, ±9.5×10-6 and ±7.25×10-5 respectively. Some calculations of the electrical properties are carried out such as the optical permittivity dielectric susceptibility and specific refractivity from the determination of the refractive index. Also, the molecular radii of the gases under investigation are computed then the transport coefficients (diffusion. viscosity and thermal conductivity) are calculated. All of these calculations are carried out at different pressures and temperatures. The experimental results of refractive index for the above mixture are compared with the results estimated using one of the mixing rules and a good agreement is achieved. Also, some physical parameters are compared with other values in another literatures.

Noble Gas Temperature Proxy for Climate Change

EPA Science Inventory

Noble gases in groundwater appear to offer a practical approach for quantitatively determining past surface air temperatures over recharge areas for any watershed. The noble gas temperature (NGT) proxy should then permit a paleothermometry of a region over time. This terrestria...

Noble gas loss may indicate groundwater flow across flow barriers in southern Nevada

USGS Publications Warehouse

Thomas, J.M.; Bryant, Hudson G.; Stute, M.; Clark, J.F.

2003-01-01

Average calculated noble gas temperatures increase from 10 to 22oC in groundwater from recharge to discharge areas in carbonate-rock aquifers of southern Nevada. Loss of noble gases from groundwater in these regional flow systems at flow barriers is the likely process that produces an increase in recharge noble gas temperatures. Emplacement of low permeability rock into high permeability aquifer rock and the presence of low permeability shear zones reduce aquifer thickness from thousands to tens of meters. At these flow barriers, which are more than 1,000 m lower than the average recharge altitude, noble gases exsolve from the groundwater by inclusion in gas bubbles formed near the barriers because of greatly reduced hydrostatic pressure. However, re-equilibration of noble gases in the groundwater with atmospheric air at the low altitude spring discharge area, at the terminus of the regional flow system, cannot be ruled out. Molecular diffusion is not an important process for removing noble gases from groundwater in the carbonate-rock aquifers because concentration gradients are small.

Noble gas and hydrocarbon tracers in multiphase unconventional hydrocarbon systems: Toward integrated advanced reservoir simulators

NASA Astrophysics Data System (ADS)

Darrah, T.; Moortgat, J.; Poreda, R. J.; Muehlenbachs, K.; Whyte, C. J.

2015-12-01

Although hydrocarbon production from unconventional energy resources has increased dramatically in the last decade, total unconventional oil and gas recovery from black shales is still less than 25% and 9% of the totals in place, respectively. Further, the majority of increased hydrocarbon production results from increasing the lengths of laterals, the number of hydraulic fracturing stages, and the volume of consumptive water usage. These strategies all reduce the economic efficiency of hydrocarbon extraction. The poor recovery statistics result from an insufficient understanding of some of the key physical processes in complex, organic-rich, low porosity formations (e.g., phase behavior, fluid-rock interactions, and flow mechanisms at nano-scale confinement and the role of natural fractures and faults as conduits for flow). Noble gases and other hydrocarbon tracers are capably of recording subsurface fluid-rock interactions on a variety of geological scales (micro-, meso-, to macro-scale) and provide analogs for the movement of hydrocarbons in the subsurface. As such geochemical data enrich the input for the numerical modeling of multi-phase (e.g., oil, gas, and brine) fluid flow in highly heterogeneous, low permeability formations Herein we will present a combination of noble gas (He, Ne, Ar, Kr, and Xe abundances and isotope ratios) and molecular and isotopic hydrocarbon data from a geographically and geologically diverse set of unconventional hydrocarbon reservoirs in North America. Specifically, we will include data from the Marcellus, Utica, Barnett, Eagle Ford, formations and the Illinois basin. Our presentation will include geochemical and geological interpretation and our perspective on the first steps toward building an advanced reservoir simulator for tracer transport in multicomponent multiphase compositional flow (presented separately, in Moortgat et al., 2015).

Noble gases, stable isotopes, and radiocarbon as tracers of flow in the Dakota aquifer, Colorado and Kansas

USGS Publications Warehouse

Clark, J.F.; Davisson, M.L.; Hudson, G.B.; Macfarlane, P.A.

1998-01-01

A suite of chemical and isotope tracers (dissolved noble gases, stable isotopes of water, radiocarbon, and CI) have been analyzed along a flow path in the Dakota aquifer system to determine likely recharge sources, ground water residence times, and the extent of mixing between local and intermediate flow systems, presumably caused by large well screens. Three water types were distinguished with the tracers, each having a very different history. Two of the water types were found in south-eastern Colorado where the Dakota is poorly confined. The tracer data suggest that the first group recharged locally during the last few thousand years and the second group was composed of ground water that recharged earlier during a cooler climate, presumably during the last glacial period (LGP) and mixed aged water. The paleotemperature record archived in this groundwater system indicates that south-eastern Colorado was about 5??C cooler during the LGP than during the late Holocene. Similar temperature changes derived from dissolved noble gases in other aquifer systems have been reported earlier for the south-western United States. The third water type was located down gradient of the first two in the confined Dakota in western and central Kansas. Groundwater residence time of this water mass is on the order of 104-105 yrs and its recharge location is near the Colorado and Kansas border down gradient of the other water types. The study shows the importance of using multiple tracers when investigating ground water systems.A suite of chemical and isotope tracers (dissolved noble gases, stable isotopes of water, radiocarbon, and CL) were analyzed along a flow path in the Dakota aquifer system to determine likely recharge sources, ground water residence times, and the extent of mixing between local and intermediate flow systems. Three water types were distinguished with the tracers, each having a very different history. Two of the water types were located in south-eastern Colorado

Infrared Matrix-Isolation Study of New Noble-Gas Compounds

NASA Astrophysics Data System (ADS)

Zhu, Cheng; Räsänen, Markku; Khriachtchev, Leonid

2016-06-01

We identify new noble-gas compounds in solid matrices using IR spectroscopy. The compounds under study belong to two types: HNgY and YNgY' where Ng is a noble-gas atom and Y and Y' are electronegative fragments. The experimental assignments are supported by ab initio calculations at the MP2(full) and CCSD(T) levels of theory with the def2-TZVPPD basis set. We have prepared and characterized two new HNgY compounds (noble-gas hydrides): HKrCCCl in a Kr matrix and HXeCCCl in a Xe matrix.I The synthesis of these compounds includes two steps: UV photolysis of HCCCl in a noble-gas matrix to form the H + CCCl fragments and annealing of the matrix to mobilize H atoms and to promote the H + Ng + CCCl = HNgCCCl reaction. An interesting observation in the experiments on HXeCCCl in a Xe matrix is the temperature-induced transformation of the three H-Xe stretching bands. This observation is explained by temperature-induced changes of local matrix morphology around the embedded HXeCCCl molecule. In these experiments, we have also obtained the IR spectrum of the CCCl radical, which is produced by photodecomposition of HCCCl. We have identified three new YNgY' compounds (fluorinated noble-gas cyanides): FKrCN in a Kr matrix and FXeCN and FXeNC in a Xe matrix.II These molecule are formed by photolysis of FCN in a noble-gas matrix due to locality of this process. The amount of these molecules increases upon thermal mobilization of the F atoms in the photolyzed matrix featuring the F + Ng + CN reaction.

Noble Gas Release Signal as a Precursor to Fracture

NASA Astrophysics Data System (ADS)

Bauer, S. J.; Lee, H.; Gardner, W. P.

2017-12-01

We present empirical results of rock strain, microfracturing, acoustic emissions, and noble gas release from laboratory triaxial experiments for a granite, basalt, shale and bedded rock salt. Noble gases are released and measured real-time during deformation using mass spectrometry. The gas release represents a precursive signal to macrofracture. Gas release is associated with increased acoustic emissions indicating that microfracturing is required to release gas and create pathways for the gas to be sensed. The gas released depends on initial gas content, pore structure and its evolution during deformation, the deformation amount, matrix permeability, deformation style and the stress/strain history. Gases are released from inter and intracrystalline sites; release rate increases as strain and microfracturing increases. The gas composition depends on lithology, geologic history and age, fluids present, and radioisotope concentrations that affect radiogenic noble gas isotope (e.g. 4He,40Ar) production. Noble gas emission and its relationship to crustal processes such as seismicity and volcanism, tectonic velocities, qualitative estimates of deep permeability, age dating of groundwater, and a signature of nuclear weapon detonation. Our result show that mechanical deformation of crustal materials is an important process controlling gas release from rocks and minerals, and should be considered in techniques which utilize gas release and/or accumulation. We propose using noble gas release to signal rock deformation in boreholes, mines and waste repositories. We postulate each rock exhibits a gas release signature which is microstructure, stress, strain, and/or permanent deformation dependent. Calibration of such relationships, for example relating gas release per rock unit volume to strain may be used to quantify rock deformation and develop predictive models.Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and

Underground Nuclear Explosions and Release of Radioactive Noble Gases

NASA Astrophysics Data System (ADS)

Dubasov, Yuri V.

2010-05-01

Over a period in 1961-1990 496 underground nuclear tests and explosions of different purpose and in different rocks were conducted in the Soviet Union at Semipalatinsk and anovaya Zemlya Test Sites. A total of 340 underground nuclear tests were conducted at the Semipalatinsk Test Site. One hundred seventy-nine explosions (52.6%) among them were classified as these of complete containment, 145 explosions (42.6%) as explosions with weak release of radioactive noble gases (RNG), 12 explosions (3.5%) as explosions with nonstandard radiation situation, and four excavation explosions with ground ejection (1.1%). Thirty-nine nuclear tests had been conducted at the Novaya Zemlya Test Site; six of them - in shafts. In 14 tests (36%) there were no RNG release. Twenty-three tests have been accompanied by RNG release into the atmosphere without sedimental contamination. Nonstandard radiation situation occurred in two tests. In incomplete containment explosions both early-time RNG release (up to ~1 h) and late-time release from 1 to 28 h after the explosion were observed. Sometimes gas release took place for several days, and it occurred either through tunnel portal or epicentral zone, depending on atmospheric air temperature.

Experimental studies and model analysis of noble gas fractionation in porous media

USGS Publications Warehouse

Ding, Xin; Kennedy, B. Mack.; Evans, William C.; Stonestrom, David A.

2016-01-01

The noble gases, which are chemically inert under normal terrestrial conditions but vary systematically across a wide range of atomic mass and diffusivity, offer a multicomponent approach to investigating gas dynamics in unsaturated soil horizons, including transfer of gas between saturated zones, unsaturated zones, and the atmosphere. To evaluate the degree to which fractionation of noble gases in the presence of an advective–diffusive flux agrees with existing theory, a simple laboratory sand column experiment was conducted. Pure CO2 was injected at the base of the column, providing a series of constant CO2 fluxes through the column. At five fixed sampling depths within the system, samples were collected for CO2 and noble gas analyses, and ambient pressures were measured. Both the advection–diffusion and dusty gas models were used to simulate the behavior of CO2 and noble gases under the experimental conditions, and the simulations were compared with the measured depth-dependent concentration profiles of the gases. Given the relatively high permeability of the sand column (5 ´ 10−11 m2), Knudsen diffusion terms were small, and both the dusty gas model and the advection–diffusion model accurately predicted the concentration profiles of the CO2 and atmospheric noble gases across a range of CO2 flux from ?700 to 10,000 g m−2 d−1. The agreement between predicted and measured gas concentrations demonstrated that, when applied to natural systems, the multi-component capability provided by the noble gases can be exploited to constrain component and total gas fluxes of non-conserved (CO2) and conserved (noble gas) species or attributes of the soil column relevant to gas transport, such as porosity, tortuosity, and gas saturation.

New method of 85Kr reduction in a noble gas based low-background detector

NASA Astrophysics Data System (ADS)

Akimov, D. Yu.; Bolozdynya, A. I.; Burenkov, A. A.; Hall, C.; Kovalenko, A. G.; Kuzminov, V. V.; Simakov, G. E.

2017-04-01

Krypton-85 is an anthropogenic beta-decaying isotope which produces low energy backgrounds in dark matter and neutrino experiments, especially those based upon liquid xenon. Several technologies have been developed to reduce the Kr concentration in such experiments. We propose to augment those separation technologies by first adding to the xenon an 85Kr-free sample of krypton in an amount much larger than the natural krypton that is already present. After the purification system reduces the total Kr concentration to the same level, the final 85Kr concentration will be reduced even further by the dilution factor. A test cell for measurement of the activity of various Kr samples has been assembled, and the activity of 25-year-old krypton has been measured. The measured activity agrees well with the expected activity accounting for the 85Kr abundance of the earth's atmosphere in 1990 and the half-life of the isotope. Additional tests with a Kr sample produced in the year 1944 (before the atomic era) have been done in order to demonstrate the sensitivity of the test cell.

Noble Gas-Uranium Coordination and Intersystem Crossing for the CUO(Ne)x(Ng)n (Ng = Ar, Kr, Xe) Complexes in Solid Neon

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andrews, Lester; Liang, Binyong; Li, Jun

2004-02-15

Atomic uranium excited by laser ablation reacts with CO in excess neon to produce the novel CUO molecule, which forms weak complexes CUO(Ne)m with neon and stronger complexes CUO(Ne)x(Ng)n (Ng = Ar, Kr, Xe) when the heavier noble gas atoms are present. The heavier CUO(Ne)m-1(Ng) complexes are identified through the effects of CO isotopic and Ng substitution on the neon matrix infrared spectra and by comparison to DFT frequency calculations on model complexes CUO(Ng) (Ng = Ne, Ar, Kr, Xe). The U-C and U-O stretching frequencies of CUO(Ne)m-1(Ng) complexes are slightly red shifted from 1047 and 872 cm-1 frequencies formore » the 1Sigma+ CUO ground state neon complex, which identifies singlet ground state CUO(Ne)m-1(Ng) complexes in solid neon. The next singlet CUO(Ne)x(Ng)2 complexes in excess neon follow in like manner. However, stretching modes and the isotopic shifts of the higher CUO(Ne)x(Ng)n complex approach those of the pure argon matrix CUO(Ar)n complex, which characterizes triple t ground state complexes by comparison to DFT frequency calculations.« less

Real-time noble gas release signaling rock deformation

NASA Astrophysics Data System (ADS)

Bauer, S. J.; Gardner, W. P.; Lee, H.

2016-12-01

We present empirical results/relationships of rock strain, microfracture density, acoustic emissions, and noble gas release from laboratory triaxial experiments for a granite and basalt. Noble gases are contained in most crustal rock at inter/intra granular sites, their release during natural and manmade stress and strain changes represents a signal of brittle/semi brittle deformation. The gas composition depends on lithology, geologic history and age, fluids present, and uranium, thorium and potassium-40 concentrations in the rocks that affect radiogenic noble gases (helium, argon) production. Noble gas emission and its relationship to crustal processes have been studied, including correlations to tectonic velocities and qualitative estimates of deep permeability from surface measurements, finger prints of nuclear weapon detonation, and as potential precursory signals to earthquakes attributed to gas release due to pre-seismic stress, dilatancy and/or rock fracturing. Helium emission has been shown as a precursor of volcanic activity. Real-time noble gas release is observed using an experimental system utilizing mass spectrometers to measure gases released during triaxial rock deformation. Noble gas release is shown to represent a sensitive precursor signal of rock deformation by relating real-time noble gas release to stress-strain state changes and acoustic emissions. We propose using noble gas release to also signal rock deformation in boreholes, mines and nuclear waste repositories. We postulate each rock exhibits a gas release signature which is microstructure, stress/strain state, and or permanent deformation dependent. Such relationships, when calibrated, may be used to sense rock deformation and then develop predictive models. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corp., for the US Dept. of Energy's National Nuclear Security Administration under

A mass spectrometric line for tritium analysis of water and noble gas measurements from different water amounts in the range of microlitres and millilitres.

PubMed

Papp, Laszlo; Palcsu, Laszlo; Major, Zoltan; Rinyu, Laszlo; Tóth, Istvan

2012-01-01

This paper describes the procedure followed for noble gas measurements for litres, millilitres and microlitres of water samples in our laboratory, including sample preparation, mass spectrometric measurement procedure, and the complete calibrations. The preparation line extracts dissolved gases from water samples of volumes of 0.2 μ l to 3 l and it separates them as noble and other chemically active gases. Our compact system handles the following measurements: (i) determination of tritium concentration of environmental water samples by the (3)He ingrowth method; (ii) noble gas measurements from surface water and groundwater; and (iii) noble gas measurements from fluid inclusions of solid geological archives (e.g. speleothems). As a result, the tritium measurements have a detection limit of 0.012 TU, and the expectation value (between 1 and 20 TU) is within 0.2 % of the real concentrations with a standard deviation of 2.4 %. The reproducibility of noble gas measurements for water samples of 20-40 ml allows us to determine solubility temperatures by an uncertainty better than 0.5 °C. Moreover, noble gas measurements for tiny water amounts (in the microlitre range) show that the results of the performed calibration measurements for most noble gas isotopes occur with a deviation of less than 2 %. Theoretically, these precisions for noble gas concentrations obtained from measurements of waters samples of a few microlitres allow us to determine noble gas temperatures by an uncertainty of less than 1 °C. Here, we present the first noble gas measurements of tiny amounts of artificial water samples prepared under laboratory conditions.

Infrared Spectroscopic and Electronic Structure Investigations of Beryllium Halide Molecules, Cations, and Anions in Noble Gas Matrices.

PubMed

Yu, Wenjie; Andrews, Lester; Wang, Xuefeng

2017-11-22

Laser-ablated Be atoms, cations, and electrons were reacted with F 2 , ClF, Cl 2 , NF 3 , CCl 4 , CF 2 Cl 2 , HCl, DCl, and SiCl 4 diluted in noble gases. The major products were the dihalides BeF 2 , BeClF, BeCl 2 , and the hydride chloride HBeCl, whose identities were confirmed by comparison with previous evaporative work, deuterium substitution, and vibrational frequency calculations. The matrix-isolated fundamental frequency of the BeF molecule is higher, and the frequency of BeCl is lower, than that determined for the gas-phase molecules. The BeF + and BeCl + cations formed strong dipole-induced dipole complexes in solid Ne, Ar, Kr, and Xe with stepwise increase in computed noble gas dissociation energies. Going down the family NgBeF + and NgBeCl + series (Ng = Ne, Ar, Kr, Xe) the Mulliken charges q(Be) decrease, while q(Ng) increases, and the dipole moments decrease, which suggests covalent bonding in the xenon species. We find that the largest intramatrix shift is Ne to Ar which follows the largest factor increase for the Ng atomic polarizabilities. Extra electrons produce Cl - , which reacts with HCl to form the stable HCl 2 - anion and possibly with BeCl 2 to give BeCl 3 - . A weak band observed in neon experiments with F 2 is probably due to BeF 3 - .

Modeling protein-small molecule interactions: structure and thermodynamics of noble gases binding in a cavity in mutant phage T4 lysozyme L99A.

PubMed

Mann, G; Hermans, J

2000-09-29

The complexes of phage T4 lysozyme L99A with noble gases have been studied by molecular dynamics simulation. In a long simulation of the complex with one Xe atom, the structure was found to undergo global conformation change involving a reversible opening and closing of the entrance to the substrate-binding site, during which the conformations of the N and C-terminal domains varied little. The distributions of Xe positions sampled in dynamics simulations were refined in terms of anisotropic Gaussian distributions via least-squares minimization of the difference between Fourier transforms. In addition, molecular transformation simulations have been applied in order to calculate the binding free energies of Xe, Kr and Ar relative to a standard state at a pressure of 1 bar. A single bound Xe is found to assume an equilibrium distribution over three adjacent preferred sites, while in a two-Xe complex, the two Xe atoms preferentially occupy two of these. The positions of the three sites agree closely with the positions of bound Xe determined in the refined crystal structure of a complex formed at a pressure of 8 bar Xe, and the calculated affinities agree well with the observed partial occupancies. At a pressure of 8 bar, a mixture of one-Xe and two-Xe complexes is present, and similarly for complexes with Kr and Ar, with single occupancy relatively more prevalent with Kr and Ar. (Binding of a third Xe atom is found to be quite unfavorable.) A comparison with simulation results for the binding of benzene to the same site leads to the conclusion that binding of Xe within cavities in proteins is common because of several favorable factors: (1) Xe has a large atomic polarizability; (2) Xe can be applied at a relatively high pressure, i.e. high chemical potential; (3) an unfavorable entropic term related to the need to orient the ligand in the binding site is absent. Finally, it is found that the model's binding energy of a water molecule in the cavity is insufficient to

Helium Isotopes and Noble Gas Abundances of Cave Dripping Water in Three Caves in East Asia

NASA Astrophysics Data System (ADS)

Chen, A. T.; Shen, C. C.; Tan, M.; Li, T.; Uemura, R.; Asami, R.

2015-12-01

Paleo-temperature recorded in nature archives is a critical parameter to understand climate change in the past. With advantages of unique inert chemical characteristics and sensitive solubilities with temperature, dissolved noble gases in speleothem inclusion water were recently proposed to retrieve terrestrial temperature history. In order to accurately apply this newly-developed speleothem noble gas temperature (NGT) as a reliable proxy, a fundamental issue about behaviors of noble gases in the karst should be first clarified. In this study, we measured noble gas contents in air and dripping water to evaluate any ratio deviation between noble gases. Cave dripping water samples was collected from three selected caves, Shihua Cave in northern China, Furong Cave in southwestern, and Gyukusen Cave in an island located in the western Pacific. For these caves are characterized by a thorough mixing and long-term storage of waters in a karst aquifer by the absence of seasonal oxygen isotope shifts. Ratios of dripping water noble gases are statistically insignificant from air data. Helium isotopic ratios in the dripping water samples match air value. The results indicate that elemental and isotopic signatures of noble gases from air can be frankly preserved in the epikarst and support the fidelity of NGT techniques.

Cosmic ray exposure histories of Apollo 14, Apollo 15, and Apollo 16 rocks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eugster, O.; Eberhardt, P.

1984-02-15

The regolith exposure history of six rocks returned by the Apollo 14, 15, and 16 missions is studied based on the cosmogenic noble gas isotopes. For each sample, the complete set of all stable noble gas isotopes and the radiaoctive isotope Kr-81 were measured. Kr-81-Kr exposure ages are calculated for rocks for which a single-stage exposure can be demonstrated. A two-stage model exposure history is derived for multistage-exposure basalt 14310 based on the amounts and isotopic ratios of the cosmogenic noble gases. The apparent Kr-81-Kr age, the depth-sensitive isostopic ratios, and fission Xe-136 results lead to the conclusion that thismore » sample was preexposed 1.75 AE ago to cosmic rays for a duration of 350 m.y. Basalt 15058 and anorthosite 15415 also reveal multistage exposures. 44 references.« less

Method and apparatus for measuring purity of noble gases

DOEpatents

Austin, Robert

2008-04-01

A device for detecting impurities in a noble gas includes a detection chamber and a source of pulsed ultraviolet light. The pulse of the ultraviolet light is transferred into the detection chamber and onto a photocathode, thereby emitting a cloud of free electrons into the noble gas within the detection chamber. The cloud of electrons is attracted to the opposite end of the detection chamber by a high positive voltage potential at that end and focused onto a sensing anode. If there are impurities in the noble gas, some or all of the electrons within the cloud will bond with the impurity molecules and not reach the sensing anode. Therefore, measuring a lower signal at the sensing anode indicates a higher level of impurities while sensing a higher signal indicates fewer impurities. Impurities in the range of one part per billion can be measured by this device.

The Thermochemical Stability of Ionic Noble Gas Compounds.

ERIC Educational Resources Information Center

Purser, Gordon H.

1988-01-01

Presents calculations that suggest stoichiometric, ionic, and noble gas-metal compounds may be stable. Bases calculations on estimated values of electron affinity, anionic radius for the noble gases and for the Born exponents of resulting crystals. Suggests the desirability of experiments designed to prepare compounds containing anionic,…

Theoretical Calculation of the Electron Transport Parameters and Energy Distribution Function for CF3I with noble gases mixtures using Monte Carlo simulation program

NASA Astrophysics Data System (ADS)

Jawad, Enas A.

2018-05-01

In this paper, The Monte Carlo simulation program has been used to calculation the electron energy distribution function (EEDF) and electric transport parameters for the gas mixtures of The trif leoroiodo methane (CF3I) ‘environment friendly’ with a noble gases (Argon, Helium, kryptos, Neon and Xenon). The electron transport parameters are assessed in the range of E/N (E is the electric field and N is the gas number density of background gas molecules) between 100 to 2000Td (1 Townsend = 10-17 V cm2) at room temperature. These parameters, namely are electron mean energy (ε), the density –normalized longitudinal diffusion coefficient (NDL) and the density –normalized mobility (μN). In contrast, the impact of CF3I in the noble gases mixture is strongly apparent in the values for the electron mean energy, the density –normalized longitudinal diffusion coefficient and the density –normalized mobility. Note in the results of the calculation agreed well with the experimental results.

High energy primary knock-on process in metal deuterium systems initiated by bombardment with noble gas ions

NASA Astrophysics Data System (ADS)

Gann, V. V.; Tolstolutskaya, G. D.

2008-08-01

An experimental study confirms the possibility of nuclear fusion reactions initiating in metal-deuterium targets by bombarding them with ions that are not the reagents of the fusion reaction, in particular, with noble gas ions. The yields of (d,d) and (d,t) reactions were measured as functions of energy (0.4-3.2 MeV) and mass of incident ions (He +, Ne +, Ar +, Kr + and Xe +). Irradiation by heavy ions produced a number of energetic deuterium atoms in the deuteride and deuterium + tritium metal targets. At ion energies of ˜0.1-1 MeV the d-d reaction yields are relatively high. A model of nuclear fusion reaction cross-sections in atomic collision cascades initiated by noble gas ion beam in metal-deuterium target is developed. The method for calculation tritium or deuterium recoil fluxes and the yield of d-d fusion reaction in subsequent collisions was proposed. It was shown that D(d,p)t and D(t,n) 4He reactions mainly occur in energy region of the recoiled D-atom from 10 keV to 250 keV. The calculated probabilities of d-d and d-t fusion reactions were found to be in a good agreement with the experimental data.

Quasimolecular emission near the Xe(5p 56s 1,3 P 1 - 5p 6 1 S 0) and Kr (4p 55s 1,3 P 1 - 4p 6 1 S 0) resonance lines induced by collisions with He atoms

NASA Astrophysics Data System (ADS)

Alekseeva, O. S.; Devdariani, A. Z.; Grigorian, G. M.; Lednev, M. G.; Zagrebin, A. L.

2017-02-01

This study is devoted to the theoretical investigation of the quasimolecular emission of Xe*-He and Kr*-He collision pairs near the Xe (5p 56s 1,3 P 1 - 5p 6 1 S 0) and Kr (4p 55s 1,3 P 1 - 4p 6 1 S 0) resonance atomic lines. The potential curves of the quasimolecules Xe(5p 56s) + He and Kr(4p 55s) + He have been obtained with the use of the effective Hamiltonian and pseudopotential methods. Based on these potential curves the processes of quasimolecular emission of Xe*+He and Kr*+He mixtures have been considered and the spectral distributions I(ħΔω) of photons emitted have been obtained in the framework of quasistatic approximation.

The origin of hydrothermal and other gases in the Kenya Rift Valley

NASA Astrophysics Data System (ADS)

Darling, W. G.; Griesshaber, E.; Andrews, J. N.; Armannsson, H.; O'Nions, R. K.

1995-06-01

The Kenya Rift Valley (KRV) is part of a major continental rift system from which much outgassing is presently occurring. Previous research on gases in the KRV has tended to concentrate on their geothermal implications; the present paper is an attempt to broaden the interpretation by consideration of new data including helium and carbon isotope analyses from a wide cross-section of sites. In order to do this, gases have been divided into categories dependent on origin. N 2 and noble gases are for the most part atmospherically derived, although their relative concentrations may be altered from ASW ratios by various physical processes. Reduced carbon (CH 4 and homologues) appears to be exclusively derived from the shallow crust, with thermogenic δ 13C values averaging -25‰ PDB for CH 4. H 2 is likely also to be crustally formed. CO 2, generally a dominant constituent, has a narrow δ 13C range averaging -3.7‰ PDB, and is likely to be derived with little modification from the upper mantle. Consideration of the ratio C/ 3He supports this view in most cases. Sulphur probably also originates there. Ratios of 3He/ 4He reach a MORB-like maximum of 8.0 R/RA and provide the best indication of an upper mantle source of gases beneath the KRV. A correlation between 3He/ 4He and the hydrocarbon parameter log (C 1/ΣC 2-4) appears to be primarily temperature related. The highest 3He/ 4He ratios in spring waters are associated with basalts, perhaps because of the leaching of basalt glasses. There may be a structural control on 3He/ 4He ratios in the KRV as a whole.

Reconstructing temperatures in the Maritime Alps, Italy, since the Last Glacial Maximum using cosmogenic noble gas paleothermometry

NASA Astrophysics Data System (ADS)

Tremblay, Marissa; Spagnolo, Matteo; Ribolini, Adriano; Shuster, David

2016-04-01

The Gesso Valley, located in the southwestern-most, Maritime portion of the European Alps, contains an exceptionally well-preserved record of glacial advances during the late Pleistocene and Holocene. Detailed geomorphic mapping, geochronology of glacial deposits, and glacier reconstructions indicate that glaciers in this Mediterranean region responded to millennial scale climate variability differently than glaciers in the interior of the European Alps. This suggests that the Mediterranean Sea somehow modulated the climate of this region. However, since glaciers respond to changes in temperature and precipitation, both variables were potentially influenced by proximity to the Sea. To disentangle the competing effects of temperature and precipitation changes on glacier size, we are constraining past temperature variations in the Gesso Valley since the Last Glacial Maximum (LGM) using cosmogenic noble gas paleothermometry. The cosmogenic noble gases 3He and 21Ne experience diffusive loss from common minerals like quartz and feldspars at Earth surface temperatures. Cosmogenic noble gas paleothermometry utilizes this open-system behavior to quantitatively constrain thermal histories of rocks during exposure to cosmic ray particles at the Earth's surface. We will present measurements of cosmogenic 3He in quartz sampled from moraines in the Gesso Valley with LGM, Bühl stadial, and Younger Dryas ages. With these 3He measurements and experimental data quantifying the diffusion kinetics of 3He in quartz, we will provide a preliminary temperature reconstruction for the Gesso Valley since the LGM. Future work on samples from younger moraines in the valley system will be used to fill in details of the more recent temperature history.

He, Ne and Ar systematics in single vesicles: Mantle isotopic ratios and origin of the air component in basaltic glasses

NASA Astrophysics Data System (ADS)

Raquin, Aude; Moreira, Manuel Alexis; Guillon, Fabien

2008-09-01

An outstanding problem in understanding the origin of the gaseous phase, particularly the rare gas compositions in magmatic rocks, is the ubiquitous atmospheric component in bulk rock samples, and whether this atmospheric component is a late stage contamination of the sample, or a recycled component though sediments or altered oceanic crust. In the present study we address this problem by analyzing single vesicles from the "popping rock 2∏D43" sample from the Mid-Atlantic Ridge using a UV laser ablation system. We have determined both elemental and isotopic compositions of He, Ne and Ar in single vesicles as well as Kr and Xe abundances. All vesicles analyzed have an isotopic composition identical to the referred degassed mantle value estimated from this same sample, despite analyzing vesicles from a wide size distribution. The atmospheric component, which is always detected in bulk samples by crushing or heating, was not detected in the single vesicles. This implies that the recycling of atmospheric noble gases in the mantle cannot explain the air-like component of this sample. The addition of the atmospheric component must occur either during the eruption, or after sample recovery.

Ab initio molecular orbital studies of the vibrational spectra of the van der Waals complexes of boron trifluoride with the noble gases.

PubMed

Ford, Thomas A

2005-05-01

The molecular structures, interaction energies, charge transfer properties and vibrational spectra of the van der Waals complexes formed between boron trifluoride and the noble gases neon, argon, krypton and xenon have been computed using second and fourth order Møller-Plesset perturbation theory and the Los Alamos National Laboratory LANL2DZ basis set. The complexes are all symmetric tops, with the noble gas atom acting as a sigma electron donor along the C3 axis of the BF3 molecule. The interaction energies are all vanishingly small, and the amount of charge transferred in each case is of the order of 0.01e. The directions of the wavenumber shifts of the symmetric bending (nu2) and antisymmetric stretching (nu3) modes of the BF3 fragment confirm those determined experimentally, and the shifts are shown to correlate well with the polarizability of the noble gas atom and the inverse sixth power of the intermonomer separation. The nu2 mode is substantially more sensitive to complexation than the nu3 vibration.

Estimating the recharge properties of the deep ocean using noble gases and helium isotopes

NASA Astrophysics Data System (ADS)

Loose, Brice; Jenkins, William J.; Moriarty, Roisin; Brown, Peter; Jullion, Loic; Naveira Garabato, Alberto C.; Torres Valdes, Sinhue; Hoppema, Mario; Ballentine, Chris; Meredith, Michael P.

2016-08-01

The distribution of noble gases and helium isotopes in the dense shelf waters of Antarctica reflects the boundary conditions near the ocean surface: air-sea exchange, sea ice formation, and subsurface ice melt. We use a nonlinear least squares solution to determine the value of the recharge temperature and salinity, as well as the excess air injection and glacial meltwater content throughout the water column and in the precursor to Antarctic Bottom Water. The noble gas-derived recharge temperature and salinity in the Weddell Gyre are -1.95°C and 34.95 psu near 5500 m; these cold, salty recharge values are a result of surface cooling as well as brine rejection during sea ice formation in Antarctic polynyas. In comparison, the global value for deep water recharge temperature is -0.44°C at 5500 m, which is 1.5°C warmer than the southern hemisphere deep water recharge temperature, reflecting a distinct contribution from the north Atlantic. The contrast between northern and southern hemisphere recharge properties highlights the impact of sea ice formation on setting the gas properties in southern sourced deep water. Below 1000 m, glacial meltwater averages 3.5‰ by volume and represents greater than 50% of the excess neon and argon found in the water column. These results indicate glacial melt has a nonnegligible impact on the atmospheric gas content of Antarctic Bottom Water.

Using noble gas tracers to estimate residual CO2 saturation in the field: results from the CO2CRC Otway residual saturation and dissolution test

NASA Astrophysics Data System (ADS)

LaForce, T.; Ennis-King, J.; Paterson, L.

2013-12-01

Residual CO2 saturation is a critically important parameter in CO2 storage as it can have a large impact on the available secure storage volume and post-injection CO2 migration. A suite of single-well tests to measure residual trapping was conducted at the Otway test site in Victoria, Australia during 2011. One or more of these tests could be conducted at a prospective CO2 storage site before large-scale injection. The test involved injection of 150 tonnes of pure carbon dioxide followed by 454 tonnes of CO2-saturated formation water to drive the carbon dioxide to residual saturation. This work presents a brief overview of the full test sequence, followed by the analysis and interpretation of the tests using noble gas tracers. Prior to CO2 injection krypton (Kr) and xenon (Xe) tracers were injected and back-produced to characterise the aquifer under single-phase conditions. After CO2 had been driven to residual the two tracers were injected and produced again. The noble gases act as non-partitioning aqueous-phase tracers in the undisturbed aquifer and as partitioning tracers in the presence of residual CO2. To estimate residual saturation from the tracer test data a one-dimensional radial model of the near-well region is used. In the model there are only two independent parameters: the apparent dispersivity of each tracer and the residual CO2 saturation. Independent analysis of the Kr and Xe tracer production curves gives the same estimate of residual saturation to within the accuracy of the method. Furthermore the residual from the noble gas tracer tests is consistent with other measurements in the sequence of tests.

On the interatomic potentials for noble gas mixtures

NASA Astrophysics Data System (ADS)

Watanabe, Kyoko; Allnatt, A. R.; Meath, William J.

1982-07-01

Recently, a relatively simple scheme for the construction of isotropic intermolecular potentials has been proposed and tested for the like species interactions involving He, Ne, Ar, Kr and H 2. The model potential has an adjustable parameter which controls the balance between its exchange and Coulomb energy components. The representation of the Coulomb energy contains a damped multipolar dispersion energy series (which is truncated through O( R-10) and provides additional flexibility through adjustment of the dispersion energy coefficients, particularly C8 and C10, within conservative error estimates. In this paper the scheme is tested further by application to interactions involving unlike noble gas atoms where the parameters in the potential model are determined by fitting mixed second virial coefficient data as a function of temperature. Generally the approach leads to potential of accuracy comparable to the best available literature potentials which are usually determined using a large base of experimental and theoretical input data. Our results also strongly indicate the need of high quality virial data.

Xe/Kr Selectivity Measurements using AgZ-PAN at Various Temperatures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Garn, Troy Gerry; Greenhalgh, Mitchell Randy; Watson, Tony Leroy

2015-05-01

In preparation for planned FY-15 Xe/Kr multi-column testing, a series of experiments were performed to determine the selectivity of Xe over Kr using the silver converted mordenite-polyacrylonitrile (AgZ-PAN) sorbent. Results from these experiments will be used for parameter selection guidelines to define test conditions for Kr gas capture purity evaluations later this year. The currently configured experimental test bed was modified by installing a new cooling apparatus to permit future multi-column testing with independent column temperature control. The modified test bed will allow for multi-column testing to facilitate a Xe separation followed by a Kr separation using engineered form sorbents.more » Selectivity experiments were run at temperatures of 295, 250 and 220 K. Two feed gas compositions of 1000 ppmv Xe, 150 ppmv Kr in either a He or an air balance were used. AgZ-PAN sorbent selectivity was calculated using Xe and Kr capacity determinations. AgZ-PAN sorbent selectivities for Xe over Kr of 72 were calculated at room temperature (295 K) using the feed gas with a He balance and 34 using the feed gas with an air balance. As the test temperatures were decreased the selectivity of Xe over Kr also decreased due to an increase in both Xe and Kr capacities. At 220 K, the sorbent selectivities for Xe over Kr were 22 using the feed gas with a He balance and 28 using the feed gas with an air balance. The selectivity results indicate that AgZ-PAN used in the first column of a multi-column configuration will provide adequate partitioning of Xe from Kr in the tested temperature range to produce a more pure Kr end product for collection.« less

Defining Noble Gas Partitioning for Carbon Capture and Storage Environments

NASA Astrophysics Data System (ADS)

Warr, O.; Masters, A.; Rochelle, C.; Ballentine, C. J.

2014-12-01

For viable CCS implementation variables such as CO2 dissolution rates, reactions with the host rock and the extent of groundwater interaction must be accurately constrained. Noble gases play an important role in these systems [e.g. 1,2]. Their application, however, requires accurate Henry's constants within dense CO2-H2O systems. Current interpretations use pure noble gas-H2O partitioning data [3,4] and assume CO2-noble gas interactions are negligible, even at high (>700 kg/m3) CO2 densities [2]. To test this assumption we experimentally determined noble gas CO2-H2O partitioning for the 170-656 kg/m3 CO2 density range; representative of most CCS environments. Contrary to assumption, CO2 density significantly affected noble gas partition coefficients. For helium, increasing CO2 density resulted in a negative deviation trend from CO2-free values whilst for argon, krypton and xenon strong, positive deviations were observed. At 656 kg/m3 these deviations were -35%, 74%, 114% and 321% respectively. This is interpreted as the CO2 phase acting as a polar solvent inducing polarisation in the noble gases. Deviation trends are well defined using a 2nd order polynomial. The effect of a dense CO2 phase can now be incorporated into existing noble gas models. We also present results from a Gibbs-Ensemble Monte Carlo molecular simulation to model partitioning for this binary system. This fundamental technique makes predictions based on the pair-potentials of interaction between the molecules. Here it gives the phase compositions and Henry coefficients for noble gases. With a proven ability in accurately replicating both the CO2-H2O system and low pressure noble gas Henry constants the focus is now on fully optimising the model to match high pressure observations. [1] Gilfillan et al. (2009) Nature 458 614-618 [2] Gilfillan et al. (2008) GCA 72 1174-1198 [3] Crovetto et al. (1982) J.Chem.Phys. 76 1077-1086 [4] Ballentine et al. in Porcelli et al. (eds.) (2002) Rev.Min.Geo. 47 539-614.

Method for introduction of gases into microspheres

DOEpatents

Hendricks, C.D.; Koo, J.C.; Rosencwaig, A.

A method is described for producing small hollow glass spheres filled with a gas by introduction of the gas during formation of the hollow glass spheres. Hollow glass microspheres having a diameter up to about 500..mu.. with both thin walls (0.5 to 4/sub ..mu../) and thick walls (5 to 20/sub ..mu../) that contain various fill gases, such as Ar, Kr, Xe, Br, D, H/sub 2/, DT, He, N/sub 2/, Ne, CO/sub 2/, etc., in the interior thereof, can be produced by the diffusion of the fill gas or gases into the microsphere during the formation thereof from a liquid droplet of glass-form-forming solution. This is accomplished by filling at least a portion of the multiple-zone drop-furnace used in producing hollow microspheres with the gas or gases of interest, and then taking advantage of the high rate of gaseous diffusion of the fill gas through the wall of the gel membrane before it transforms into a glass microsphere as it is processed in the multiple-zone furnace.

MRI of the lung gas-space at very low-field using hyperpolarized noble gases

NASA Technical Reports Server (NTRS)

Venkatesh, Arvind K.; Zhang, Adelaide X.; Mansour, Joey; Kubatina, Lyubov; Oh, Chang Hyun; Blasche, Gregory; Selim Unlu, M.; Balamore, Dilip; Jolesz, Ferenc A.; Goldberg, Bennett B.;

Apparatus for preparing a solution of a hyperpolarized noble gas for NMR and MRI analysis

DOEpatents

Pines, Alexander [Berkeley, CA; Budinger, Thomas [Berkeley, CA; Navon, Gil [Ramat Gan, IL; Song, Yi-Qiao [Berkeley, CA; Appelt, Stephan [Waiblingen, DE; Bifone, Angelo [Rome, IT; Taylor, Rebecca [Berkeley, CA; Goodson, Boyd [Berkeley, CA; Seydoux, Roberto [Berkeley, CA; Room, Toomas [Albany, CA; Pietrass, Tanja [Socorro, NM

2008-06-10

The present invention relates generally to nuclear magnetic resonance (NMR) techniques for both spectroscopy and imaging. More particularly, the present invention relates to methods in which hyperpolarized noble gases (e.g., Xe and He) are used to enhance and improve NMR and MRI. Additionally, the hyperpolarized gas solutions of the invention are useful both in vitro and in vivo to study the dynamics or structure of a system. When used with biological systems, either in vivo or in vitro, it is within the scope of the invention to target the hyperpolarized gas and deliver it to specific regions within the system.

Signal-to-noise ratio comparison of encoding methods for hyperpolarized noble gas MRI

NASA Technical Reports Server (NTRS)

Zhao, L.; Venkatesh, A. K.; Albert, M. S.; Panych, L. P.

2001-01-01

Some non-Fourier encoding methods such as wavelet and direct encoding use spatially localized bases. The spatial localization feature of these methods enables optimized encoding for improved spatial and temporal resolution during dynamically adaptive MR imaging. These spatially localized bases, however, have inherently reduced image signal-to-noise ratio compared with Fourier or Hadamad encoding for proton imaging. Hyperpolarized noble gases, on the other hand, have quite different MR properties compared to proton, primarily the nonrenewability of the signal. It could be expected, therefore, that the characteristics of image SNR with respect to encoding method will also be very different from hyperpolarized noble gas MRI compared to proton MRI. In this article, hyperpolarized noble gas image SNRs of different encoding methods are compared theoretically using a matrix description of the encoding process. It is shown that image SNR for hyperpolarized noble gas imaging is maximized for any orthonormal encoding method. Methods are then proposed for designing RF pulses to achieve normalized encoding profiles using Fourier, Hadamard, wavelet, and direct encoding methods for hyperpolarized noble gases. Theoretical results are confirmed with hyperpolarized noble gas MRI experiments. Copyright 2001 Academic Press.

The solubility of rare gases in fused silica: A numerical evaluation

NASA Astrophysics Data System (ADS)

Guillot, Bertrand; Guissani, Yves

1996-07-01

The solubility of rare gases in a simulated model of fused silica is evaluated by the test particle method. It is shown that the order of magnitude of the rare gas solubility in liquid silica is mainly governed by the entropy of cavity formation and only marginally by the solvation energy of the solute in the melt. Hence, the hierarchy of solubilities is dictated by the size of the noble gases: The smaller the atom the higher the solubility. Moreover, the solubility exhibits only a moderate temperature dependence at fixed density. In silica glass the same solubility hierarchy is found (in agreement with the experimental data) although the energetic contribution to the absorption process may become significant, particularly when the temperature decreases. These results in silica are in strong contrast with those obtained in liquid water where the energetic contribution to the rare gas solubility is large enough to overcompensate the entropic loss of cavity formation, the net result being that light noble gases (e.g., He) are less soluble than heavier ones (e.g., Xe). These contrasting behaviors are explained by pointing out that the liquid phase occurs in very different temperature ranges for these two systems (SiO2 and H2O) while the rare gas-solvent interaction energy is essentially of the same order of magnitude. Finally, the structure of silica around helium and neon atoms is found to be interstitial (cristobalitelike) while in the case of heavier rare gases, the structure of cavities is more reminiscent of the polyhedral arrangement encountered with clathrasils.

Kr/Xe Separation over a Chabazite Zeolite Membrane

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feng, Xuhui; Zong, Zhaowang; Elsaidi, Sameh K.

2016-08-10

Cryogenic distillation, the current conventional technology to separate Krypton and Xenon from air, and from nuclear reprocessing technologies, is an energy-intensive and expensive process. Membrane technology could potentially make this challenging industrial separation less energy intensive and economically viable. We demonstrate that chabazite zeolite SAPO-34 membranes effectively separated Kr/Xe gas mixtures at industrially relevant compositions. Control over membrane thickness and average crystal size led to industrial range permeances and high separation selectivities. Specifically, SAPO-34 membranes can separate Kr/Xe mixtures with Kr permeances as high as 361.4 GPU and separation selectivities of 34.8 for molar compositions close to typical concentrations ofmore » these two gases in air. In addition, SAPO-34 membranes separated Kr/Xe mixtures with Kr permeances as high as 525.7 GPU and separation selectivities up to 45.1 for molar compositions as might be encountered in nuclear reprocessing technologies. Molecular sieving and differences in diffusivities were identified as the dominant separation mechanisms.« less

The temperature and precipitation reconstructions on Swiss stalagmites with a special emphasis on altitude gradient using noble-gases, δO-18 and δD of fluid inclusions

NASA Astrophysics Data System (ADS)

Ghadiri, Elaheh; Brennwald, Matthias; Kipfer, Rolf

2017-04-01

We present the results of an application of 'Combined Vacuum Crushing and Sieving (CVCS)' system (e.g., allowing to crush samples to defined grain size in vacuum) for the first time to stalagmites grown in cold climates during the last glacial-interglacial transition, but at different altitudes. Recently, concentrations of dissolved atmospheric noble gases in fluid inclusions of stalagmites were used to reconstruct past ambient cave temperatures, the annual mean temperature and hydrological conditions when the water was trapped. To reconstruct temperatures from noble gases (noble gas temperature: NGT) in water-filled inclusions, we processed samples from Swiss stalagmites M6 from Milandre cave (400 m.a.s.l) and GEF1 from Grotte aux Fées cave (895 m.a.s.l) covering the climatic transitions Allerød-Younger Dryas-Holocene. Water content. The amount of water extracted per unit mass of calcite fabric (e.g., 'water yield': WT) was shown to be a measure of the total water content. The data shows that the WT systematically changes with δ18Ocalcite of the calcite. We therefore conclude that WT records can be linked on changes in drip rates and thus can be used to track changes of past precipitation even in cold regions. Noble gases. Noble gas analysis shows that the annual mean temperatures in Milandre cave were 2.2±2.0°C during the late Allerød and dropped to 0±2°C at the Younger Dryas. Such temperatures close 0°C indicate that drip water supply stopped in response to the formation of permafrost conditions around the cave preventing further stalagmite growth. However, one late Holocene sample gave a cave temperature of 8.7±1.4°C agreeing generally with present day annual mean temperature. The annual mean temperature of 5.7±1.3°C from GEF1 was determined for the early Holocene. The observed data show systematic variations with sample elevation, e.g., higher temperature from lower altitude and vice versa. Combining the isotopic composition of water in fluid

Appraisal of transport and deformation in shale reservoirs using natural noble gas tracers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heath, Jason E.; Kuhlman, Kristopher L.; Robinson, David G.

2015-09-01

This report presents efforts to develop the use of in situ naturally-occurring noble gas tracers to evaluate transport mechanisms and deformation in shale hydrocarbon reservoirs. Noble gases are promising as shale reservoir diagnostic tools due to their sensitivity of transport to: shale pore structure; phase partitioning between groundwater, liquid, and gaseous hydrocarbons; and deformation from hydraulic fracturing. Approximately 1.5-year time-series of wellhead fluid samples were collected from two hydraulically-fractured wells. The noble gas compositions and isotopes suggest a strong signature of atmospheric contribution to the noble gases that mix with deep, old reservoir fluids. Complex mixing and transport of fracturingmore » fluid and reservoir fluids occurs during production. Real-time laboratory measurements were performed on triaxially-deforming shale samples to link deformation behavior, transport, and gas tracer signatures. Finally, we present improved methods for production forecasts that borrow statistical strength from production data of nearby wells to reduce uncertainty in the forecasts.« less

Ab initio studies of the Rg–NO{sup +}(X{sup 1}Σ{sup +}) van der Waals complexes (Rg = He, Ne, Ar, Kr, and Xe)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Orek, Cahit; Bulut, Niyazi, E-mail: jklos@umd.edu, E-mail: francois.lique@univ-lehavre.fr, E-mail: bulut-niyazi@yahoo.com; Kłos, Jacek, E-mail: jklos@umd.edu, E-mail: francois.lique@univ-lehavre.fr, E-mail: bulut-niyazi@yahoo.com

2016-05-28

We used the explicitly correlated variant of the coupled clusters method with single, double, and noniterative triple excitations [CCSD(T)-F12] to compute two-dimensional potential energy surfaces of van der Waals complexes formed by rare gas atoms (Rg) and NO{sup +}(X{sup 1}Σ{sup +}) cations. We used the correlation-consistent, triple-zeta (cc-pVTZ-F12) atomic basis sets, and for Kr and Xe rare gases, we employed corresponding pseudopotential cc-pVTZ-PP-F12 atomic basis sets. These basis sets were additionally augmented with mid-bond functions. The complexes are all of skewed T-shape type with Rg atom being closer to the N-side. Using analytical representation of the potentials, we have estimatedmore » zero-point energy corrected dissociation energies from anharmonic calculations with BOUND program and also from the harmonic approximation. The binding energies increase with the polarization of the Rg atom in series from He to Xe and are 196 cm{sup −1}, 360 cm{sup −1}, 1024 cm{sup −1}, 1434 cm{sup −1}, and 2141 cm{sup −1}, respectively. Their corresponding dissociation energies are 132 cm{sup −1}, 300 cm{sup −1}, 927 cm{sup −1}, 1320 cm{sup −1}, and 1994 cm{sup −1} for the complexes with He to Xe, respectively. We find good agreement with previous theoretical and experimental results. The harmonic vibrational frequencies were calculated for the bending and stretching modes of the Rg–NO{sup +} complexes.« less

The determination of accurate dipole polarizabilities alpha and gamma for the noble gases

NASA Technical Reports Server (NTRS)

Rice, Julia E.; Taylor, Peter R.; Lee, Timothy J.; Almloef, Jan

1989-01-01

The static dipole polarizabilities alpha and gamma for the noble gases helium through xenon were determined using large flexible one-particle basis sets in conjunction with high-level treatments of electron correlation. The electron correlation methods include single and double excitation coupled-cluster theory (CCSD), an extension of CCSD that includes a perturbational estimate of connected triple excitations, CCSD(T), and second order perturbation theory (MP2). The computed alpha and gamma values are estimated to be accurate to within a few percent. Agreement with experimental data for the static hyperpolarizability gamma is good for neon and xenon, but for argon and krypton the differences are larger than the combined theoretical and experimental uncertainties. Based on our calculations, we suggest that the experimental value of gamma for argon is too low; adjusting this value would bring the experimental value of gamma for krypton into better agreement with our computed result. The MP2 values for the polarizabilities of neon, argon, krypton and zenon are in reasonabe agreement with the CCSD and CCSD(T) values, suggesting that this less expensive method may be useful in studies of polarizabilities for larger systems.

Volatile elements - water, carbon, nitrogen, noble gases - on Earth

NASA Astrophysics Data System (ADS)

Marty, B.

2017-12-01

Understanding the origin and evolution of life-bearing volatile elements (water, carbon, nitrogen) on Earth is a fruitful and debated area of research. In his pioneering work, W.W. Rubey inferred that the terrestrial atmosphere and the oceans formed from degassing of the mantle through geological periods of time. Early works on noble gas isotopes were consistent with this view and proposed a catastrophic event of mantle degassing early in Earth's history. We now have evidence, mainly from noble gas isotopes, that several cosmochemical sources contributed water and other volatiles at different stages of Earth's accretion. Potential contributors include the protosolar nebula gas that equilibrated with magma oceans, inner solar system bodies now represented by chondrites, and comets. Stable isotope ratios suggest volatiles where primarily sourced by planetary bodies from the inner solar system. However, recent measurements by the European Space Agency Rosetta probe on the coma of Comet 67P/Churyumov-Gerasimenko permit to set quantitative constraints on the cometary contribution to the surface of our planet. The surface and mantle reservoirs volatile elements exchanged volatile elements through time, with rates that are still uncertain. Some mantle regions remained isolated from whole mantle convection within the first tens to hundreds million years after start of solar system formation. These regions, now sampled by some mantle plumes (e.g., Iceland, Eifel) preserved their volatile load, as indicated by extinct and extant radioactivity systems. The abundance of volatile elements in the mantle is still not well known. Different approaches, such as high pressure experimental petrology, noble gas geochemistry, modelling, resulted in somewhat contrasted estimates, varying over one order of magnitude for water. Comparative planetology, that is, the study of volatiles on the Moon, Venus, Mars, Vesta, will shed light on the sources and strengths of these elements in the

Genesis Noble Gas Measurements

NASA Technical Reports Server (NTRS)

Hohenberg, Charles M.

2005-01-01

The original thrust of our Genesis funding was to extend and refine the noble gas analytical capabilities of this laboratory to improve the precision and accuracy of noble gas measurements in order to optimize the scientific return from the Genesis Mission. This process involved both instrumental improvement (supplemented by a SRLIDAP instrument grant) and refinement of technique. The Genesis landing mishap shifted our emphasis to the irregular aluminum heat shield material from the flat collector wafers. This has required redesign of our laser extraction cells to accommodate the longer focal lengths required for laser extraction from non-flat surfaces. Extraction of noble gases from solid aluminum surfaces, rather than thin coatings on transparent substrates has required refinement of controlled-depth laser ablation techniques. Both of these bring new problems, both with potentially higher blanks form larger laser cells and the larger quantities of evaporated aluminum which can coat the sapphire entrance ports. This is mainly a problem for the heavy noble gases where larger extraction areas are required, necessitating the new aluminum vapor containment techniques described below. With the Genesis Mission came three new multiple multiplier noble gas mass spectrometers to this laboratory, one built solely by us (Supergnome-M), one built in collaboration with Nu-Instruments (Noblesse), and one built in collaboration with GVI (Helix). All of these have multiple multiplier detection sections with the Nu-Instruments using a pair of electrostatic quad lenses for isotope spacing and the other two using mechanically adjustable positions for the electron multipliers. The Supergnome-M and Noblesse are installed and running. The GVI instrument was delivered a year late (in March 2005) and is yet to be installed by GVI. As with all new instruments there were some initial development issues, some of which are still outstanding. The most serious of these are performance issues

The ATTA-Hefei Instrument for Radioactive Noble-gas Dating

NASA Astrophysics Data System (ADS)

Hu, S.; Cheng, C.; Cheng, G.; Sun, Y. R.; Tu, L.; Yang, G.

2013-12-01

Long-lived noble-gas isotopes 85Kr (10.8 y), 39Ar (269 y) and 81Kr (229 ky) are ideal tracers for dating environmental samples such as groundwater and ice. Together with 14C, these nuclides can be used to cover the whole range of 100-106 y. Atom Trap Trace Analysis (ATTA) is an emerging method for the analysis of these isotopes at an isotopic abundance level as low as 10^-16 [1,2]. The ATTA instrument built in Hefei, China, can determine the isotopic abundances of 85Kr and 81Kr with typically 5-10% accuracy using krypton gas samples of a few micro-liters (STP) krypton gas [3]. The krypton gas sample can be extracted from several liters of air using a distillation-chromatograph setup with a typical efficiency of 85%, while the air sample can be extracted from groundwater or ices. The typical sample size for ATTA measurement is 100L groundwater or 40Kg ices. One such ATTA beamline can handle about 100 samples per year. [1] Chen, C. Y. et al. Ultrasensitive isotope trace analyses with a magneto-optical trap. Science 286, 1139-1141 (1999). [2] Jiang, W. et al. 39Ar detection at the 10-16 isotopic abundance level with atom trap trace analysis. Phys. Rev. Lett. 106, 103001 (2011). [3] Yang, G. -M. et al. Analysis of 85Kr: a comparison at the 10-14 level using micro-liter samples, Sci. Rep. 3, 1596 (2013). Relative uncertainty of the determined 85Kr abundance by the ATTA-Hefei instrument.

Initial results of noble gases in micrometeorites from the Transantarctic Mountains, Antarctica

NASA Astrophysics Data System (ADS)

Baecker, B.; Cordier, C.; Folco, L.; Trieloff, M.; Ott, U.

2012-12-01

The bulk of extraterrestrial matter collected by Earth is in the form of micrometeorites, which have a main flux onto Earth at about 220 μm in diameter [1]. According to the petrographic and geochemical data, most of the small micrometeorites have been related to CM chondrites [2]. Recent studies suggest that larger micrometeorites (> 300μm) mostly derive from ordinary chondrite sources e.g. [3-5]. Following some models [6], they may have made important contributions to the volatile inventory of the Earth. We have initiated a coupled comprehensive survey of noble gas contents and petrography in micrometeorites. While helium and neon are generally dominated by the solar wind contribution, the inventory of heavy primordial noble gases has been hardly characterized so far. In particular, useful data are lacking on the diagnostic isotopic composition of xenon. We hope to fill this gap, since huge amounts of material are available. This might make a contribution towards understanding some aspects of the formation of the solar system and in particular the terrestrial atmosphere. We will present results obtained on "large" micrometeorites from Victoria Land, Transantarctic Mountains. These were collected during a PNRA (Programma Nazionale delle Ricerche in Antartide, Italy) expedition on top of the Miller Butte micrometeorite traps #45 b and c [7]. We reported first results in [8]. Our research includes however, also material from other collections, e.g. CONCORDIA [9, 10]. [1] Love, S.G., Brownlee, D.E. (1993) Science 262, 550-553. [2] Kurat, G. et al. (1994) Geochimica et Cosmochimica Acta 58, 3879-3904. [3] Genge, M.J. et al. (2008) Meteoritics & Planetary Science 43, 497-515. [4] Dobrica, E. et al. (2011) Meteoritics & Planetary Science 46, 1363-1375. [5] Van Ginneken M. et al. (2012) Meteoritics & Planetary Science 47, 228-247. [6] Maurette, M. et al. (2000) Planetary and Space Science 48, 1117-1137. [7] Rochette P. et al. (2008) Proceedings of the National Academy

Not all Primordial Noble Gas Signatures are Associated with OIBs and Mantle Plumes - Mantle Heterogeneity, Primordial Shallow Sources and a Solar-like He, Ne Signature in an Ancient North American Craton

NASA Astrophysics Data System (ADS)

Ma, L.; Castro, M. C.; Hall, C. M.

2007-12-01

The presence of primordial He and Ne components in ocean island basalts (OIBs) as well as a mantle He/heat flux ratio lower than the production ratio near mid-ocean ridges have historically been used to support the existence of a two-layer mantle convection model. This would comprise a lower, primordial, undegassed reservoir from which He removal to the upper degassed mantle would be impeded. Arguments based on He and heat transport have been recently invalidated by Castro et al. (2005) and should no longer be used to justify the presence of two such distinct mantle reservoirs. Indeed, it was shown that such low He/heat flux ratios are expected and do not reflect a He deficit in the original crust or mantle reservoir. By contrast, the occurrence of a He/heat flux ratio greater than the radiogenic production ratio can only result from a past mantle thermal event in which the released heat has already escaped while the released He remains, and is slowly rising to the surface. Such a high He/heat flux ratio is present in shallow groundwaters of the Michigan Basin. We now present results of a new noble gas study conducted in the Michigan Basin, in which 38 deep (0.5-3.6km) brine samples were collected and analyzed for all noble gas abundances and isotopic ratios. As expected from previously computed shallow high He/heat flux ratios, both He and Ne isotopic ratios clearly indicate the presence of a mantle component. Of greater significance is the primordial, solar-like signature, of this mantle component. It is also the first primordial signature ever recorded in crustal fluids in a continental region. Because no hotspots or hotspot tracks are known in the area, it is highly unlikely for such primordial, solar-like signature to result from a mantle plume-related mechanism originating deep in the mantle. We argue that such a primordial signature can be explained by a shallow noble gas reservoir in the subcontinental lithospheric mantle (SCLM) beneath the Michigan Basin

Structural Measurements from Images of Noble Gas Diffusion

NASA Astrophysics Data System (ADS)

Cadman, Robert V.; Kadlecek, Stephen J.; Emami, Kiarash; MacDuffie Woodburn, John; Vahdat, Vahid; Ishii, Masaru; Rizi, Rahim R.

2009-03-01

Magnetic resonance imaging of externally polarized noble gases such as ^3He has been used for pulmonary imaging for more than a decade. Because gas diffusion is impeded by the alveoli, the diffusion coefficient of gas in the lung, measured on a time scale of milliseconds, is reduced compared to that of the same gas mixture in the absence of restrictions. When the alveolar walls decay, as in emphysema, diffusivity in the lung increases. In this paper, the relationship between diffusion measurements and the size of the restricting structures will be discussed. The simple case of diffusion in an impermeable cylinder, a structure similar to the upper respiratory airways in mammals, has been studied. A procedure will be presented by which airways of order 2 mm in diameter may be accurately measured; demonstration experiments with plastic tubes will also be presented. The additional developments needed before this technique becomes practical will be briefly discussed.

Characterizing the Noble Gas Isotopic Composition of the Barnett Shale and Strawn Group and Constraining the Source of Stray Gas in the Trinity Aquifer, North-Central Texas.

PubMed

Wen, Tao; Castro, M Clara; Nicot, Jean-Philippe; Hall, Chris M; Pinti, Daniele L; Mickler, Patrick; Darvari, Roxana; Larson, Toti

2017-06-06

This study presents the complete set of stable noble gases for Barnett Shale and Strawn Group production gas together with stray flowing gas in the Trinity Aquifer, Texas. It places new constraints on the source of this stray gas and further shows that Barnett and Strawn gas have distinct crustal and atmospheric noble gas signatures, allowing clear identification of these two sources. Like stray gas, Strawn gas is significantly more enriched in crustal 4 He*, 21 Ne*, and 40 Ar* than Barnett gas. The similarity of Strawn and stray gas crustal noble gas signatures suggests that the Strawn is the source of stray gas in the Trinity Aquifer. Atmospheric 22 Ne/ 36 Ar ratios of stray gas mimic also that of Strawn, further reinforcing the notion that the source of stray gas in this aquifer is the Strawn. While noble gas signatures of Strawn and stray gas are consistent with a single-stage water degassing model, a two-stage oil modified groundwater exsolution fractionation model is required to explain the light atmospheric noble gas signature of Barnett Shale production gas. These distinct Strawn and Barnett noble gas signatures are likely the reflection of distinct evolution histories with Strawn gas being possibly older than that of Barnett Shale.

A first-principles study of He, Xe, Kr and O incorporation in thorium carbide

NASA Astrophysics Data System (ADS)

Pérez Daroca, D.; Llois, A. M.; Mosca, H. O.

2015-05-01

Thorium-based materials are currently being investigated in relation with their potential utilization in Generation-IV reactors as nuclear fuels. Understanding the incorporation of fission products and oxygen is very important to predict the behavior of nuclear fuels. A first approach to this goal is the study of the incorporation energies and stability of these elements in the material. By means of first-principles calculations within the framework of density functional theory, we calculate the incorporation energies of He, Xe, Kr and O atoms in Th and C vacancy sites, in tetrahedral interstitials and in Schottky defects along the 〈1 1 1〉 and 〈1 0 0〉 directions. We also analyze atomic displacements, volume modifications and Bader charges. This kind of results for ThC, to the best authors' knowledge, have not been obtained previously, neither experimentally, nor theoretically. This should deal as a starting point towards the study of the complex behavior of fission products in irradiated ThC.

In Situ measurement of Kr and Xe in the atmosphere of Mars

NASA Astrophysics Data System (ADS)

Conrad, P. G.; Malespin, C.; Franz, H. B.; Trainer, M. G.; Pepin, R. O.; Schwenzer, S. P.; Manning, H. L.; Atreya, S. K.; Wong, M. H.; Jones, J. H.; Owen, T. C.; Mahaffy, P. R.

2015-12-01

Abstract: The Sample Analysis at Mars (SAM) investigation [1] on NASA's Mars Science Laboratory mission has measured the six stable isotopes of krypton and the nine stable isotopes of xenon from the surface of Mars. Using semi-static mass spectrometry (MS) to measure the Kr, and static MS experiments (first ever on another planet) to measure the xenon, we have obtained isotopic ratios of these heavy noble gas elements with greatly improved precision over the Viking Measurements. The Viking landers detected both Kr and Xe [2] with a reported precision of ±20%, insufficient for in situ isotope measurement. Using the Viking observation of high 129Xe relative to Earth or to solar wind, Bogard & Johnson [3] and Swindle et al. [4] recognized that Shergottite meteorites may hold trapped Martian atmosphere, from which Swindle's team later reported precise noble gas isotope ratios, solidifying the theory that these meteorites were of martian origin. Our data are in very good agreement with the Swindle et al. [4] analysis, and the isotopic distributions of Kr and Xe in present day Martian atmosphere support the Pepin [5] model of massive hydrodynamic escape of the martian atmosphere early after formation. References: [1] Mahaffy, Paul R., et al. Space Science Revs 170.1-4 (2012): 401-478. [2] Owen, T., et al. Science 194.4271 (1976): 1293-1295. [3] Bogard, D. D. & Johnson, P. (1983) Science, 221: 651-654. [4] Swindle, T. D., M. W. Caffee, and C. M. Hohenberg. Geochim et Cosmochim Acta 50.6 (1986): 1001-1015. [5] Pepin, Robert O. Icarus 111.2 (1994): 289-304.

Gaseous 83mKr generator of monoenergetic electrons based on 83Rb deposited in zeolite

NASA Astrophysics Data System (ADS)

Sentkerestiová, J.; Vénos, D.; Slezák, M.

2017-09-01

The gaseous 83mKr electron source is currently used in neutrino mass experiments KATRIN and Project 8, dark matter experiments XENON, LUX and DarkSide, and ALICE (CERN) experiment. The main attractive features of this radioactive noble gas are its monoenergetic conversion electrons with well known energies and a half-life of 1.8 h, which is short enough to avoid any long-lasting contamination of the system. The long half-life of the mother 83Rb isotope (T1/2 = 86.2 d) enables more time demanding measurement. Particularly, in the neutrino mass experiments with gaseous tritium in which the 83mKr is applied in the same manner as the tritium, the K-32 conversion electrons with energy conveniently close to the beta spectrum endpoint represent an important test and calibration tool. Here, the design and characteristics of the gaseous 83mKr generator, including the 83mKr source itself, for KATRIN (KArlsruhe TRItium Neutrino) experiment are presented.

Carbynes - Carriers of primordial noble gases in meteorites

NASA Technical Reports Server (NTRS)

Whittaker, A. G.; Watts, E. J.; Lewis, R. S.; Anders, E.

1980-01-01

Five carbynes (triply bonded allotropes of carbon) have been found by electron diffraction in the Allende and Murchison carbonaceous chondrites: carbon VI, VIII, X, XI, and (tentatively) XII. From the isotopic composition of the associated noble-gas components, it appears that the carbynes in Allende (C3V chondrite) are local condensates from the solar nebula, whereas at least two carbynes in Murchison (C2 chondrite) are of exotic, presolar origin. They may be dust grains that condensed in stellar envelopes and trapped isotropically anomalous matter from stellar nucleosynthesis.

Noble gas trapping and fractionation during synthesis of carbonaceous matter. [in meteorites

NASA Technical Reports Server (NTRS)

Frick, U.; Mack, R.; Chang, S.

1979-01-01

An investigation of noble gas entrapment during synthesis of carbonaceous, macromolecular, and kerogen-like substances is presented. High molecular weight organic matter synthesized in aqueous condensation reactions contained little gas, and the composition was consistent with fractionation due to noble gas solubility in water; however, propane soot produced during a modified Miller-Urey experiment in an aritificial gas mixture contained high concentrations of trapped noble gases that displayed strong elemental fractionation from their reservoirs. It is concluded that theses experiemnts show that processes exist for synthesis of carbonaceous carriers that result in high noble gas concentrations and strong elemental fractionation at temperatures well above those required by absorption to achieve similar effects.

Noble Gas Isotopic Signatures and X-Ray and Electron Diffraction Characteristics of Tagish Lake Carbonaceous Chondrite

NASA Technical Reports Server (NTRS)

Nakamura, T.; Noguchi, T.; Zolensky, M. E.; Takaoka, N.

2001-01-01

Noble gas isotopic signatures and X-ray and electron diffraction characteristics of Tagish Lake indicate that it is a unique carbonaceous chondrite rich in saponite, Fe-Mg-Ca carbonate, primordial noble gases, and presolar grains. Additional information is contained in the original extended abstract.

Removal of I, Rn, Xe and Kr from off gas streams using PTFE membranes

DOEpatents

Siemer, Darryl D.; Lewis, Leroy C.

1990-01-01

A process for removing I, R, Xe and Kr which involves the passage of the off gas stream through a tube-in-shell assembly, whereby the tubing is a PTFE membrane which permits the selective passages of the gases for removing and isolating the gases.

Removal of I, Rn, Xe and Kr from off gas streams using PTFE membranes

DOEpatents

Siemer, Darryl D.; Lewis, Leroy C.

1990-08-07

A process for removing I, R, Xe and Kr which involves the passage of the off gas stream through a tube-in-shell assembly, whereby the tubing is a PTFE membrane which permits the selective passages of the gases for removing and isolating the gases.

Looking for a correlation between terrestrial age and noble gas record of H chondrites

NASA Astrophysics Data System (ADS)

Loeken, Th.; Schultz, L.

1994-07-01

On the basis of statistically significant concentration differences of some trace elements, it has been suggested that H chondrites found in Antarctica and Modern Falls represent members of different extraterrestrial populations with different thermal histories. It was also concluded that H chondrites found in Victoria Land (Allan Hills) differ chemically from those found in Queen Maud Land (Yamato Mountains), an effect that could be based on the different terrestrial age distribution of both groups. This would imply a change of the meteoroid flux hitting the Earth on a timescale that is comparable to typical terrestrial ages of Antarctic chondrites. A comparison of the noble gas record of H chondrites from the Allan Hills icefields and Modern Fall shows that the distributions of cosmic-ray exposure ages and the concentrations of radiogenic He-4 and Ar-40 are very similar. In an earlier paper we compared the noble gas measurements of 20 Yamato H contents with meteorites from the Allan Hills region and Modern Falls. Similar distributions were found. The distribution of cosmic-ray exposure ages and radiogenic He-4 and Ar-40 gas contents as a function of the terrestrial age is investigated in these chondrites. The distribution shows the well-known 7-Ma-cluster indicating that about 40% of the H chondrites were excavated from their parent body in a single event. Both populations, Antarctic Meteorites and Modern Falls, exhibit the same characteristic feature: a major meteoroid-producing event about 7 Ma. This indicates that one H-group population delivers H chondrites to Antarctica and the rest of the world. Cosmic-ray exposure ages and thermal-history indicaters like radiogenic noble gases show no evidence of a change in the H chondrite meteoroid population during the last 200,000 years.

David Noble's Battle to Defend the 'Sacred Space' of the Classroom.

ERIC Educational Resources Information Center

Young, Jeffrey R.

2000-01-01

Reports on the crusade of David F. Noble, a history professor at York University (Ontario), against distance education, which he sees as the latest episode in the saga of the corporatization of American higher education. Notes Noble's views on the relationship between politics and technology, intellectual property issues of courseware, and the…

Where is the Earth's missing xenon?

NASA Technical Reports Server (NTRS)

Wacker, J. F.; Anders, E.

1984-01-01

Highly volatile elements (e.g., T1, Pb, B, C1, Br, etc.) in the Earth's crust occur in C-chondrite proportions, and so do the atmospheric noble gases Ne, Ar, and Kr. This has led to the suggestion that the Earth acquired its volatiles from a late veneer of C-chondrite-like material. A glaring exception is Xe, which is depleted approx. 20x relative to Ne, Ar, Kr. Three explanations are discussed for the depletion: (1) Xe is preferentially trapped in the crust, either in sediments (3) or in Antarctic ice (4); (2) the Earth's noble gas inventory is non-chondritic (5); or (3) Xe is incompletely outgassed from the mantle.

Infrared spectroscopy of isoprene in noble gas matrices

NASA Astrophysics Data System (ADS)

Ito, Fumiyuki

2018-06-01

In this study, the infrared absorption spectra of 2-methyl-1,3-butadiene (isoprene) in noble gas matrices (Ar, Kr, and Xe) have been reported. The vibrational structure observed at cryogenic temperature, in combination with anharmonic vibrational calculations using density functional theory, helped in unambiguously assigning the fundamental modes of isoprene unresolved in the previous gas phase measurements, which would be of basic importance in the remote sensing of this molecule. A careful comparison with the most recent gas phase study [Brauer et al., Atmos. Meas. Tech. 7 (2014) 3839-3847.] led us to alternative assignments of the weak bands.

Gas geochemistry of Sierra Negra volcano, Galapagos hot spot

NASA Astrophysics Data System (ADS)

Taran, Y.; Christenson, B.; Sumino, H.; Kennedy, B.

2010-12-01

We report chemical and isotopic compositions of gases from the Mina Azufral fumarolic field of Sierra Negra volcano, Isabela Island, Galápagos, collected in 2004 and compare our data with the data by Giggenbach (unpublished) collected in 1990 and Goff et al. (2000) collected in 1995. New results include the noble gas elemental and isotope abundances and nitrogen isotope ratios for the discharges. Maximum fumarole temperatures and ratios of major components (C/S/Cl/N) changed very little between 1995 and 2004, but the water fraction varied significantly over this period (39 mol% in 1990; 77% in 1995 and 52% in 2004). Carbon and helium isotopic compositions were stable (-3 to -4‰ and 16-18Ra, respectively), and water isotopic composition showed a notable negative oxygen shift from the local meteoric water value depending on the relative water content and thus controlled by the H2O-CO2 oxygen isotope fractionation. In terms of the noble gas abundances and isotopic ratios, heavy noble gases (Kr and Xe) are mainly of the atmospheric origin. Ne isotopic ratios also show strong meteoric signatures, but fall along the 20Ne/22Ne - 21Ne/22Ne air-deep mantle mixing trend for Fernandina glasses (Kurz et al., 2009). 40Ar/36Ar ratios up to 400 show a notable contribution of radiogenic Ar, and 40Ar*/4He ~ 0.3 ratios are consistent with un-degassed upper mantle values. Despite the high He/Ne ratios in gases collected in 2004, and only trace air contamination attributable to sampling, the nitrogen isotope ratios (~ -1 ‰) show a high fraction of the air-saturated water in the volcanic vapor. The chemical composition of the parent magmatic gas is difficult to characterise due to significant interaction between magmatic and hydrothermal system fluids beneath the Sierra Negra caldera. Never-the-less, some important indicators can be estimated: CO2/3He ≈ 3.5x10^9; N2/He <30; CO2/N2 >500. The last value is much higher than the accepted value of ~ 100 for the upper mantle.

Environmental conditions affecting concentrations of He, CO2, O2 and N2 in soil gases

USGS Publications Warehouse

Hinkle, Margaret E.

1994-01-01

The measurement of concentrations of volatile species in soil gases has potential for use in geochemical exploration for concealed ore deposits and for monitoring of subsurface contaminants. However, the interpretation of anomalies in surficial gases can be difficult because soil-gas concentrations are dependent on both meteorological and environmental conditions.For this study, concentrations of He, CO2, O2 and N2 and meteorological conditions were monitored for 10–14 months at eight nonmineralized sites in both humid and dry environments. Gases were collected at 0.6–0.7-m depth at seven sites. At one site, gases were collected from 0.3-, 0.6-, 1.2-, and 2.0-m depths; diurnal monitoring studies were conducted at this site also. Rain and snowfall, soil and air temperatures, barometric pressure, and relative humidity were monitored at all the sites. The sand, silt and clay content, and the organic carbon content of surficial soil were measured at each site.Meteorological conditions generally affected He and CO2 concentrations in the same way at all the sites; however, these effects were modified by local environmental conditions. Both seasonal and diurnal concentration changes occurred. The most important seasonal concentration changes were related to rain and snowfall and soil and air temperatures. Seasonal changes tended to be larger then the diurnal changes, but both could be related to the same processes. Local conditions of soil type and organic content affected the amount of pore space and moisture present in the soil and therefore the soil-gas concentrations.

Thermally and chemically responsive nanoporous materials for efficient capture of fission product gases.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stroeve, Pieter; Faller, Roland

The objective of this project was to develop robust, high-efficiency materials for capture of fission product gases such as He, Xe and Kr in scenarios relevant for both reactor fuels and reprocessing operations. The relevant environments are extremely harsh, encompassing temperatures up to 1500 °C, high levels of radiation, as well as potential exposures to highly-reactive chemicals such as nitric acid and organic solvents such as kerosene. The requirement for nanostructured capture materials is driven in part by the very short (few micron) diffusion distances for product gases in nuclear fuel. We achieved synthesis, characterization and detailed modeling of themore » materials. Although not all materials reviewed in this report will be feasible for the ultimate goal of integration in nuclear fuel, nevertheless each material studied has particular properties which will enable an optimized material to be efficiently developed and characterized.« less

Study of performance characteristics of noble metal thermocouple materials to 2000 C

NASA Technical Reports Server (NTRS)

Freeze, P. D.; Thomas, D.; Edelman, S.; Stern, J.

1972-01-01

Three performance characteristics of noble metal thermocouples in various environments are discussed. Catalytic effects cause significant errors when noble metal thermocouple materials are exposed to air containing unburned gases in temperature ranges from 25 C to 1500 C. The thermoelectric stability of the iridium 40 rhodium to iridium thermocouple system at 2000 C in an oxidizing medium is described. The effects of large and small temperature gradients on the accuracy and stability of temperature measurements are analyzed.

Cosmogenic 3He in detrital gold

NASA Astrophysics Data System (ADS)

Stuart, Finlay; Yakubovich, Olga; Caracedo, Ana; Nesterenok, Alexander

2017-04-01

Since the measurement of cosmogenic He in an alluvial diamond by McConville and Reynolds (1996) the application of cosmogenic noble gases to individual detrital grains to quantify surface processes has not been vigorously pursued. The likely low rate of diffusion of cosmogenic He in native metals, and their resistance to weathering and disintegration during erosion and transport, makes them a potential record of long-term Earth surface processes. In an effort to assess the extent that detrital refractory metals record the exposure history during transport and storage we have undertaken a reconnaissance study of the He isotope composition in 18 grains (2-200 mg) of native gold, copper, silver, and PtPd, Pt3Fe and OsIr alloys from alluvial placer deposits from around the world. 4He is dominantly the result of U and Th decay within the grains, or decay of 190Pt in the Pt-rich alloys. 3He is measurable in 13 grains, concentrations range up to 2.7E+6 atoms/g. 3He/4He are always in excess of the crustal radiogenic ratio, up to 306 Ra. Although nucleogenic 3He produced by (n,α) reactions on 6Li, and 3He from trapped hydrothermal fluids, are present, the majority of the 3He is cosmogenic in origin. Using newly calculated cosmogenic 3He production rates in heavy metals, and a determination of the effect of implantation based on the stopping distances of spallogenic 3He and 3H, the grains have 3Hecos concentrations that are equivalent to 0.35 to 1.5 Ma exposure at Earth's surface. In a study of detrital gold grains from several sites in Scotland we have found that 10 % have 3He concentrations that are significantly in excess of that generated since the Last Glacial Maximum. These studies demonstrate that, with refinement, cosmogenic 3He in refractory detrital minerals can be used to quantify sediment transport and storage on the 1-10 Ma timescale. P. McConville & J.H. Reynolds (1989). Geochim. Cosmochim. Acta, 53, 2365-75.

He, U, and Th Depth Profiling of Apatite and Zircon Using Laser Ablation Noble Gas Mass Spectrometry and SIMS

NASA Astrophysics Data System (ADS)

Monteleone, B. D.; van Soest, M. C.; Hodges, K. V.; Hervig, R.; Boyce, J. W.

2008-12-01

Conventional (U-Th)/He thermochronology utilizes single or multiple grain analyses of U- and Th-bearing minerals such as apatite and zircon and does not allow for assessment of spatial variation in concentration of He, U, or Th within individual crystals. As such, age calculation and interpretation require assumptions regarding 4He loss through alpha ejection, diffusive redistribution of 4He, and U and Th distribution as an initial condition for these processes. Although models have been developed to predict 4He diffusion parameters, correct for the effect of alpha ejection on calculated cooling ages, and account for the effect of U and Th zonation within apatite and zircon, measurements of 4He, U, and Th distribution have not been combined within a single crystal. We apply ArF excimer laser ablation, combined with noble gas mass spectrometry, to obtain depth profiles within apatite and zircon crystals in order to assess variations in 4He concentration with depth. Our initial results from pre-cut, pre-heated slabs of Durango apatite, each subjected to different T-t schedules, suggest a general agreement of 4He profiles with those predicted by theoretical diffusion models (Farley, 2000). Depth profiles through unpolished grains give reproducible alpha ejection profiles in Durango apatite that deviate from alpha ejection profiles predicted for ideal, homogenous crystals. SIMS depth profiling utilizes an O2 primary beam capable of sputtering tens of microns and measuring sub-micron resolution variation in [U], [Th], and [Sm]. Preliminary results suggest that sufficient [U] and [Th] zonation is present in Durango apatite to influence the form of the 4He alpha ejection profile. Future work will assess the influence of measured [U] and [Th] zonation on previously measured 4He depth profiles. Farley, K.A., 2000. Helium diffusion from apatite; general behavior as illustrated by Durango fluorapatite. J. Geophys. Res., B Solid Earth Planets 105 (2), 2903-2914.

Coexistence and interfacial properties of a triangle-well mimicking the Lennard-Jones fluid and a comparison with noble gases.

PubMed

Bárcenas, M; Reyes, Y; Romero-Martínez, A; Odriozola, G; Orea, P

2015-02-21

Coexistence and interfacial properties of a triangle-well (TW) fluid are obtained with the aim of mimicking the Lennard-Jones (LJ) potential and approach the properties of noble gases. For this purpose, the scope of the TW is varied to match vapor-liquid densities and surface tension. Surface tension and coexistence curves of TW systems with different ranges were calculated with replica exchange Monte Carlo and compared to those data previously reported in the literature for truncated and shifted (STS), truncated (ST), and full Lennard-Jones (full-LJ) potentials. We observed that the scope of the TW potential must be increased to approach the STS, ST, and full-LJ properties. In spite of the simplicity of TW expression, a remarkable agreement is found. Furthermore, the variable scope of the TW allows for a good match of the experimental data of argon and xenon.

Observation of the Kaiser Effect Using Noble Gas Release Signals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bauer, Stephen J.

The Kaiser effect was defined in the early 1950s (Kaiser 1953) and was extensively reviewed and evaluated by Lavrov (2002) with a view toward understanding stress estimations. The Kaiser effect is a stress memory phenomenon which has most often been demonstrated in rock using acoustic emissions. During cyclic loading–unloading–reloading, the acoustic emissions are near zero until the load exceeds the level of the previous load cycle. Here, we sought to explore the Kaiser effect in rock using real-time noble gas release. Laboratory studies using real-time mass spectrometry measurements during deformation have quantified, to a degree, the types of gases releasedmore » (Bauer et al. 2016a, b), their release rates and amounts during deformation, estimates of permeability created from pore structure modifications during deformation (Gardner et al. 2017) and the impact of mineral plasticity upon gas release. We found that noble gases contained in brittle crystalline rock are readily released during deformation.« less

Observation of the Kaiser Effect Using Noble Gas Release Signals

DOE PAGES

Bauer, Stephen J.

2017-10-24

The Kaiser effect was defined in the early 1950s (Kaiser 1953) and was extensively reviewed and evaluated by Lavrov (2002) with a view toward understanding stress estimations. The Kaiser effect is a stress memory phenomenon which has most often been demonstrated in rock using acoustic emissions. During cyclic loading–unloading–reloading, the acoustic emissions are near zero until the load exceeds the level of the previous load cycle. Here, we sought to explore the Kaiser effect in rock using real-time noble gas release. Laboratory studies using real-time mass spectrometry measurements during deformation have quantified, to a degree, the types of gases releasedmore » (Bauer et al. 2016a, b), their release rates and amounts during deformation, estimates of permeability created from pore structure modifications during deformation (Gardner et al. 2017) and the impact of mineral plasticity upon gas release. We found that noble gases contained in brittle crystalline rock are readily released during deformation.« less

Method for introduction of gases into microspheres

DOEpatents

Hendricks, Charles D.; Koo, Jackson C.; Rosencwaig, Allan

1981-01-01

A method for producing small hollow glass spheres filled with a gas by introduction of the gas during formation of the hollow glass spheres. Hollow glass microspheres having a diameter up to about 500.mu. with both thin walls (0.5 to 4.mu.) and thick walls (5 to 20.mu.) that contain various fill gases, such as Ar, Kr, Xe, Br, DT, H.sub.2, D.sub.2, He, N.sub.2, Ne, CO.sub.2, etc. in the interior thereof, can be produced by the diffusion of the fill gas or gases into the microsphere during the formation thereof from a liquid droplet of glass-forming solution. This is accomplished by filling at least a portion of the multiple-zone drop-furnace used in producing hollow microspheres with the gas or gases of interest, and then taking advantage of the high rate of gaseous diffusion of the fill gas through the wall of the gel membrane before it transforms into a glass microsphere as it is processed in the multiple-zone furnace. Almost any gas can be introduced into the inner cavity of a glass microsphere by this method during the formation of the microsphere provided that the gas is diffused into the gel membrane or microsphere prior to its transformation into glass. The process of this invention provides a significant savings of time and related expense of filling glass microspheres with various gases. For example, the time for filling a glass microballoon with 1 atmosphere of DT is reduced from about two hours to a few seconds.

Microscopic search for the carrier phase Q of the trapped planetary noble gases in Allende, Leoville, and Vigarano

NASA Astrophysics Data System (ADS)

Vis, R. D.; Mrowiec, A.; Kooyman, P. J.; Matsubara, K.; Heymann, D.

2002-10-01

High-resolution transmission electron microscopy micrographs of acid-resistant residues of the Allende, Leoville, and Vigarano meteorites show a great variety of carbon structures: curved and frequently twisted and intertwined graphene sheets, abundant carbon black-like particles, and hollow "sacs". It is suggested that perhaps all of these are carriers for the planetary Q-noble gases in these meteorites. Most of these materials are pyrocarbons that probably formed by the pyrolysis of hydrocarbons either in a gas phase, or on hot surfaces of minerals. An attempt was made to analyze for argon with particle-induced x-ray emission in 143 spots of grains of floating and suspended matter from freeze-dry cycles of an Allende bulk sample in water, and floating "black balls" from sonication in water of samples from the Allende meteorite. The chemical compositions of these particles were obtained, but x-ray signals at the wavelength of argon were obtained on only a few spots.

Static electric polarizabilities and first hyperpolarizabilities of molecular ions RgH + (Rg = He, Ne, Ar, Kr, Xe): ab initio study

NASA Astrophysics Data System (ADS)

Cukras, Janusz; Antušek, Andrej; Holka, Filip; Sadlej, Joanna

2009-06-01

Extensive ab initio calculations of static electric properties of molecular ions of general formula RgH + (Rg = He, Ne, Ar, Kr, Xe) involving the finite field method and coupled cluster CCSD(T) approach have been done. The relativistic effects were taken into account by Douglas-Kroll-Hess approximation. The numerical stability and reliability of calculated values have been tested using the systematic sequence of Dunning's cc-pVXZ-DK and ANO-RCC-VQZP basis sets. The influence of ZPE and pure vibrational contribution has been discussed. The component αzz has increasing trend in RgH + while the relativistic effect on αzz leads to a small increase of this molecular parameter.

Cryogenic method for measuring nuclides and fission gases

DOEpatents

Perdue, P.T.; Haywood, F.F.

1980-05-02

A cryogenic method is provided for determining airborne gases and particulates from which gamma rays are emitted. A special dewar counting vessel is filled with the contents of the sampling flask which is immersed in liquid nitrogen. A vertically placed sodium-iodide or germanium-lithium gamma-ray detector is used. The device and method are of particular use in measuring and identifying the radioactive noble gases including emissions from coal-fired power plants, as well as fission gases released or escaping from nuclear power plants.

Noble gas isotopes in mineral springs within the Cascadia Forearc, Wasihington and Oregon

USGS Publications Warehouse

McCrory, Patricia A.; Constantz, James E.; Hunt, Andrew G.

2014-01-01

This U.S. Geological Survey report presents laboratory analyses along with field notes for a pilot study to document the relative abundance of noble gases in mineral springs within the Cascadia forearc of Washington and Oregon. Estimates of the depth to the underlying Juan de Fuca oceanic plate beneath the sample sites are derived from the McCrory and others (2012) slab model. Some of these springs have been previously sampled for chemical analyses (Mariner and others, 2006), but none currently have publicly available noble gas data. Helium isotope values as well as the noble gas values and ratios presented below will be used to determine the sources and mixing history of these mineral waters.

Diffusion of Helium in the mantle: an explanation for MORB-OIB patterns of 3He/4He ratios

NASA Astrophysics Data System (ADS)

Morgan, W. J.; Morgan, J. P.

2011-12-01

barren matrix to contribute its 3He and 4He to the MORB melt which results in an excess of helium relative to neon and argon. This extraction of helium from the longtime-diffused-into barren matrix also can explain the uniformity of the 3/4 ratio in MORB as opposed to the variability of 3/4 in OIB where the individual lumps each contribute their own variable contents. What is lacking in this explanation are data on diffusion rates of the noble gases under deep mantle conditions. What experimental data exists suggest helium diffuses sufficiently fast, but published data only go up to ≈1300 °C, and at only uppermost mantle pressures. Can experiments in diamond anvils or calculations that include 'helium atoms' in molecular dynamics models give diffusion constants to test this hypothesis?

The Saturn Probe Interior and aTmosphere Explorer (SPRITE) Mission

NASA Astrophysics Data System (ADS)

Simon, Amy; Banfield, Donald; Atkinson, David; SPRITE Science Team

2018-01-01

A key question in planetary science is how the planets formed in our Solar System, and, by extension, in exoplanet systems. The abundances of the noble gases (He, Ne, Ar, Kr, Xe), heavy elements (C, N, O, S), and their isotopes provide important forensic clues as to location and time of formation in the early Solar System. Jupiter and Saturn contain most of the planetary mass in our solar system, and their chemical fingerprints will distinguish between competing models of the formation of all the planets. After the end of the Cassini mission, some of these elements have only ambiguous values above the cloud tops, while others (particularly the noble gases) have not been measured at all. Resolving this requires direct in situ measurements. The proposed NASA New Frontiers Saturn PRobe Interior and aTmosphere Explorer (SPRITE) mission delivers an instrumented entry probe from a carrier relay spacecraft that also provides context imaging. The powerful probe instrument suite is comprised of a Quadrupole Mass Spectrometer, a Tunable Laser Spectrometer, and an Atmospheric Structure Instrument including a Doppler Wind Experiment and a simple backscatter nephelometer. These instruments measure the elemental and isotopic abundances of helium, the heavier noble gases, and the major elements, as well as constraining cloud properties, 3-D atmospheric dynamics, and disequilibrium chemistry to at least 10 bars in Saturn's troposphere. In situ measurements of Saturn's atmosphere by SPRITE will provide a significantly improved context for interpreting the results from the Galileo probe, Juno, and Cassini missions. SPRITE will revolutionize our understanding of the formation and evolution of the gas giant planets, and ultimately the present-day structure of the Solar System.

Radiogenic 3He/4He Estimates and Their Effect on Calculating Plio-Pleistocene Cosmogenic 3He Ages of Alluvial-Fan Terraces in the Lower Colorado River Basin, USA

NASA Astrophysics Data System (ADS)

Fenton, C.; Pelletier, J.

2005-12-01

helium in Black Mountain basalt samples is 0.011. Other noble gas studies have shown that radiogenic 3He/4He is independent of the U content, nearly independent of the Th content, and strongly influenced by the Li content of a rock; we find the same results. It is assumed that mantle gases are released when the sample is crushed into a fine powder before melting in a furnace under vacuum. To correct for the possible presence of mantle gases in our age-calculations, we crushed two samples under vacuum to measure the R/Ra value (7.9 and 16.03) of mantle helium trapped in fluid inclusions in olivines and pyroxenes. Based on our 3He corrections and calculations, boulders on these alluvial fans range in age from 10 ka to 2.7 Ma.

Colloidally separated samples from Allende residues - Noble gases, carbon and an ESCA-study

NASA Technical Reports Server (NTRS)

Ott, U.; Kronenbitter, J.; Flores, J.; Chang, S.

1984-01-01

Results are presented which strengthen the hypothesis of heterogeneity among the carbon- and nitrogen-bearing phases of the Allende meteorite. These data also highlight the possibility of performing physical separations yielding samples in which some of the noble gas- and carbon-bearing phases are extraordinarily predominant over others. The conclusion, based on mass and isotope balance arguments, that a significant portion of the carbonaceous matter in Allende is likely to be gas-poor or gas-free need not weaken the case for carbonaceous carriers for the major noble gas components. The concept that acid-soluble carbonaceous phases contain a multiplicity of components, each of which may have formed under a multiplicity of different physical-chemical conditions, is reemphasized by the results of the present study.

Optimizing Noble Gas-Water Interactions via Monte Carlo Simulations.

PubMed

Warr, Oliver; Ballentine, Chris J; Mu, Junju; Masters, Andrew

2015-11-12

In this work we present optimized noble gas-water Lennard-Jones 6-12 pair potentials for each noble gas. Given the significantly different atomic nature of water and the noble gases, the standard Lorentz-Berthelot mixing rules produce inaccurate unlike molecular interactions between these two species. Consequently, we find simulated Henry's coefficients deviate significantly from their experimental counterparts for the investigated thermodynamic range (293-353 K at 1 and 10 atm), due to a poor unlike potential well term (εij). Where εij is too high or low, so too is the strength of the resultant noble gas-water interaction. This observed inadequacy in using the Lorentz-Berthelot mixing rules is countered in this work by scaling εij for helium, neon, argon, and krypton by factors of 0.91, 0.8, 1.1, and 1.05, respectively, to reach a much improved agreement with experimental Henry's coefficients. Due to the highly sensitive nature of the xenon εij term, coupled with the reasonable agreement of the initial values, no scaling factor is applied for this noble gas. These resulting optimized pair potentials also accurately predict partitioning within a CO2-H2O binary phase system as well as diffusion coefficients in ambient water. This further supports the quality of these interaction potentials. Consequently, they can now form a well-grounded basis for the future molecular modeling of multiphase geological systems.

Two- and three-photon ionization in the noble gases

DOE Office of Scientific and Technical Information (OSTI.GOV)

McGuire, E.J.

1981-08-01

By using a characteristic Green's function for an exactly solvable Schroedinger equation with an approximation to the central potential of Hermann and Skillman, the cross section for nonresonant two- and three-photon ionization of Ne, Ar, Kr, and Xe were calculated in jl coupling. Expressions for cross sections in jl coupling are given. Comparison with the Ar two-photon cross section of Pindzola and Kelly, calculated using the many-body theory, the dipole-length approximation, and LS coupling shows a disagreement of as much as a factor of 2. The disagreement appears to arise from distortion introduced by shifting the Green's-function resonances to experimentalmore » values.« less

Efficient 3He/4He separation in a nanoporous graphenylene membrane.

PubMed

Qu, Yuanyuan; Li, Feng; Zhao, Mingwen

2017-08-16

Helium-3 is a precious noble gas, which is essential in many advanced technologies such as cryogenics, isotope labeling and nuclear weapons. The current imbalance of 3 He demand and supply shortage leads to the search for an efficient membrane with high performance for 3 He separation. In this study, based on first-principles calculations, we demonstrated that highly efficient 3 He harvesting can be achieved in a nanoporous graphenylene membrane with industrially-acceptable selectivity and permeance. The quantum tunneling effect leads to 3 He harvesting with high efficiency via kinetic sieving. Both the quantum tunneling effect and zero-point energy (ZPE) determine the 3 He/ 4 He separation via thermally-driven equilibrium sieving, where the ZPE effect dominates efficient 3 He/ 4 He separation between two reservoirs. The quantum effects revealed in this work suggest that the nanoporous graphenylene membrane is promising for efficient 3 He harvesting that can be exploited for industrial applications.

Investigation of the Discharge Characteristics of the T6 Hollow Cathode Operating on Several Inert Gases and a Kr/Xe Mixture

NASA Astrophysics Data System (ADS)

Ahmed Rudwan, M.; Gabriel, S. B.

2002-01-01

Investigation of the discharge characteristics of the T6 hollow cathode operating on several inert Xenon is currently the propellant of choice for gridded ion thrusters. But in order to make deep space missions feasible, an increase in the Specific Impulse (SI) that these thrusters can achieve is necessary. One method of achieving this is to use a propellant with a lower atomic mass (e.g. argon), as the propellant exhaust velocity is inversely proportional to the square root of the propellant mass. However, the feasibility of operating the hollow cathode using these alternative propellants has to be demonstrated. Moreover, interest in decreasing the propellant cost in missions and ground testing (especially life tests) have led to the comprehensive discharge characterisation of several gases that will be presented in this paper. A Kr/Xe mixture in the naturally occurring ratio, for example, could offer a 15 times cost saving when compared to pure xenon and 2-3 times cost saving when compared to pure krypton. The T6 hollow cathode discharge behaviour as well as its initiation characteristics have been studied. The tests were carried out in diode configuration using a T6 hollow cathode with an enclosed keeper design employing xenon, krypton, argon and a Kr/Xe mix. The discharge initiation tests were undertaken with a view to investigate some of the factors thought to influence the starting potential such as mass flow rate and tip temperature. It was found that, for mass flow rates ranging from 0.2-1.1 mg/s and cathode tip temperatures ranging from 900-1300oC, the breakdown potential was less than 50V for argon, less than 25V for krypton, less than 21V for xenon and less than 35V for the Kr/Xe mix. The discharge initiation results were then compared to those obtained by Fearn et al. with a T5 cathode operating on mercury and with a T6 cathode utilising an open keeper design using xenon propellant. The xenon breakdown potentials were found to be lower than those

Origins of geothermal gases at Yellowstone

USGS Publications Warehouse

Lowenstern, Jacob B.; Bergfeld, Deborah; Evans, William C.; Hunt, Andrew G.

2015-01-01

Gas emissions at the Yellowstone Plateau Volcanic Field (YPVF) reflect open-system mixing of gas species originating from diverse rock types, magmas, and crustal fluids, all combined in varying proportions at different thermal areas. Gases are not necessarily in chemical equilibrium with the waters through which they vent, especially in acid sulfate terrain where bubbles stream through stagnant acid water. Gases in adjacent thermal areas often can be differentiated by isotopic and gas ratios, and cannot be tied to one another solely by shallow processes such as boiling-induced fractionation of a parent liquid. Instead, they inherit unique gas ratios (e.g., CH4/He) from the dominant rock reservoirs where they originate, some of which underlie the Quaternary volcanic rocks. Steam/gas ratios (essentially H2O/CO2) of Yellowstone fumaroles correlate with Ar/He and N2/CO2, strongly suggesting that H2O/CO2 is controlled by addition of steam boiled from water rich in atmospheric gases. Moreover, H2O/CO2 varies systematically with geographic location, such that boiling is more enhanced in some areas than others. The δ13C and 3He/CO2 of gases reflect a dominant mantle origin for CO2 in Yellowstone gas. The mantle signature is most evident at Mud Volcano, which hosts gases with the lowest H2O/CO2, lowest CH4 concentrations and highest He isotope ratios (~16Ra), consistent with either a young subsurface intrusion or less input of crustal and meteoric gas than any other location at Yellowstone. Across the YPVF, He isotope ratios (3He/4He) inversely vary with He concentrations, and reflect varied amounts of long- stored, radiogenic He added to the magmatic endmember within the crust. Similarly, addition of CH4 from organic-rich sediments is common in the eastern thermal areas at Yellowstone. Overall, Yellowstone gases reflect addition of deep, high-temperature magmatic gas (CO2-rich), lower-temperatures crustal gases (4He- and CH4-bearing), and those gases (N2, Ne, Ar) added

Platinum-coated non-noble metal-noble metal core-shell electrocatalysts

DOEpatents

Adzic, Radoslav; Zhang, Junliang; Mo, Yibo; Vukmirovic, Miomir

2015-04-14

Core-shell particles encapsulated by a thin film of a catalytically active metal are described. The particles are preferably nanoparticles comprising a non-noble core with a noble metal shell which preferably do not include Pt. The non-noble metal-noble metal core-shell nanoparticles are encapsulated by a catalytically active metal which is preferably Pt. The core-shell nanoparticles are preferably formed by prolonged elevated-temperature annealing of nanoparticle alloys in an inert environment. This causes the noble metal component to surface segregate and form an atomically thin shell. The Pt overlayer is formed by a process involving the underpotential deposition of a monolayer of a non-noble metal followed by immersion in a solution comprising a Pt salt. A thin Pt layer forms via the galvanic displacement of non-noble surface atoms by more noble Pt atoms in the salt. The overall process is a robust and cost-efficient method for forming Pt-coated non-noble metal-noble metal core-shell nanoparticles.

The interstellar formation and spectra of the noble gas, proton-bound HeHHe+, HeHNe+ and HeHAr+ complexes

NASA Astrophysics Data System (ADS)

Stephan, Cody J.; Fortenberry, Ryan C.

2017-07-01

The sheer interstellar abundance of helium makes any bound molecules or complexes containing it of potential interest for astrophysical observation. This work utilizes high-level and trusted quantum chemical techniques to predict the rotational, vibrational and rovibrational traits of HeHHe+, HeHNe+ and HeHAr+. The first two are shown to be strongly bound, while HeHAr+ is shown to be more of a van der Waals complex of argonium with a helium atom. In any case, the formation of HeHHe+ through reactions of HeH+ with HeH3+ is exothermic. HeHHe+ exhibits the quintessentially bright proton-shuttle motion present in all proton-bound complexes in the 7.4 micron range making it a possible target for telescopic observation at the mid-/far-Infrared crossover point and a possible tracer for the as-of-yet unobserved helium hydride cation. Furthermore, a similar mode in HeHNe+ can be observed to the blue of this close to 6.9 microns. The brightest mode of HeHAr+ is dimmed due the reduced interaction of the helium atom with the central proton, but this fundamental frequency can be found slightly to the red of the Ar-H stretch in the astrophysically detected argonium cation.

Investigation of the noble gas solubility in H 2O-CO 2 bearing silicate liquids at moderate pressure II: the extended ionic porosity (EIP) model

NASA Astrophysics Data System (ADS)

Nuccio, P. M.; Paonita, A.

2000-12-01

A semi-theoretical model is proposed to predict partitioning of noble gases between any silicate liquid and a H 2O-CO 2 gas phase with noble gas as a minor component, in a large range of pressures (at least up to 300 MPa). The model is based on the relationship between the concentration of dissolved noble gas and ionic porosity of the melt, found by Carroll and Stolper [Geochim. Cosmochim. Acta 57 (1993) 5039-5051] for H 2O-CO 2 free melts. It evaluates the effect of dissolved H 2O and CO 2 on the melt ionic porosity and, consequently on Henry's constants of noble gases. The fugacities of the noble gases in the H 2O-CO 2-noble gas mixtures are also considered in our equilibrium calculations of dissolved gas by using a modified Redlich-Kwong equation of state for the H 2O-CO 2-noble gas system. The formulated model (referred to as the extended ionic porosity model) clearly predicts a positive dependence of noble gas solubility on dissolved H 2O in melt, which becomes negligible when water concentration is higher than 3 wt%. Oppositely, noble gas solubility decreases as a consequence of increasing CO 2 in both basaltic and rhyolitic melts. The increase of noble gas solubility as a consequence of H 2O addition to the melt grows exponentially with the increase of the noble gas atomic size. As a result, although xenon solubility is much lower than the helium solubility in anhydrous melts, they become almost comparable at several percent of dissolved H 2O in the melt. On this basis, an exponential augmentation of the number of large free spaces in silicate liquid can be inferred in relation to increasing dissolved H 2O. Comparison between our predicted values and available experimental data [A. Paonita et al., Earth Planet. Sci. Lett. 181 (2000) 595-604] shows good agreement. At present, the EIP model is the unique tool which predicts how the main volatiles in magmatic systems affect the noble gas solubility in silicate melts, therefore it should be taken into account

Dipole, quadrupole, and octupole terms in the long-range hyperfine frequency shift for hydrogen in the presence of inert gases

NASA Astrophysics Data System (ADS)

Greenwood, W. G.; Tang, K. T.

1987-03-01

The R-6, R-8, and R-10 terms in the long-range expansion for the hyperfine frequency shift are calculated for hydrogen in the presence of He, Ne, Ar, Kr, and Xe. The R-6 terms are based on the dipole oscillator strength sums. For helium, the R-8 and R-10 terms are based on quadrupole and octupole oscillator strength sums. For the heavier inert gases, the results for the R-8 and R-10 terms are obtained from the sum rules and the static polarizabilities. Upper bounds are also determined for the R-8 and R-10 terms.

Application unit for the administration of contrast gases for pulmonary magnetic resonance imaging: optimization of ventilation distribution for (3) He-MRI.

PubMed

Güldner, M; Becker, St; Wolf, U; Düber, C; Friesenecker, A; Gast, K K; Heil, W; Hoffmann, C; Karpuk, S; Otten, E W; Rivoire, J; Salhi, Z; Scholz, A; Schreiber, L M; Terekhov, M

2015-09-01

MRI of lung airspaces using gases with MR-active nuclei ((3) He, (129) Xe, and (19) F) is an important area of research in pulmonary imaging. The volume-controlled administration of gas mixtures is important for obtaining quantitative information from MR images. State-of-the-art gas administration using plastic bags (PBs) does not allow for a precise determination of both the volume and timing of a (3) He bolus. A novel application unit (AU) was built according to the requirements of the German medical devices law. Integrated spirometers enable the monitoring of the inhaled gas flow. The device is particularly suited for hyperpolarized (HP) gases (e.g., storage and administration with minimal HP losses). The setup was tested in a clinical trial (n = 10 healthy volunteers) according to the German medicinal products law using static and dynamic ventilation HP-(3) He MRI. The required specifications for the AU were successfully realized. Compared to PB-administration, better reproducibility of gas intrapulmonary distribution was observed when using the AU for both static and dynamic ventilation imaging. The new AU meets the special requirements for HP gases, which are storage and administration with minimal losses. Our data suggest that gas AU-administration is superior to manual modes for determining the key parameters of dynamic ventilation measurements. © 2014 Wiley Periodicals, Inc.

High-order nonlinear susceptibilities of He

NASA Astrophysics Data System (ADS)

Liu, W.-C.; Clark, Charles W.

1996-05-01

High-order nonlinear optical response of noble gases to intense laser radiation is of considerable experimental interest, but is difficult to measure or calculate accurately. We have begun a set of calculations of frequency-dependent nonlinear susceptibilities of He 1s^2, within the framework of Rayleigh-Schrödinger perturbation theory at lowest applicable order, with the goal of providing critically evaluated atomic data for modelling high harmonic generation processes. The atomic Hamiltonian is decomposed in term of Hylleraas coordinates and spherical harmonics using the formalism of Pont and Shakeshaft (M. Pont and R. Shakeshaft, Phy. Rev. A 51), 257 (1995), and the hierarchy of inhomogeneous equations of perturbation theory is solved iteratively. A combination of Hylleraas and Frankowski basis functions is used(J. D. Baker, Master thesis, U. Delaware (1988); J. D. Baker, R. N. Hill, and J. D. Morgan, AIP Conference Proceedings 189) 123(1989); the compact Hylleraas basis provides a highly accurate representation of the ground state wavefunction, whereas the diffuse Frankowski basis functions efficiently reproduce the correct asymptotic structure of the perturbed orbitals.

The production rate of cosmogenic 21-Ne in chondrites deduced from 81-Kr measurements

NASA Technical Reports Server (NTRS)

Schultz, L.; Freundel, M.

1986-01-01

Cosmogenic Ne-21 is used widely to calculate exposure ages of stone meteorites. In order to do so, the production rate P(21) must be known. This rate, however, is dependent on the chemical composition of the meteorite as well as the mass of, and position within, the meteoroid during its exposure to the cosmic radiation. Even for a mean shielding the production rates determined from measurments of different radionuclides vary by a factor of two. A method that can be used to determine exposure ages of meteorites that avoids shielding and chemical composition corrections is the -81-Kr-Kr-method. However, for chondrites, in many cases, the direct determination of production rates for the Kr isotopes is prevented by the trapped gases and the neutron effects on bromine. Therefore, this method was applied to four eucrite falls and then their 81-Kr-83-Kr-ages were compared to their cosmogenic Ne-21 and Ar-38 concentrations. The eucrites Bouvante-le-Haut, Juvinas, Sioux County, and Stannern were chosen for these measurements because of their similar chemical composition regarding the major elements.

Polymeric membrane materials: new aspects of empirical approaches to prediction of gas permeability parameters in relation to permanent gases, linear lower hydrocarbons and some toxic gases.

PubMed

Malykh, O V; Golub, A Yu; Teplyakov, V V

2011-05-11

Membrane gas separation technologies (air separation, hydrogen recovery from dehydrogenation processes, etc.) use traditionally the glassy polymer membranes with dominating permeability of "small" gas molecules. For this purposes the membranes based on the low free volume glassy polymers (e.g., polysulfone, tetrabromopolycarbonate and polyimides) are used. On the other hand, an application of membrane methods for VOCs and some toxic gas recovery from air, separation of the lower hydrocarbons containing mixtures (in petrochemistry and oil refining) needs the membranes with preferable penetration of components with relatively larger molecular sizes. In general, this kind of permeability is characterized for rubbers and for the high free volume glassy polymers. Data files accumulated (more than 1500 polymeric materials) represent the region of parameters "inside" of these "boundaries." Two main approaches to the prediction of gas permeability of polymers are considered in this paper: (1) the statistical treatment of published transport parameters of polymers and (2) the prediction using model of ≪diffusion jump≫ with consideration of the key properties of the diffusing molecule and polymeric matrix. In the frames of (1) the paper presents N-dimensional methods of the gas permeability estimation of polymers using the correlations "selectivity/permeability." It is found that the optimal accuracy of prediction is provided at n=4. In the frames of the solution-diffusion mechanism (2) the key properties include the effective molecular cross-section of penetrating species to be responsible for molecular transportation in polymeric matrix and the well known force constant (ε/k)(eff i) of {6-12} potential for gas-gas interaction. Set of corrected effective molecular cross-section of penetrant including noble gases (He, Ne, Ar, Kr, Xe), permanent gases (H(2), O(2), N(2), CO), ballast and toxic gases (CO(2), NO(,) NO(2), SO(2), H(2)S) and linear lower hydrocarbons (CH(4

Using noble gas ratios to determine the origin of ground ice

NASA Astrophysics Data System (ADS)

Utting, Nicholas; Lauriol, Bernard; Lacelle, Denis; Clark, Ian

2016-01-01

Argon, krypton and xenon have different solubilities in water, meaning their ratios in water are different from those in atmospheric air. This characteristic is used in a novel method to distinguish between ice bodies which originate from the compaction of snow (i.e. buried snow banks, glacial ice) vs. ice which forms from the freezing of groundwater (i.e. pingo ice). Ice which forms from the compaction of snow has gas ratios similar to atmospheric air, while ice which forms from the freezing of liquid water is expected to have gas ratios similar to air-equilibrated water. This analysis has been conducted using a spike dilution noble gas line with gas extraction conducted on-line. Samples were mixed with an aliquot of rare noble gases while being melted, then extracted gases are purified and cryogenically separated. Samples have been analysed from glacial ice, buried snow bank ice, intrusive ice, wedge ice, cave ice and two unknown ice bodies. Ice bodies which have formed from different processes have different gas ratios relative to their formation processes.

Use of IMS data and its potential for research through global noble gases concentration maps

NASA Astrophysics Data System (ADS)

Terzi, Lucrezia; Kalinowski, Martin; Gueibe, Christophe; Camps, Johan; Gheddou, Abdelhakim; Kusmierczyk-Michulec, Jolanta; Schoeppner, Michael

2017-04-01

The Comprehensive Nuclear-Test-Ban Treaty (CTBT) established for verification purposes a global monitoring system for atmospheric radioisotopes and noble gas radioactivity. Daily activity concentrations have been collected worldwide for over 15 years providing unique data sets with long term time series that can be used for atmospheric circulation dynamics analysis. In this study, we want to emphasize the value of worldwide noble gas data by reconstructing global xenon concentration maps and comparing these observations with ATM simulations. By creating a residual plot, we can improve our understanding of our source estimation level for each region.

Fullerenes and interplanetary dust at the Permian-Triassic boundary.

PubMed

Poreda, Robert J; Becker, Luann

2003-01-01

We recently presented new evidence that an impact occurred approximately 250 million years ago at the Permian-Triassic boundary (PTB), triggering the most severe mass extinction in the history of life on Earth. We used a new extraterrestrial tracer, fullerene, a third carbon carrier of noble gases besides diamond and graphite. By exploiting the unique properties of this molecule to trap noble gases inside of its caged structure (helium, neon, argon), the origin of the fullerenes can be determined. Here, we present new evidence for fullerenes with extraterrestrial noble gases in the PTB at Graphite Peak, Antarctica, similar to PTB fullerenes from Meishan, China and Sasayama, Japan. In addition, we isolated a (3)He-rich magnetic carrier phase in three fractions from the Graphite Peak section. The noble gases in this magnetic fraction were similar to zero-age deep-sea interplanetary dust particles (IDPs) and some magnetic grains isolated from the Cretaceous-Tertiary boundary. The helium and neon isotopic compositions for both the bulk Graphite Peak sediments and an isolated magnetic fraction from the bulk material are consistent with solar-type gases measured in zero-age deep-sea sediments and point to a common source, namely, the flux of IDPs to the Earth's surface. In this instance, the IDP noble gas signature for the bulk sediment can be uniquely decoupled from fullerene, demonstrating that two separate tracers are present (direct flux of IDPs for (3)He vs. giant impact for fullerene).

Escape and fractionation of volatiles and noble gases from Mars-sized planetary embryos and growing protoplanets

NASA Astrophysics Data System (ADS)

Odert, P.; Lammer, H.; Erkaev, N. V.; Nikolaou, A.; Lichtenegger, H. I. M.; Johnstone, C. P.; Kislyakova, K. G.; Leitzinger, M.; Tosi, N.

2018-06-01

Planetary embryos form protoplanets via mutual collisions, which can lead to the development of magma oceans. During their solidification, significant amounts of the mantles' volatile contents may be outgassed. The resulting H2O/CO2 dominated steam atmospheres may be lost efficiently via hydrodynamic escape due to the low gravity of these Moon- to Mars-sized objects and the high stellar EUV luminosities of the young host stars. Protoplanets forming from such degassed building blocks after nebula dissipation could therefore be drier than previously expected. We model the outgassing and subsequent hydrodynamic escape of steam atmospheres from such embryos. The efficient outflow of H drags along heavier species like O, CO2, and noble gases. The full range of possible EUV evolution tracks of a young solar-mass star is taken into account to investigate the atmospheric escape from Mars-sized planetary embryos at different orbital distances. The estimated envelopes are typically lost within a few to a few tens of Myr. Furthermore, we study the influence on protoplanetary evolution, exemplified by Venus. In particular, we investigate different early evolution scenarios and constrain realistic cases by comparing modeled noble gas isotope ratios with present observations. Isotope ratios of Ne and Ar can be reproduced, starting from solar values, under hydrodynamic escape conditions. Solutions can be found for different solar EUV histories, as well as assumptions about the initial atmosphere, assuming either a pure steam atmosphere or a mixture with accreted hydrogen from the protoplanetary nebula. Our results generally favor an early accretion scenario with a small amount of residual hydrogen from the protoplanetary nebula and a low-activity Sun, because in other cases too much CO2 is lost during evolution, which is inconsistent with Venus' present atmosphere. Important issues are likely the time at which the initial steam atmosphere is outgassed and/or the amount of CO2

Research of medical gases in Poland

PubMed Central

2013-01-01

Research of medical gases is well established in Poland and has been marked with the foundation of several professional societies. Numerous academic centers including those dealing with hyperbaric and diving medicine conduct studies of medical gases, in vast majority supported with intramural funds. In general, Polish research of medical gases is very much clinical in nature, covering new applications and safety of medical gases in medicine; on the other hand there are several academic centers pursuing preclinical studies, and elaborating basic theories of gas physiology and mathematical modeling of gas exchange. What dominates is research dealing with oxygen and ozone as well as studies of anesthetic gases and their applications. Finally, several research directions involving noble gas, hydrogen and hydrogen sulfide for cell protection, only begin to gain recognition of basic scientists and clinicians. However, further developments require more monetary spending on research and clinical testing as well as formation of new collective bodies for coordinating efforts in this matter. PMID:23916016

Proton affinities of maingroup-element hydrides and noble gases: trends across the periodic table, structural effects, and DFT validation.

PubMed

Swart, Marcel; Rösler, Ernst; Bickelhaupt, F Matthias

2006-10-01

We have carried out an extensive exploration of the gas-phase basicity of archetypal neutral bases across the periodic system using the generalized gradient approximation (GGA) of the density functional theory (DFT) at BP86/QZ4P//BP86/TZ2P. First, we validate DFT as a reliable tool for computing proton affinities and related thermochemical quantities: BP86/QZ4P//BP86/TZ2P is shown to yield a mean absolute deviation of 2.0 kcal/mol for the proton affinity at 298 K with respect to experiment, and 1.2 kcal/mol with high-level ab initio benchmark data. The main purpose of this work is to provide the proton affinities (and corresponding entropies) at 298 K of the neutral bases constituted by all maingroup-element hydrides of groups 15-17 and the noble gases, that is, group 18, and periods 1-6. We have also studied the effect of step-wise methylation of the protophilic center of the second- and third-period bases. Copyright 2006 Wiley Periodicals, Inc.

Noble Gas Proxy Evidence Of Holocene Climate Fluctuations In The Elwha Watershed, Olympic Mountains, Washington

EPA Science Inventory

Paleotempertures retrieved from the groundwater archives in the largest watershed (≈800 km2) in the Olympic Mountains suggest asynchronous Olympic Peninsula climate responses during the Everson interstade period after the last continental glacial maximum. Dissolved noble gases fr...

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kim, W.; Korea Basic Science Institute; Stepanyan, S. S.

We present a device for spin-exchange optical pumping system to produce large quantities of polarized noble gases for Magnetic Resonance Imaging (MRI). A method and design of apparatus for pumping the polarization of noble gases is described. The method and apparatus enable production, storage and usage of hyperpolarized noble gases for different purposes, including Magnetic Resonance Imaging of human and animal subjects. Magnetic imaging agents breathed into lungs can be observed by the radio waves of the MRI scanner and report back physical and functional information about lung's health and desease. The technique known as spin exchange optical pumping ismore » used. Nuclear magnetic resonance is implemented to measure the polarization of hyperpolarized gas. The cells prepared and sealed under high vacuum after handling Alkali metals into the cell and filling with the {sup 3}He-N{sub 2} mixture. The cells could be refilled. The {sup 3}He reaches around 50% polarization in 5-15 hours.« less

Noble gas as tracers for CO2 deep input in petroleum reservoirs

NASA Astrophysics Data System (ADS)

Pujol, Magali; Stuart, Finlay; Gilfillan, Stuart; Montel, François; Masini, Emmanuel

2016-04-01

The sub-salt hydrocarbon reservoirs in the deep offshore part of the Atlantic Ocean passive margins are a new key target for frontier oil and gas exploration. Type I source rocks locally rich in TOC (Total Organic Carbon) combined with an important secondary connected porosity of carbonate reservoirs overlain by an impermeable salt layer gives rise to reservoirs with high petroleum potential. However, some target structures have been found to be mainly filled with CO2 rich fluids. δ13C of the CO2 is generally between -9 and -4 permil, compatible with a deep source (metamorphic or mantle). Understanding the origin of the CO2 and the relative timing of its input into reservoir layers in regard to the geodynamic context appears to be a key issue for CO2 risk evaluation. The inertness and ubiquity of noble gases in crustal fluids make them powerful tools to trace the origin and migration of mixed fluids (Ballentine and Burnard 2002). The isotopic signature of He, Ne and Ar and the elemental pattern (He to Xe) of reservoir fluid from pressurized bottom hole samples provide an insight into fluid source influences at each reservoir depth. Three main end-members can be mixed into reservoir fluids (e.g. Gilfillan et al., 2008): atmospheric signature due to aquifer recharge, radiogenic component from organic fluid ± metamorphic influence, and mantle input. Their relative fractionation provides insights into the nature of fluid transport (Burnard et al., 2012)and its relative migration timing. In the studied offshore passive margin reservoirs, from both sides of South Atlantic margin, a strong MORB-like magmatic CO2 influence is clear. Hence, CO2 charge must have occurred during or after lithospheric break-up. CO2 charge(s) history appears to be complex, and in some cases requires several inputs to generate the observed noble gas pattern. Combining the knowledge obtained from noble gas (origin, relative timing, number of charges) with organic geochemical and thermodynamic

Isotopic Evidence for a Martian Regolith Component in Martian Meteorites

NASA Technical Reports Server (NTRS)

Rao, M. N.; Nyquist, L. E.; Bogard, D. D.; Garrison, D. H.; Sutton, S.

2009-01-01

Noble gas measurements in gas-rich impact-melt (GRIM) glasses in EET79001 shergottite showed that their elemental and isotopic composition is similar to that of the Martian atmosphere [1-3]. The GRIM glasses contain large amounts of Martian atmospheric gases. Those measurements further suggested that the Kr isotopic composition of Martian atmosphere is approximately similar to that of solar Kr. The (80)Kr(sub n) - (80)Kr(sub M) mixing ratio in the Martian atmosphere reported here is approximately 3%. These neutron-capture reactions presumably occurred in the glass-precursor regolith materials containing Sm- and Br- bearing mineral phases near the EET79001/ Shergotty sites on Mars. The irradiated materials were mobilized into host rock voids either during shock-melting or possibly by earlier aeolian / fluvial activity.

Magma Dynamics at Mid-Ocean Ridges by Noble Gas Kinetic Fractionation: Assessment of Magmatic Ascent Rates and Mantle Composition

NASA Astrophysics Data System (ADS)

Paonita, A.; Martelli, M.

2007-12-01

Topical scientific literature on magma degassing at mid-ocean ridges more and more focuses on exsolution processes occurring under conditions that are far from thermodynamic equilibrium between bubbles and silicate melt. Indeed, the dynamics of magma ascent and decompression can be faster than that of CO2 diffusion into bubbles, in which case the diffusivity ratios among volatiles are the main control of the composition of the exsolving gas phase. We have developed a model of bubble growth in silicate melts that calculates the extent of both CO2 supersaturation and kinetic fractionation among noble gases in vesicles in relation to the decompressive rate of basaltic melts. The model predicts that, due to comparable Ar and CO2 diffusivity, magma degassing at low pressure fractionates both He/Ar and He/CO2 ratios by a similar extent, while the slower CO2 diffusion at high pressure causes early kinetic effects on Ar/CO2 ratio and dramatically changes the degassing paths. By using this tool, we have reviewed the global He-Ar-CO2 dataset of fluid inclusions in mid-ocean-ridge glasses. We display that non-equilibrium fractionations among He, Ar and CO2, driven by their different diffusivities in silicate melts, are common in most of the natural conditions of magma decompression and their signature strongly depends on pressure of degassing. The different geochemical signatures among suites of data coming from different ridge segments mainly depend on the depth of the magma chamber where the melt was stored. Moreover, variations inside a single suite emerge due to the interplay between variable ascent speed of magma and cooling rate of the emplaced lava. As a result, two data groups coming from the Pito Seamount suite (Easter Microplate East ridge), showing different degree of CO2 supersaturation and He/Ar fractionation, provide ascent rates which differ by ten folds or even more. The large variations in both the He/CO2 and Ar/CO2 ratios at almost constant He/Ar, displayed

Groundwater residence time and paleohydrology in the Baltic Artesian basin:isotope geochemical data

NASA Astrophysics Data System (ADS)

Vaikmae, R.; Gerber, C.; Purtschert, R.; Aeschbach, W.; Raidla, V., Sr.; Lu, Z. T.; Zappala, J. C.; Mueller, P.; Mokrik, R., Sr.; Jiang, W.

2016-12-01

In this study of the Cambrian aquifer system(CAS) in the Baltic Artesian Basin(BAS) (, chemistry, stable isotopes, noble gas measurements, and dating tracers were combined for study the flow and recharge dynamics of the system over the last million years We find that the variability in chemical composition, stable isotopes and noble gas content in the basin is predominately controlled by mixing of three distinct water masses: Holocene and Pleistocene interglacial water, glacial meltwater, and brine. 81Kr is a nearly ideal dating tracer for such old systems. The radiogenic 4He and 40Ar provide additional information, but are more difficult to interpret in terms of groundwater age. In this study, we did not consider diffusive loss of 81Kr to stagnant water, which might result in an overestimation of groundwater ages ). However, the relatively high porosity and large thickness of the CAS, together with the presumed high salinity and low Kr content of the stagnant water all diminish the effect of diffusive 81Kr loss on age estimates. Our results confirm that under normal conditions, underground production of 81Kr is not affecting the dating results. 81Kr, 4He, and 40Ar all indicate a residence time of the brine of more than 1-3 Ma. Some uncertainty about the brine formation process remains, but the combination of chemical and stable isotope composition of the brine, noble gas concentrations and dating results favors evaporative enrichment of seawater. Tracer ages of interglacial water and glacial meltwater are on the order of several hundred thousand years, which means that several reversals of the flow direction in the CAS as a result of the paleoclimatology of the area have to be taken into account. Under such conditions, small vertical leakage, through fracture zones for example, might considerably impact the net flow pattern. Due to the cyclic flow direction reversals, the aquifer was probably in a transient state over most of the last 1 Ma period.

Noble gases and halogens in Graves Nunataks 06129: The complex thermal history of a felsic asteroid crust

NASA Astrophysics Data System (ADS)

Claydon, Jennifer L.; Crowther, Sarah A.; Fernandes, Vera A.; Gilmour, Jamie D.

2015-06-01

The meteorite Graves Nunataks 06128/06129 is a rare example of felsic asteroidal crust. Knowledge of its history can help shed light on the evolution processes of planetesimals. The noble gases can be used to constrain both the chronology of meteorites and the processes that result in movements of volatile elements on asteroidal bodies. We have examined the I-Xe and Ar-Ar systems of the plagioclase-rich achondrite, Graves Nunataks 06129 by high-resolution laser step-heating of irradiated samples. Iodine and 129Xe∗ are both present but are released at different temperatures and do not show a correlation, therefore the I-Xe system in GRA 06129 has no chronological significance. We propose that radiogenic 129Xe∗ was lost from primary phases and parentless 129Xe∗ was later introduced into the rock by interaction with a fluid sourced from a reservoir that evolved with a high I/Xe ratio. This could have been the same halogen-rich fluid that induced the conversion of merrillite and pyroxene into chlorapatite. Inherited 40Ar (i.e. not generated by in situ decay of 40K) is also present in one of three fragments studied here and may have been introduced at the same time as parentless 129Xe∗.

Noble Gases in Iddingsite from the Lafayette Meteorite: Evidence for Liquid Water on Mars in the Last Few Hundred Million Years

NASA Technical Reports Server (NTRS)

Swindle, T. D.; Treiman, A. H.; Lindstrom, D. J.; Brkland, M. K.; Cohen, B. A.; Grier, J. A.; Li, B.; Olson, E. K.

2000-01-01

We analyzed noble gases from 18 samples of weathering products ("iddingsite") from the Lafayette meteorite. Potassium-argon ages of 12 samples range from near zero to 670 +/- 91 Ma. These ages confirm the martian origin of the iddingsite, but it is not clear whether any or all of the ages represent iddingsite formation as opposed to later alteration or incorporation of martian atmospheric Ar-40. In any case, because iddingsite formation requires liquid water, this data requires the presence of liquid water near the surface of Mars at least as recently as 1300 Ma ago, and probably as recently as 650 Ma ago. Krypton and Xe analysis of a single 34 microg sample indicates the presence of fractionated martian atmosphere within the iddingsite. This also confirms the martian origin of the iddingsite. The mechanism of incorporation could either be through interaction with liquid water during iddingsite formation or a result of shock implantation of adsorbed atmospheric gas.

Late Impacts and the Origins of the Atmospheres on the Terrestrial Planets

NASA Astrophysics Data System (ADS)

Mukhopadhyay, S.; Stewart, S. T.; Lock, S. J.; Parai, R.; Tucker, J. M.

2014-12-01

Models for the origin of terrestrial atmospheres typically require an intricate sequence of events, including hydrodynamic escape, outgassing of mantle volatiles and late delivery. Here we discuss the origin of the atmospheres on the terrestrial planets in light of new ideas about the formation of the Moon, giant impact induced atmospheric loss and recent noble gas measurements. Our new measurements indicate that noble gases in the Earth's atmosphere cannot be derived from any combination of fractionation of a nebular-derived atmosphere followed by outgassing of deep or shallow mantle volatiles. While Ne in the mantle retains a nebular component, the present-day atmosphere has no memory of nebular gases. Rather, atmospheric noble gases have a close affinity to chondrites. On the other hand, Venus's atmosphere has 20 and 70 times higher abundance of 20Ne and 36Ar, respectively, and a 20Ne/22Ne ratio closer to the solar value than Earth's atmosphere. While the present atmosphere of Mars is significantly fractionated in the lighter noble gases due to long term atmospheric escape, the Kr isotopic ratios in Martian atmosphere are identical to solar. Thus, while Earth's atmosphere has no memory of accretion of nebular gases, atmospheres on both Venus and Mars preserve at least a component of nebular gases. To explain the above observations, we propose that a common set of processes operated on the terrestrial planets, and that their subsequent evolutionary divergence is simply explained by planetary size and the stochastic nature of giant impacts. We present geochemical observations and simulations of giant impacts to show that most of Earth's mantle was degassed and the outgassed volatiles were largely lost during the final sequence of giant impacts onto Earth. Earth's noble gases were therefore dominantly derived from late-accreting planetesimals. In contrast, Venus did not suffer substantial atmospheric loss by a late giant impact and retains a higher abundance of

Screening metal-organic frameworks for selective noble gas adsorption in air: effect of pore size and framework topology.

PubMed

Parkes, Marie V; Staiger, Chad L; Perry, John J; Allendorf, Mark D; Greathouse, Jeffery A

2013-06-21

The adsorption of noble gases and nitrogen by sixteen metal-organic frameworks (MOFs) was investigated using grand canonical Monte Carlo simulation. The MOFs were chosen to represent a variety of net topologies, pore dimensions, and metal centers. Three commercially available MOFs (HKUST-1, AlMIL-53, and ZIF-8) and PCN-14 were also included for comparison. Experimental adsorption isotherms, obtained from volumetric and gravimetric methods, were used to compare krypton, argon, and nitrogen uptake with the simulation results. Simulated trends in gas adsorption and predicted selectivities among the commercially available MOFs are in good agreement with experiment. In the low pressure regime, the expected trend of increasing adsorption with increasing noble gas polarizabilty is seen. For each noble gas, low pressure adsorption correlates with several MOF properties, including free volume, topology, and metal center. Additionally, a strong correlation exists between the Henry's constant and the isosteric heat of adsorption for all gases and MOFs considered. Finally, we note that the simulated and experimental gas selectivities demonstrated by this small set of MOFs show improved performance compared to similar values reported for zeolites.

Origin and Processes Highlighted By Noble Gases Geochemistry of Submarine Gas Emissions from Seeps at the Aquitaine Shelf (Bay of Biscay):

NASA Astrophysics Data System (ADS)

Battani, A.; Ruffine, L.; Donval, J. P.; Bignon, L.; Pujol, M.; Levaché, D.

2014-12-01

Noble gases are widely used as tracers to both determine fluid origin and identify transfer processes governing fluid flow in natural systems. This work presents the preliminary results and interpretations from submarine gas samples collected during the GAZCOGNE2 cruise (2013). The seepage activity and the spatial distribution of the widespread emission sites encountered at this area are described by (Dupré et al. 2014). Gas composition shows that methane is the dominant species compared to the C2+. The associated δ13C and δD signatures point to a biogenic origin- through CO2 reduction- of the gas. Helium concentrations are very low, ranging from 0.1 and 2.3 ppm, indicating a low residence time of the fluids in the subsurface. However, the resulting helium isotopic ratios are mostly crustal fingerprinted (around 0.02). The R/Ra values sometimes exhibit higher value of 0.2, indicative either an ASW (air saturated water) value, or the fingerprint of ancient mantle helium, the later in agreement with the geological structural context of the Parentis Basin. Most of the samples exhibit a mixing between ASW and air, probably by excess air addition to the initial ASW concentration. The elemental Ne/Ar ratio is remarkably constant for the totality of the samples, with a value typical of ASW (0.2). This result implies that the migrating gas phase is "stripping" the original water matrix from its noble gas content, as described by Gillfillian et al., 2008. This further indicates that an intermediate reservoir of biogenic gas should be present at depth. The GAZCOGNE study is co-funded by TOTAL and IFREMER as part of the PAMELA (Passive Margin Exploration Laboratories) scientific project. References: Dupré, S., L. Berger, N. Le Bouffant, C. Scalabrin, and J. F. Bourillet (2014), Fluid emissions at the Aquitaine Shelf (Bay of Biscay, France): a biogenic origin or the expression of hydrocarbon leakage?, Continental Shelf Research, doi:10.1016/j.csr.2014.07.004. Gilfillan S

On the siting of gases shock-emplaced from internal cavities in basalt

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wiens, R.C.

1988-12-01

Noble gases were extracted by stepped combustion and crushing from basalts which contained gas-filled cavities of controlled sizes prior to shock at 40 GPa. Analysis of fractions enriched and depleted in shock glass from a single sample gave a factor of 2 higher gas abundances in the glass-rich separate. Release patterns were nearly identical, suggesting similar siting (in glass) in both fractions. Crushing of a sample released {approximately}45% of implanted noble gases, but only {approximately}17% of N{sub 2}, indicating that most or all of the noble gas was trapped in vesicles. Analysis by SEM/EDS confirmed the presence of vesicles inmore » glassy areas, with an average diameter of {approximately}10 {mu}m. Samples with relatively large pre-shock cavities were found to consist of up to 70-80% glass locally and generally exhibit greater local shock effects than solid and densely-packed particulate targets at the same shock pressure, though the latter give higher glass emplacement efficiencies. The petrographic results indicate that in situ production of glassy pockets grossly similar to those in the shergottite EETA 79001 is possible from shock reverberations in the vicinity of a vug. However, the siting of the gases points to a more complex scenario, in which SPB gas and melt material were probably injected into EETA 79001.« less

Issues Involving The OSI Concept of Operation For Noble Gas Radionuclide Detection

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carrigan, C R; Sun, Y

2011-01-21

The development of a technically sound protocol for detecting the subsurface release of noble gas radionuclides is critical to the successful operation of an on site inspection (OSI) under the CTBT and has broad ramifications for all aspects of the OSI regime including the setting of specifications for both sampling and analysis equipment used during an OSI. With NA-24 support, we are investigating a variety of issues and concerns that have significant bearing on policy development and technical guidance regarding the detection of noble gases and the creation of a technically justifiable OSI concept of operation. The work at LLNLmore » focuses on optimizing the ability to capture radioactive noble gases subject to the constraints of possible OSI scenarios. This focus results from recognizing the difficulty of detecting gas releases in geologic environments - a lesson we learned previously from the LLNL Non-Proliferation Experiment (NPE). Evaluation of a number of important noble gas detection issues, potentially affecting OSI policy, has awaited the US re-engagement with the OSI technical community. Thus, there have been numerous issues to address during the past 18 months. Most of our evaluations of a sampling or transport issue necessarily involve computer simulations. This is partly due to the lack of OSI-relevant field data, such as that provided by the NPE, and partly a result of the ability of LLNL computer-based models to test a range of geologic and atmospheric scenarios far beyond what could ever be studied in the field making this approach very highly cost effective. We review some highlights of the transport and sampling issues we have investigated during the past year. We complete the discussion of these issues with a description of a preliminary design for subsurface sampling that is intended to be a practical solution to most if not all the challenges addressed here.« less

New experimental stopping power data of 4He, 16O, 40Ar, 48Ca and 84Kr projectiles in different solid materials

NASA Astrophysics Data System (ADS)

Trzaska, W. H.; Knyazheva, G. N.; Perkowski, J.; Andrzejewski, J.; Khlebnikov, S. V.; Kozulin, E. M.; Malkiewicz, T.; Mutterer, M.; Savelieva, E. O.

2018-03-01

New experimental data on energy loss of 4He, 16O, 40Ar, 48Ca and 84Kr ions in thin, self-supporting foils of C, Al, Ni, Ag, Lu, Au, Pb and Th are presented. The measurements, using the TOF-E method, were done in a very broad energy range around the stopping power maximum; typically from 0.1 to 11 MeV/u. When available, the extracted stopping power values are compared with the previously published data. The overall agreement is good although a fair comparison is difficult as the covered energy range is much larger than in previous measurements. The small error bars and a broad coverage allowed us to test the predictions of theoretical codes: PASS, CasP, and semi-empirical programs: SRIM, LET, MSTAR, and the Hubert table predictions. The deviations of PASS predictions from the experimental data do not exceed 20% for all the measured combinations. CasP predictions are within 15% from the data for heavier ions but diverge up to 40% for lighter ions. Semi-empirical approaches, including SRIM, deviate from the experimental data by less than 5% for the regions already covered by previous experiments but err by about 10-20% for the ion/target combinations that were not measured before: Ca in Lu as well as Kr in Lu, Pb, and Th.

Noble gas composition of subcontinental lithospheric mantle: An extensively degassed reservoir beneath Southern Patagonia

NASA Astrophysics Data System (ADS)

Jalowitzki, Tiago; Sumino, Hirochika; Conceição, Rommulo V.; Orihashi, Yuji; Nagao, Keisuke; Bertotto, Gustavo W.; Balbinot, Eduardo; Schilling, Manuel E.; Gervasoni, Fernanda

2016-09-01

Patagonia, in the Southern Andes, is one of the few locations where interactions between the oceanic and continental lithosphere can be studied due to subduction of an active spreading ridge beneath the continent. In order to characterize the noble gas composition of Patagonian subcontinental lithospheric mantle (SCLM), we present the first noble gas data alongside new lithophile (Sr-Nd-Pb) isotopic data for mantle xenoliths from Pali-Aike Volcanic Field and Gobernador Gregores, Southern Patagonia. Based on noble gas isotopic compositions, Pali-Aike mantle xenoliths represent intrinsic SCLM with higher (U + Th + K)/(3He, 22Ne, 36Ar) ratios than the mid-ocean ridge basalt (MORB) source. This reservoir shows slightly radiogenic helium (3He/4He = 6.84-6.90 RA), coupled with a strongly nucleogenic neon signature (mantle source 21Ne/22Ne = 0.085-0.094). The 40Ar/36Ar ratios vary from a near-atmospheric ratio of 510 up to 17700, with mantle source 40Ar/36Ar between 31100-6800+9400 and 54000-9600+14200. In addition, the 3He/22Ne ratios for the local SCLM endmember, at 12.03 ± 0.15 to 13.66 ± 0.37, are higher than depleted MORBs, at 3He/22Ne = 8.31-9.75. Although asthenospheric mantle upwelling through the Patagonian slab window would result in a MORB-like metasomatism after collision of the South Chile Ridge with the Chile trench ca. 14 Ma, this mantle reservoir could have remained unhomogenized after rapid passage and northward migration of the Chile Triple Junction. The mantle endmember xenon isotopic ratios of Pali-Aike mantle xenoliths, which is first defined for any SCLM-derived samples, show values indistinguishable from the MORB source (129Xe/132Xe =1.0833-0.0053+0.0216 and 136Xe/132Xe =0.3761-0.0034+0.0246). The noble gas component observed in Gobernador Gregores mantle xenoliths is characterized by isotopic compositions in the MORB range in terms of helium (3He/4He = 7.17-7.37 RA), but with slightly nucleogenic neon (mantle source 21Ne/22Ne = 0.065-0.079). We

High temperature, oxidation resistant noble metal-Al alloy thermocouple

NASA Technical Reports Server (NTRS)

Smialek, James L. (Inventor); Gedwill, Michael G. (Inventor)

1994-01-01

A thermocouple is disclosed. The thermocouple is comprised of an electropositive leg formed of a noble metal-Al alloy and an electronegative leg electrically joined to form a thermocouple junction. The thermocouple provides for accurate and reproducible measurement of high temperatures (600 - 1300 C) in inert, oxidizing or reducing environments, gases, or vacuum. Furthermore, the thermocouple circumvents the need for expensive, strategic precious metals such as rhodium as a constituent component. Selective oxidation of rhodium is also thereby precluded.

Crater function moments: Role of implanted noble gas atoms

NASA Astrophysics Data System (ADS)

Hobler, Gerhard; Maciążek, Dawid; Postawa, Zbigniew

2018-04-01

Spontaneous pattern formation by energetic ion beams is usually explained in terms of surface-curvature dependent sputtering and atom redistribution in the target. Recently, the effect of ion implantation on surface stability has been studied for nonvolatile ion species, but for the case of noble gas ion beams it has always been assumed that the implanted atoms can be neglected. In this work, we show by molecular dynamics (MD) and Monte Carlo (MC) simulations that this assumption is not valid in a wide range of implant conditions. Sequential-impact MD simulations are performed for 1-keV Ar, 2-keV Kr, and 2-keV Xe bombardments of Si, starting with a pure single-crystalline Si target and running impacts until sputtering equilibrium has been reached. The simulations demonstrate the importance of the implanted ions for crater-function estimates. The atomic volumes of Ar, Kr, and Xe in Si are found to be a factor of two larger than in the solid state. To extend the study to a wider range of energies, MC simulations are performed. We find that the role of the implanted ions increases with the ion energy although the increase is attenuated for the heavier ions. The analysis uses the crater function formalism specialized to the case of sputtering equilibrium.

The Origin of Noble Gas Isotopic Heterogeneity in Icelandic Basalts

NASA Technical Reports Server (NTRS)

Dixon, E. T.; Honda, M.; McDougall, I.

2001-01-01

Two models for generation of heterogeneous He, Ne and Ar isotopic ratios in Icelandic basalts are evaluated using a mixing model and the observed noble gas elemental ratios in Icelandic basalts,Ocean island Basalt (OIBs) and Mid-Ocean Ridge Basalt (MORBs). Additional information is contained in the original extended abstract.

Matrix effect on vibrational frequencies: Experiments and simulations for HCl and HNgCl (Ng = Kr and Xe)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kalinowski, Jaroslaw; Räsänen, Markku; Lignell, Antti

2014-03-07

We study the environmental effect on molecules embedded in noble-gas (Ng) matrices. The experimental data on HXeCl and HKrCl in Ng matrices is enriched. As a result, the H−Xe stretching bands of HXeCl are now known in four Ng matrices (Ne, Ar, Kr, and Xe), and HKrCl is now known in Ar and Kr matrices. The order of the H−Xe stretching frequencies of HXeCl in different matrices is ν(Ne) < ν(Xe) < ν(Kr) < ν(Ar), which is a non-monotonous function of the dielectric constant, in contrast to the “classical” order observed for HCl: ν(Xe) < ν(Kr) < ν(Ar) < ν(Ne).more » The order of the H−Kr stretching frequencies of HKrCl is consistently ν(Kr) < ν(Ar). These matrix effects are analyzed theoretically by using a number of quantum chemical methods. The calculations on these molecules (HCl, HXeCl, and HKrCl) embedded in single Ng{sup ′} layer cages lead to very satisfactory results with respect to the relative matrix shifts in the case of the MP4(SDQ) method whereas the B3LYP-D and MP2 methods fail to fully reproduce these experimental results. The obtained order of frequencies is discussed in terms of the size available for the Ng hydrides in the cages, probably leading to different stresses on the embedded molecule. Taking into account vibrational anharmonicity produces a good agreement of the MP4(SDQ) frequencies of HCl and HXeCl with the experimental values in different matrices. This work also highlights a number of open questions in the field.« less

Pathway to Cryogen Free Production of Hyperpolarized Krypton-83 and Xenon-129

PubMed Central

Six, Joseph S.; Hughes-Riley, Theodore; Stupic, Karl F.; Pavlovskaya, Galina E.; Meersmann, Thomas

2012-01-01

Hyperpolarized (hp) 129Xe and hp 83Kr for magnetic resonance imaging (MRI) are typically obtained through spin-exchange optical pumping (SEOP) in gas mixtures with dilute concentrations of the respective noble gas. The usage of dilute noble gases mixtures requires cryogenic gas separation after SEOP, a step that makes clinical and preclinical applications of hp 129Xe MRI cumbersome. For hp 83Kr MRI, cryogenic concentration is not practical due to depolarization that is caused by quadrupolar relaxation in the condensed phase. In this work, the concept of stopped flow SEOP with concentrated noble gas mixtures at low pressures was explored using a laser with 23.3 W of output power and 0.25 nm linewidth. For 129Xe SEOP without cryogenic separation, the highest obtained MR signal intensity from the hp xenon-nitrogen gas mixture was equivalent to that arising from 15.5±1.9% spin polarized 129Xe in pure xenon gas. The production rate of the hp gas mixture, measured at 298 K, was 1.8 cm3/min. For hp 83Kr, the equivalent of 4.4±0.5% spin polarization in pure krypton at a production rate of 2 cm3/min was produced. The general dependency of spin polarization upon gas pressure obtained in stopped flow SEOP is reported for various noble gas concentrations. Aspects of SEOP specific to the two noble gas isotopes are discussed and compared with current theoretical opinions. A non-linear pressure broadening of the Rb D1 transition was observed and taken into account for the qualitative description of the SEOP process. PMID:23209620

International comparison CCQM-K113—noble gas mixture

NASA Astrophysics Data System (ADS)

Lim, Jeong Sik; Lee, Jinbok; Moon, Dongmin; Tshilongo, James; Qiao, Han; Shuguo, Hu; Tiqiang, Zhang; Kelley, Michael E.; Rhoderick, George C.; Konopelko, L. A.; Kolobova, A. V.; Vasserman, I. I.; Zavyalov, S. V.; Gromova, E. V.; Efremova, O. V.

2017-01-01

Noble gases are one of the key elements used in the various processes of the bulbs industry, automotive industry, space industry, lasers industry, display industry as well as the semiconductor industry. Considering continuous growth, the provision of a reliable standard is required for those industries to improve their productivity. In this report, a result of the key comparison, CCQM-K113: noble gas mixture, is presented. Nominal amount-of-substance fractions of argon, neon, krypton, and xenon in helium are 20, 10, 2, and 1 cmol/mol, respectively. Main text To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCQM, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

Irreversible adsorption of atmospheric helium on olivine: A lobster pot analogy

NASA Astrophysics Data System (ADS)

Protin, Marie; Blard, Pierre-Henri; Marrocchi, Yves; Mathon, François

2016-04-01

This study reports new experimental results that demonstrate that large amounts of atmospheric helium may be adsorbed onto the surfaces of olivine grains. This behavior is surface-area-related in that this contamination preferentially affects grains that are smaller than 125 μm in size. One of the most striking results of our study is that in vacuo heating at 900 °C for 15 min is not sufficient to completely remove the atmospheric contamination. This suggests that the adsorption of helium may involve high-energy trapping of helium through irreversible anomalous adsorption. This trapping process of helium can thus be compared to a ;lobster pot; adsorption: atmospheric helium easily gets in, but hardly gets out. While this type of behavior has previously been reported for heavy noble gases (Ar, Kr, Xe), this is the first time that it has been observed for helium. Adsorption of helium has, until now, generally been considered to be negligible on silicate surfaces. Our findings have significant implications for helium and noble gas analysis of natural silicate samples, such as for cosmic-ray exposure dating or noble gas characterization of extraterrestrial material. Analytical procedures in future studies should be adapted in order to avoid this contamination. The results of this study also allow us to propose an alternative explanation for previously described matrix loss of cosmogenic 3He.

In situ measurement of atmospheric krypton and xenon on Mars with Mars Science Laboratory

DOE PAGES

Conrad, P. G.; Malespin, C. A.; Franz, H. B.; ...

2016-11-01

Mars Science Laboratory's Sample Analysis at Mars (SAM) investigation has measured all of the stable isotopes of the heavy noble gases krypton and xenon in the martian atmosphere, in situ, from the Curiosity Rover at Gale Crater, Mars. Previous knowledge of martian atmospheric krypton and xenon isotope ratios has been based upon a combination of the Viking mission's krypton and xenon detections and measurements of noble gas isotope ratios in martian meteorites. But, the meteorite measurements reveal an impure mixture of atmospheric, mantle, and spallation contributions. The xenon and krypton isotopic measurements reported here include the complete set of stablemore » isotopes, unmeasured by Viking. Our new results generally agree with Mars meteorite measurements but also provide a unique opportunity to identify various non-atmospheric heavy noble gas components in the meteorites. Kr isotopic measurements define a solar-like atmospheric composition, but deviating from the solar wind pattern at 80Kr and 82Kr in a manner consistent with contributions originating from neutron capture in Br. The Xe measurements suggest an intriguing possibility that isotopes lighter than 132Xe have been enriched to varying degrees by spallation and neutron capture products degassed to the atmosphere from the regolith, and a model is constructed to explore this possibility. Such a spallation component, but, is not apparent in atmospheric Xe trapped in the glassy phases of martian meteorites.« less

In situ measurement of atmospheric krypton and xenon on Mars with Mars Science Laboratory

NASA Astrophysics Data System (ADS)

Conrad, P. G.; Malespin, C. A.; Franz, H. B.; Pepin, R. O.; Trainer, M. G.; Schwenzer, S. P.; Atreya, S. K.; Freissinet, C.; Jones, J. H.; Manning, H.; Owen, T.; Pavlov, A. A.; Wiens, R. C.; Wong, M. H.; Mahaffy, P. R.

2016-11-01

Mars Science Laboratory's Sample Analysis at Mars (SAM) investigation has measured all of the stable isotopes of the heavy noble gases krypton and xenon in the martian atmosphere, in situ, from the Curiosity Rover at Gale Crater, Mars. Previous knowledge of martian atmospheric krypton and xenon isotope ratios has been based upon a combination of the Viking mission's krypton and xenon detections and measurements of noble gas isotope ratios in martian meteorites. However, the meteorite measurements reveal an impure mixture of atmospheric, mantle, and spallation contributions. The xenon and krypton isotopic measurements reported here include the complete set of stable isotopes, unmeasured by Viking. The new results generally agree with Mars meteorite measurements but also provide a unique opportunity to identify various non-atmospheric heavy noble gas components in the meteorites. Kr isotopic measurements define a solar-like atmospheric composition, but deviating from the solar wind pattern at 80Kr and 82Kr in a manner consistent with contributions originating from neutron capture in Br. The Xe measurements suggest an intriguing possibility that isotopes lighter than 132Xe have been enriched to varying degrees by spallation and neutron capture products degassed to the atmosphere from the regolith, and a model is constructed to explore this possibility. Such a spallation component, however, is not apparent in atmospheric Xe trapped in the glassy phases of martian meteorites.

In Situ Measurement of Atmospheric Krypton and Xenon on Mars with Mars Science Laboratory

NASA Technical Reports Server (NTRS)

Conrad, P. G.; Malespin, C. A.; Franz, H. B.; Pepin, R. O.; Trainer, M. G.; Schwenzer, S. P.; Atreya, S. K.; Freissinet, C.; Jones, J. H.; Manning, H.;

In situ measurement of atmospheric krypton and xenon on Mars with Mars Science Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Conrad, P. G.; Malespin, C. A.; Franz, H. B.

Mars Science Laboratory's Sample Analysis at Mars (SAM) investigation has measured all of the stable isotopes of the heavy noble gases krypton and xenon in the martian atmosphere, in situ, from the Curiosity Rover at Gale Crater, Mars. Previous knowledge of martian atmospheric krypton and xenon isotope ratios has been based upon a combination of the Viking mission's krypton and xenon detections and measurements of noble gas isotope ratios in martian meteorites. But, the meteorite measurements reveal an impure mixture of atmospheric, mantle, and spallation contributions. The xenon and krypton isotopic measurements reported here include the complete set of stablemore » isotopes, unmeasured by Viking. Our new results generally agree with Mars meteorite measurements but also provide a unique opportunity to identify various non-atmospheric heavy noble gas components in the meteorites. Kr isotopic measurements define a solar-like atmospheric composition, but deviating from the solar wind pattern at 80Kr and 82Kr in a manner consistent with contributions originating from neutron capture in Br. The Xe measurements suggest an intriguing possibility that isotopes lighter than 132Xe have been enriched to varying degrees by spallation and neutron capture products degassed to the atmosphere from the regolith, and a model is constructed to explore this possibility. Such a spallation component, but, is not apparent in atmospheric Xe trapped in the glassy phases of martian meteorites.« less

The atmospheric inventory of Xenon and noble cases in shales The plastic bag experiment

NASA Technical Reports Server (NTRS)

Bernatowicz, T. J.; Podosek, F. A.; Honda, M.; Kramer, F. E.

1984-01-01

A novel trapped gas analysis protocol is applied to five shales in which the samples are sealed in air to eliminate the possibility of gas loss in the preanalysis laboratory vacuum exposure of a conventional protocol. The test is aimed at a determination concerning the hypothesis that atmospheric noble gases occur in the same proportion as planetary gases in meteorites, and that the factor-of-23 deficiency of air Xe relative to planetary Xe is made up by Xe stored in shales or other sedimentary rocks. The results obtained do not support the shale hypothesis.

Using noble gases measured in spring discharge to trace hydrothermal processes in the Norris Geyser Basin, Yellowstone National Park, U.S.A.

USGS Publications Warehouse

Gardner, W.P.; Susong, D.D.; Solomon, D.K.; Heasler, H.P.

2010-01-01

Dissolved noble gas concentrations in springs are used to investigate boiling of hydrothermal water and mixing of hydrothermal and shallow cool water in the Norris Geyser Basin area. Noble gas concentrations in water are modeled for single stage and continuous steam removal. Limitations on boiling using noble gas concentrations are then used to estimate the isotopic effect of boiling on hydrothermal water, allowing the isotopic composition of the parent hydrothermal water to be determined from that measured in spring. In neutral chloride springs of the Norris Geyser Basin, steam loss since the last addition of noble gas charged water is less than 30% of the total hydrothermal discharge, which results in an isotopic shift due to boiling of ?? 2.5% ??D. Noble gas concentrations in water rapidly and predictably change in dual phase systems, making them invaluable tracers of gas-liquid interaction in hydrothermal systems. By combining traditional tracers of hydrothermal flow such as deuterium with dissolved noble gas measurements, more complex hydrothermal processes can be interpreted. ?? 2010 Elsevier B.V.

Production of Mg and Al Auger electrons by noble gas ion bombardment of Mg and Al surfaces

NASA Technical Reports Server (NTRS)

Ferrante, J.; Pepper, S. V.

1976-01-01

Relative production efficiencies of Mg and Al Auger electrons by He, Ne, Ar, Kr, and Xe ion bombardment are reported as a function of ion energy for energies not exceeding 3 keV. The experimental apparatus employed consisted of a LEED-Auger system equipped with an ion gun and a four-grid retarding-potential analyzer. It is found that: (1) the shape of the ion-excited Auger signal was independent of the rare gas and quite symmetric; (2) the Al signal was about an order of magnitude smaller than the Mg signal for a given bombarding species and ion-gun voltage; (3) no signal was observed for He(+) bombardment under any of the experimental conditions; (4) signal strengths were independent of temperature and ion dose; (5) the Auger production efficiencies differed by no more than a factor of two among the different gases - except for He(+) - on a given metal; (6) all the signal strengths increased with increasing ion-gun voltage, with no maximum exhibited; and (7) the apparent threshold energy for the Al signal was higher than that for the Mg signal. The differences between the results for the two metals are attributed to the fact that the Al 2p orbital lies deeper in energy and closer to the nucleus than the corresponding Mg orbital.

A review of noble gas geochemistry in relation to early Earth history

NASA Technical Reports Server (NTRS)

Kurz, M. D.

1985-01-01

One of the most fundamental noble gas constraints on early Earth history is derived from isotopic differences in (129)Xe/(130)Xe between various terrestrial materials. The short half life (17 m.y.) of extinct (129I, parent of (129)Xe, means that these differences must have been produced within the first 100 m.y. after terrestrial accretion. The identification of large anomalies in (129)Xe/(130)Xe in mid ocean ridge basalts (MORB), with respect to atmospheric xenon, suggests that the atmosphere and upper mantle have remained separate since that time. This alone is a very strong argument for early catastrophic degassing, which would be consistent with an early fractionation resulting in core formation. However, noble gas isotopic systematics of oceanic basalts show that the mantle cannot necessarily be regarded as a homogeneous system, since there are significant variations in (3)He/(4)He, (40)Ar/(36)Ar, and (129)Xe/(130)Xe. Therefore, the early degassing cannot be considered to have acted on the whole mantle. The specific mechanisms of degassing, in particular the thickness and growth of the early crust, is an important variable in understanding present day noble gas inventories. Another constraint can be obtained from rocks that are thought to be derived from near the lithosphere asthenosphere boundary: ultramafic xenoliths.

Protracted storage of CR chondrules in a region of the disk transparent to galactic cosmic rays

NASA Astrophysics Data System (ADS)

Roth, Antoine S. G.; Metzler, Knut; Baumgartner, Lukas P.; Hofmann, Beda A.; Leya, Ingo

2017-10-01

Renazzo-type carbonaceous (CR) chondrites are accretionary breccias that formed last. As such they are ideal samples to study precompaction exposures to cosmic rays. Here, we present noble gas data for 24 chondrules and 3 dark inclusion samples (DIs) from Shişr 033 (CR2). The meteorite was selected based on the absence of implanted solar wind noble gases and an anomalous oxygen isotopic composition of the DIs; the oxygen isotopes match those in CV3 and CO3 chondrites. Our samples contain variable mixtures of galactic cosmic ray (GCR)-produced cosmogenic noble gases and trapped noble gases of presolar origin. Remarkably, all chondrules have cosmogenic 3He and 21Ne concentrations up to 4.3 and 7.1 times higher than the DIs, respectively. We derived an average 3He-21Ne cosmic ray exposure (CRE) age for Shişr 033 of 2.03 ± 0.20 Ma (2 SD) and excesses in cosmogenic 3He and 21Ne in chondrules (relative to the DIs) in the range (in 10-8 cm3STP/g) 3.99-7.76 and 0.94-1.71, respectively. Assuming present-day GCR flux density, the excesses translate into average precompaction 3He-21Ne CRE ages of 3.1-27.3 Ma depending on the exposure geometry. The data can be interpreted assuming a protracted storage of a single chondrule generation prior to the final assembly of the Shişr 033 parent body in a region of the disk transparent to GCRs.

CO-oxidation catalysts: Low-temperature CO oxidation over Noble-Metal Reducible Oxide (NMRO) catalysts

NASA Technical Reports Server (NTRS)

Herz, Richard K.

1990-01-01

Oxidation of CO to CO2 is an important reaction technologically and environmentally and a complex and interesting reaction scientifically. In most cases, the reaction is carried out in order to remove CO as an environmental hazard. A major application of heterogeneous catalysts is catalytic oxidation of CO in the exhaust of combustion devices. The reaction over catalysts in exhaust gas is fast and often mass-transfer-limited since exhaust gases are hot and O2/CO ratios are high. The main challenges to catalyst designers are to control thermal sintering and chemical poisoning of the active materials. The effect of the noble metal on the oxide is discussed, followed by the effect of the oxide on the noble metal, the interaction of the noble metal and oxide to form unique catalytic sites, and the possible ways in which the CO oxidation reaction is catalyzed by the NMRO materials.

Low-field MRI of laser polarized noble gas

NASA Technical Reports Server (NTRS)

Tseng, C. H.; Wong, G. P.; Pomeroy, V. R.; Mair, R. W.; Hinton, D. P.; Hoffmann, D.; Stoner, R. E.; Hersman, F. W.; Cory, D. G.; Walsworth, R. L.

1998-01-01

NMR images of laser polarized 3He gas were obtained at 21 G using a simple, homebuilt instrument. At such low fields magnetic resonance imaging (MRI) of thermally polarized samples (e.g., water) is not practical. Low-field noble gas MRI has novel scientific, engineering, and medical applications. Examples include portable systems for diagnosis of lung disease, as well as imaging of voids in porous media and within metallic systems.

Noble gas isotopes and halogens in volatile-rich inclusions in diamonds

NASA Technical Reports Server (NTRS)

Burgess, Raymond; Turner, Grenville

1994-01-01

Application of the (40)Ar-(39)Ar method and noble gas studies to diamonds has increased our understanding of their age relationships to the host kimberlite or lamproite, and of the source and composition of volatile-rich fluids in the upper mantle. The properties of diamond (inert, high mechanical strength and low gas diffusivities) means they are especially useful samples for studying gases trapped deep within the earth (less than 150 km) as they are unlikely to have undergone loss or exchange of entrapped material since formation. Volatile-rich fluids (H2O-CO2) are important agents for metasomatic processes in the upper mantle, and the noble gases and halogens preferentially partition into this phase leading to a strong geochemical coherence between these groups of elements. The abundances of the halogens in the major reservoirs of the Earth shows a marked progression from chlorine, concentrated in the oceans, through to iodine which, through its affinity to organic material, is concentrated mainly in sediments. Abundances in the upper mantle are low. This is particularly true for iodine which is of special interest in view of its potential significance as an indicator of sediment recycling and by way of its link to (129)Xe amomalies in the mantle through the low extinct isotope (129)I. Extensions of the (40)Ar-(39)Ar technique enable measurements of halogens and other elements (K, Ca, Ba, U) by production of noble gas isotopes from these species during neutron irradiation. Samples analyzed in this way include 15 coated stones from an unknown source in Zaire, 3 boarts from the Jwaneng and 1 boart from the Orapa kimberlites, both in Botswana.

Noble Gas Inventory of Micrometeorites Collected at the Transantarctic Mountains (TAM) and Indications for Their Provenance

NASA Technical Reports Server (NTRS)

Ott, U.; Baecker, B.; Folco, L.; Cordier, C.

2016-01-01

A variety of processes have been considered possibly contributing the volatiles including noble gases to the atmospheres of the terrestrial planets (e.g., [1-3]). Special consideration has been given to the concept of accretion of volatile-rich materials by the forming planets. This might include infalling planetesimals and dust, and could include material from the outer asteroid belt, as well as cometary material from the outer solar system. Currently, the dominant source of extraterrestrial material accreted by the Earth is represented by micrometeorites (MMs) with sizes mostly in the 100-300 micron range [3, 4]). Their role has been assessed by [3], who conclude that accretion of early micrometeorites played a major role in the formation of the terrestrial atmosphere and oceans. We have therefore set out to investigate in more detail the inventory of noble gases in MMs. Here we summarize some of our results obtained on MMs collected in micrometeorite traps of the Transantarctic Mountains [5].

Simulation of angular-resolved RABBITT measurements in noble-gas atoms

NASA Astrophysics Data System (ADS)

Bray, Alexander W.; Naseem, Faiza; Kheifets, Anatoli S.

2018-06-01

We simulate angular-resolved RABBITT (reconstruction of attosecond beating by interference of two-photon transitions) measurements on valence shells of noble-gas atoms (Ne, Ar, Kr, and Xe). Our nonperturbative numerical simulation is based on solution of the time-dependent Schrödinger equation (TDSE) for a target atom driven by an ionizing XUV and dressing IR fields. From these simulations we extract the angular-dependent magnitude and phase of the RABBITT oscillations and deduce the corresponding angular anisotropy β parameter and Wigner time delay τW for the single XUV photon absorption that initiates the RABBITT process. Said β and τW parameters are compared with calculations in the random-phase approximation with exchange (RPAE), which includes intershell correlation. This comparison is used to test various effective potentials employed in the one-electron TDSE. In lighter atoms (Ne and Ar), several effective potentials are found to provide accurate simulations of RABBITT measurements for a wide range of photon energies up to 100 eV above the valence-shell threshold. In heavier atoms (Kr and Xe), the onset of strong correlation with the d shell restricts the validity of the single active electron approximation to several tens of eV above the valence-shell threshold.

Noble gas signatures in the Island of Maui, Hawaii: Characterizing groundwater sources in fractured systems

USGS Publications Warehouse

Niu, Yi; Castro, M. Clara; Hall, Chris M.; Gingerich, Stephen B.; Scholl, Martha A.; Warrier, Rohit B.

2017-01-01

Uneven distribution of rainfall and freshwater scarcity in populated areas in the Island of Maui, Hawaii, renders water resources management a challenge in this complex and ill-defined hydrological system. A previous study in the Galapagos Islands suggests that noble gas temperatures (NGTs) record seasonality in that fractured, rapid infiltration groundwater system rather than the commonly observed mean annual air temperature (MAAT) in sedimentary systems where infiltration is slower thus, providing information on recharge sources and potential flow paths. Here we report noble gas results from the basal aquifer, springs, and rainwater in Maui to explore the potential for noble gases in characterizing this type of complex fractured hydrologic systems. Most samples display a mass-dependent depletion pattern with respect to surface conditions consistent with previous observations both in the Galapagos Islands and Michigan rainwater. Basal aquifer and rainwater noble gas patterns are similar and suggest direct, fast recharge from precipitation to the basal aquifer. In contrast, multiple springs, representative of perched aquifers, display highly variable noble gas concentrations suggesting recharge from a variety of sources. The distinct noble gas patterns for the basal aquifer and springs suggest that basal and perched aquifers are separate entities. Maui rainwater displays high apparent NGTs, incompatible with surface conditions, pointing either to an origin at high altitudes with the presence of ice or an ice-like source of undetermined origin. Overall, noble gas signatures in Maui reflect the source of recharge rather than the expected altitude/temperature relationship commonly observed in sedimentary systems.

Quantitative assessment of magmatic refill and overpressure in crustal reservoirs by monitoring He isotope composition from volcanic gases: the case of Mt Etna (Italy)

NASA Astrophysics Data System (ADS)

Paonita, Antonio; Caracausi, Antonio; Martelli, Mauro; Rizzo, Andrea

2016-04-01

There is agreement in recognizing episodes of magma injection into crustal chambers as main triggers of eruptive activity of volcanoes (Caricchi et al., 2014). These events cause in fact a buildup of the internal pressure in magma chamber, which in turn controls outpouring magma amount, possible failure of wall-rocks, dike opening, up to a potential eruption. Assessment of the time-dependent pressurization while occurring in chamber is therefore challenging aim of current volcanological research. Recent advancements in estimating the time-dependent pressurization as long as occurring in chamber come from inverse modeling of ground deformation data, which does not however calculate internal evolution of the magma reservoir (Gregg et al., 2013; Cannavò et al., 2015). On the other hand, the geochemistry of volcanic gases has basically addressed to the pressure(depth) of gas exsolution so far (Caracausi et al., 2003; Aiuppa et al., 2007; Paonita et al., 2012). We developed an pioneering tool that computes the changes of 3He/4He isotope ratio of volcanic gases with respect to a background, as a function of the time-dependent outflow of volatiles from a chamber subjected to evolution of internal pressure through an injection event. Our approach postulates a low-3He/4He gas endmember coming from resident magmas stored in crust, that mixes with a high-3He/4He gas endmember from deep parental magmas refilling the deep chamber. We couple a mass balance between the two gas endmembers to a physical model of the magma chamber. When a deep input pressurizes the chamber, the latter releases large amounts of the high-3He/4He gas endmember, so as to change 3He/4He of discharged volcanic gases. We applied the model to the long-term series of He isotope ratios from geochemical monitoring of some peripheral gas emissions at the base of Mt Etna, fed by magmatic degassing occurring at 200-400 MPa (Paonita et al., 2012). The isotope ratios have in fact displayed phases of increase

Clast Selection and Metallographic Cooling Rates: Initial Results on Type 1A and 2A Mesosiderites

NASA Technical Reports Server (NTRS)

Baecker, B.; Cohen, B. A.; Rubin, A. E.; Frasl, B.; Corrigan, C. M.

2017-01-01

We initiated a comprehensive study on selected clasts and metal of mesosiderites using SEM, electron microprobe and the complete suite of noble gases. Here we report initial results on the petrography of selected clasts and metallographic cooling rates using the central Ni method used in sev-eral publications. We focus on the approach of selecting grains in least recrystallized mesosiderites. Hence, especially (lithic) clasts in type 1A, 1B, 2A and 2B are the first choice. They provide highest primitive-ness and least annealing/metamorphism. All grains selected should be in close proximity to each other. Lithic clasts in mesosiderites are of high interest be-cause of their igneous texture and similarity to eucrites and howardite petrography. We find pyrox-enes (px) and plagioclase (plag) attached to each other which implies a common formation history. It will be interesting to see differences and similarities in their noble gas inventory (CRE ages, trapped components and closure temperature). In addition, we will investi-gate variations of the lithic clasts toward similar grains in the thick sections which are not igneous. Plag grains are the best bases for noble gas measurements con-cerning He to Ar and Ar-Ar dating since it delivers im-portant target elements. We focus on plag grains in close contact to olivine (olv) / px grains to assess weth-er both grains show noble gas patterns being similar or different. Phosphate grains are suitable for Kr and Xe measurements since they yield REE abundances (tar-get elements).

Detection of Noble Gas Radionuclides from an Underground Nuclear Explosion During a CTBT On-Site Inspection

NASA Astrophysics Data System (ADS)

Carrigan, Charles R.; Sun, Yunwei

2014-03-01

The development of a technically sound approach to detecting the subsurface release of noble gas radionuclides is a critical component of the on-site inspection (OSI) protocol under the Comprehensive Nuclear Test Ban Treaty. In this context, we are investigating a variety of technical challenges that have a significant bearing on policy development and technical guidance regarding the detection of noble gases and the creation of a technically justifiable OSI concept of operation. The work focuses on optimizing the ability to capture radioactive noble gases subject to the constraints of possible OSI scenarios. This focus results from recognizing the difficulty of detecting gas releases in geologic environments—a lesson we learned previously from the non-proliferation experiment (NPE). Most of our evaluations of a sampling or transport issue necessarily involve computer simulations. This is partly due to the lack of OSI-relevant field data, such as that provided by the NPE, and partly a result of the ability of computer-based models to test a range of geologic and atmospheric scenarios far beyond what could ever be studied by field experiments, making this approach very highly cost effective. We review some highlights of the transport and sampling issues we have investigated and complete the discussion of these issues with a description of a preliminary design for subsurface sampling that addresses some of the sampling challenges discussed here.

Chemical composition measurements of the atmosphere of Jupiter with the Galileo Probe mass spectrometer

NASA Technical Reports Server (NTRS)

Niemann, H. B.; Atreya, S. K.; Carignan, G. R.; Donahue, T. M.; Haberman, J. A.; Harpold, D. N.; Hartle, R. E.; Hunten, D. M.; Kasprzak, W. T.; Mahaffy, P. R.;

Chemical composition measurements of the atmosphere of Jupiter with the Galileo Probe mass spectrometer.

PubMed

Niemann, H B; Atreya, S K; Carignan, G R; Donahue, T M; Haberman, J A; Harpold, D N; Hartle, R E; Hunten, D M; Kasprzak, W T; Mahaffy, P R; Owen, T C; Spencer, N W

1998-01-01

The Galileo Probe entered the atmosphere of Jupiter on December 7, 1995. Measurements of the chemical and isotopic composition of the Jovian atmosphere were obtained by the mass spectrometer during the descent over the 0.5 to 21 bar pressure region over a time period of approximately 1 hour. The sampling was either of atmospheric gases directly introduced into the ion source of the mass spectrometer through capillary leaks or of gas, which had been chemically processed to enhance the sensitivity of the measurement to trace species or noble gases. The analysis of this data set continues to be refined based on supporting laboratory studies on an engineering unit. The mixing ratios of the major constituents of the atmosphere hydrogen and helium have been determined as well as mixing ratios or upper limits for several less abundant species including: methane, water, ammonia, ethane, ethylene, propane, hydrogen sulfide, neon, argon, krypton, and xenon. Analysis also suggests the presence of trace levels of other 3 and 4 carbon hydrocarbons, or carbon and nitrogen containing species, phosphine, hydrogen chloride, and of benzene. The data set also allows upper limits to be set for many species of interest which were not detected. Isotope ratios were measured for 3He/4He, D/H, 13C/12C, 20Ne/22Ne, 38Ar/36Ar and for isotopes of both Kr and Xe.

Chemical composition measurements of the atmosphere of jupiter with the galileo probe mass spectrometer

NASA Astrophysics Data System (ADS)

Niemann, H. B.; Atreya, S. K.; Carignan, G. R.; Donahue, T. M.; Haberman, J. A.; Harpold, D. N.; Hartle, R. E.; Hunten, D. M.; Kasprzak, W. T.; Mahaffy, P. R.; Owen, T. C.; Spencer, N. W.

The Galileo Probe entered the atmosphere of Jupiter on December 7, 1995. Measurements of the chemical and isotopic composition of the Jovian atmosphere were obtained by the mass spectrometer during the descent over the 0.5 to 21 bar pressure region over a time period of approximately 1 hour. The sampling was either of atmospheric gases directly introduced into the ion source of the mass spectrometer through capillary leaks or of gas, which had been chemically processed to enhance the sensitivity of the measurement to trace species or noble gases. The analysis of this data set continues to be refined based on supporting laboratory studies on an engineering unit. The mixing ratios of the major constituents of the atmosphere hydrogen and helium have been determined as well as mixing ratios or upper limits for several less abundant species including: methane, water, ammonia, ethane, ethylene, propane, hydrogen sulfide, neon, argon, krypton, and xenon. Analysis also suggests the presence of trace levels of other 3 and 4 carbon hydrocarbons, or carbon and nitrogen containing species, phosphine, hydrogen chloride, and of benzene. The data set also allows upper limits to be set for many species of interest which were not detected. Isotope ratios were measured for ^3He/^4He, D/H, ^13C/^12C, ^20Ne/^22Ne, ^38Ar/^36Ar and for isotopes of both Kr and Xe.

Characterizing Uranus with an Ice giant Planetary Origins Probe (Ice-POP)

NASA Technical Reports Server (NTRS)

Marley, Mark S.; Fortney, Jonathan; Nettelmann, Nadine; Zahnle, Kevin J.

2013-01-01

detected in Neptune but not in Uranus. A measurement of the abundance of either would constrain the source mechanisms for these molecules (exogenic or internal). A major surprise from the Galileo Entry Probe was that the heavier noble gases Ar, Kr, and Xe are enhanced in Jupiter's atmosphere at a level comparable to what was seen for the chemically active volatiles N, C, and S. It had been generally expected that Ar, Kr, and Xe would be present in solar abundances, as all were expected to accrete with hydrogen during the gravitational capture of nebular gases. Enhanced abundances of Ar, Kr, and Xe is equivalent to saying that these noble gases have been separated from hydrogen. There are several mechanisms that could accomplish this but these hypotheses require further testing. Measurement of noble gas abundances in an ice giant would constrain the planetary formation and nebular mechanisms responsible for this enhancement. Standard three-layer models of Uranus find that the outer, predominantly H/He layer of Uranus does not reach pressures high enough (approximately 1 Mbar) for H2 to transition to liquid metallic hydrogen. However, valid models can also be constructed with a smaller intermediate water-rich layer, with hydrogen then reaching the metallic hydrogen phase. If this occurs, He should phase separate from the hydrogen and ``rain out," taking along a substantial abundance of Ne, as suggested for Jupiter (and likely also for Saturn). Hence He and Ne depletions could be probes of the planet's structure in the much deeper interior. A determination of Uranus' atmospheric abundances, particularly of the noble gasses, is thus critical to understanding the formation of Uranus, and giant planets in general. These measurements can only be performed with an entry probe. The second key measurement would be a temperature-pressure sounding to provide ground truth for remote measurements of atmospheric temperature and composition and to constrain the internal heat flow. This

Noble Gas Analysis for Mars Robotic Missions: Evaluating K-Ar Age Dating for Mars Rock Analogs and Martian Shergottites

NASA Technical Reports Server (NTRS)

Park, J.; Ming, D. W.; Garrison, D. H.; Jones, J. H.; Bogard, D. D.; Nagao, K.

2009-01-01

The purpose of this noble gas investigation was to evaluate the possibility of measuring noble gases in martian rocks and air by future robotic missions such as the Mars Science Laboratory (MSL). The MSL mission has, as part of its payload, the Sample Analysis at Mars (SAM) instrument, which consists of a pyrolysis oven integrated with a GCMS. The MSL SAM instrument has the capability to measure noble gas compositions of martian rocks and atmosphere. Here we suggest the possibility of K-Ar age dating based on noble gas release of martian rocks by conducting laboratory simulation experiments on terrestrial basalts and martian meteorites. We provide requirements for the SAM instrument to obtain adequate noble gas abundances and compositions within the current SAM instrumental operating conditions, especially, a power limit that prevents heating the furnace above approx.1100 C. In addition, Martian meteorite analyses from NASA-JSC will be used as ground truth to evaluate the feasibility of robotic experiments to constrain the ages of martian surface rocks.

Thomas Mann's Tonio Kröger: a study of the protagonist's emergence from the schizoid to the depressive position.

PubMed

Zlotnick-Woldenberg, C

2000-01-01

The protagonist of Thomas Mann's novella Tonio Kröger is examined in terms of object-relational theory. This approach is briefly compared with the interpretation that might be offered by structural theorists. Kröger, the son of an authoritarian and prototypical Germanic father and an artistic and sensuous mother from the south, is tormented by what he sees as his dual heritage. Unable to accept that he can be both an artist and a respectable member of bourgeois society, he employs splitting as a primary defense mechanism both intrapsychically and interpersonally, projecting these opposing ideologies onto others including Hans, Inge, and Lisabetta. Alternately idealizing and demonizing these characters, projections of his internal conflict, he is unable to achieve an integrated sense of himself or others, functioning primarily in the schizoid position. His emergence from the schizoid into the more mature depressive position, having been foreshadowed in a series of dream sequences, occurs at the end of the work when he comes to accept the view that artistic impulses and bourgeois discipline are not incompatible.

Field Continuous Measurement of Dissolved Gases with a CF-MIMS: Applications to the Physics and Biogeochemistry of Groundwater Flow.

PubMed

Chatton, Eliot; Labasque, Thierry; de La Bernardie, Jérôme; Guihéneuf, Nicolas; Bour, Olivier; Aquilina, Luc

2017-01-17

In the perspective of a temporal and spatial exploration of aquatic environments (surface and groundwater), we developed a technique for field continuous measurements of dissolved gases with a precision better than 1% for N 2 , O 2 , CO 2 , He, Ar, 2% for Kr, 8% for Xe, and 3% for CH 4 , N 2 O and Ne. With a large resolution (from 1 × 10 -9 to 1 × 10 -2 ccSTP/g) and a capability of high frequency analysis (1 measure every 2 s), the CF-MIMS (Continuous Flow Membrane Inlet Mass Spectrometer) is an innovative tool allowing the investigation of a large panel of hydrological and biogeochemical processes in aquatic systems. Based on the available MIMS technology, this study introduces the development of the CF-MIMS (conception for field experiments, membrane choices, ionization) and an original calibration procedure allowing the quantification of mass spectral overlaps and temperature effects on membrane permeability. This study also presents two field applications of the CF-MIMS involving the well-logging of dissolved gases and the implementation of groundwater tracer tests with dissolved 4 He. The results demonstrate the analytical capabilities of the CF-MIMS in the field. Therefore, the CF-MIMS is a valuable tool for the field characterization of biogeochemical reactivity, aquifer transport properties, groundwater recharge, groundwater residence time and aquifer-river exchanges from few hours to several weeks experiments.

PALOMA : an isotope analyzer using static mass spectrometry, coupled with cryogenic and chemical trapping, for the MSL mission to Mars

NASA Astrophysics Data System (ADS)

Chassefiere, E.; Jambon, A.; Berthelier, J.-J.; Goulpeau, G.; Leblanc, F.; Montmessin, F.; Sarda, P.; Agrinier, P.; Fouchet, T.; Waite, H.

The technique of GCMS analysis has to be completed by static mass spectrometry for precise in-situ measurements of the isotopic composition of planetary atmospheres (noble gases, stable isotopes), and volatile outgassed products from solid sample pyrolysis. Static mass spectrometry, coupled with gas separation by cryo-separation and gettering, is commonly used in the laboratory to study volatiles extracted from terrestrial and meteoritic samples. Such an instrument (PALOMA) is presently developed in our laboratories, and it will be coupled with a Pyr-GCMS analyzer (MACE), built by a US consortium of science laboratories and industrials (University of Michigan, Southwest Research Institute, JPL, Ball Aerospace). The MACE/PALOMA experiment will be proposed on the NASA Mars Science Laboratory mission, planned to be launched in 2009. The scientific objectives of PALOMA, coupled with MACE, may be listed as follows : (i) search for isotopic signatures of past life in atmosphere, rock, dust and ice samples, with emphasis on carbon, nitrogen and hydrogen; (ii) accurately measure isotopic composition of atmospheric noble gases, and stable isotopes, in order to better constrain past escape, surface interaction, outgassing history and climate evolution; (iii) precisely measure diurnal/ seasonal variations of isotopic ratios of H2O, CO2, and N2, for improving our understanding of present and past climate, and of the role of water cycle. Main measurement objectives are : (i) C, H, O, N isotopic composition in both organic evolved samples (provided by MACE pyrolysis system) and atmosphere with high accuracy (a few per mil at 1-s level); (ii) noble gas (He, Ne, Ar, Kr, Xe) and stable (C, H, O, N) isotope composition in atmosphere with high accuracy (a few per mil at 1-s level); (iii) molecular and isotopic composition of inorganic evolved samples (salts, hydrates, nitrates, {ldots}), including ices; (iv) diurnal and seasonal monitoring of D/H in water vapor, and water ice.

Postcollision interaction in noble gas clusters: observation of differences in surface and bulk line shapes.

PubMed

Lindblad, A; Fink, R F; Bergersen, H; Lundwall, M; Rander, T; Feifel, R; Ohrwall, G; Tchaplyguine, M; Hergenhahn, U; Svensson, S; Björneholm, O

2005-12-01

The surface and bulk components of the x-ray photoelectron spectra of free noble gas clusters are shown to display differences in the influence of postcollision interaction between the photoelectron and the Auger electron on the spectral line shape; the bulk component is observed to be less affected than the surface and atomic parts of the spectra. A model for postcollision interaction in nonmetallic solids and clusters is also provided which takes the polarization screening into account. Core-level photoelectron spectra of Ar, Kr, and Xe have been recorded to verify the dependence of the postcollision interaction effect on the polarizability of the sample.

Theory of warm ionized gases: equation of state and kinetic Schottky anomaly.

PubMed

Capolupo, A; Giampaolo, S M; Illuminati, F

2013-10-01

Based on accurate Lennard-Jones-type interaction potentials, we derive a closed set of state equations for the description of warm atomic gases in the presence of ionization processes. The specific heat is predicted to exhibit peaks in correspondence to single and multiple ionizations. Such kinetic analog in atomic gases of the Schottky anomaly in solids is enhanced at intermediate and low atomic densities. The case of adiabatic compression of noble gases is analyzed in detail and the implications on sonoluminescence are discussed. In particular, the predicted plasma electron density in a sonoluminescent bubble turns out to be in good agreement with the value measured in recent experiments.

Physiological response of rats to delivery of helium and xenon: implications for hyperpolarized noble gas imaging

NASA Technical Reports Server (NTRS)

Ramirez, M. P.; Sigaloff, K. C.; Kubatina, L. V.; Donahue, M. A.; Venkatesh, A. K.; Albert, M. S.; ALbert, M. S. (Principal Investigator)

2000-01-01

The physiological effects of various hyperpolarized helium and xenon MRI-compatible breathing protocols were investigated in 17 Sprague-Dawley rats, by continuous monitoring of blood oxygen saturation, heart rate, EKG, temperature and endotracheal pressure. The protocols included alternating breaths of pure noble gas and oxygen, continuous breaths of pure noble gas, breath-holds of pure noble gas for varying durations, and helium breath-holds preceded by two helium rinses. Alternate-breath protocols up to 128 breaths caused a decrease in oxygen saturation level of less than 5% for either helium or xenon, whereas 16 continuous-breaths caused a 31.5% +/- 2.3% decrease in oxygen saturation for helium and a 30.7% +/- 1. 3% decrease for xenon. Breath-hold protocols up to 25 s did not cause the oxygen saturation to fall below 90% for either of the noble gases. Oxygen saturation values below 90% are considered pathological. At 30 s of breath-hold, the blood oxygen saturation dropped precipitously to 82% +/- 0.6% for helium, and to 76.5% +/- 7. 4% for xenon. Breath-holds longer than 10 s preceded by pre-rinses caused oxygen saturation to drop below 90%. These findings demonstrate the need for standardized noble gas inhalation procedures that have been carefully tested, and for continuous physiological monitoring to ensure the safety of the subject. We find short breath-hold and alternate-breath protocols to be safe procedures for use in hyperpolarized noble gas MRI experiments. Copyright 2000 John Wiley & Sons, Ltd.

ns2np4 (n = 4, 5) lone pair triplets whirling in M*F2E3 (M* = Kr, Xe): Stereochemistry and ab initio analyses

NASA Astrophysics Data System (ADS)

Galy, Jean; Matar, Samir F.

2017-02-01

The stereochemistry of ns2np4 (n = 4, 5) lone pair LP characterizing noble gas Kr and Xe (labeled M*) in M*F2 difluorides is examined within coherent crystal chemistry and ab initio visualizations. M*2+ in such oxidation state brings three lone pairs (E) and difluorides are formulated M*F2E3. The analyses use electron localization function (ELF) obtained within density functional theory calculations showing the development of the LP triplets whirling {E3} quantified in the relevant chemical systems. Detailed ELF data analyses allowed showing that in α KrF2E3 and isostructural XeF2E3 difluorides the three E electronic clouds merge or hybridize into a torus and adopt a perfect gyration circle with an elliptical section, while in β KrF2 the network architecture deforms the whole torus into an ellipsoid shape. Original precise metrics are provided for the torus in the different compounds under study. In KrF2 the geometric changes upon β → α phase transition is schematized and mechanisms for the transformation with temperature or pressure are proposed. The results are further highlighted by electronic band structure calculations which show similar features of equal band gaps of 3 eV in both α and β KrF2 and a reorganization of frontier orbitals due to the different orientations of the F-Kr-F linear molecule in the two tetragonal structures.

Sequential two-photon double ionization of noble gases by circularly polarized XUV radiation

NASA Astrophysics Data System (ADS)

Gryzlova, E. V.; Grum-Grzhimailo, A. N.; Kuzmina, E. I.; Strakhova, S. I.

2014-10-01

Photoelectron angular distributions (PADs) and angular correlations between two emitted electrons in sequential two-photon double ionization (2PDI) of atoms by circularly polarized radiation are studied theoretically. In particular, the sequential 2PDI of the valence n{{p}6} shell in noble gas atoms (neon, argon, krypton) is analyzed, accounting for the first-order corrections to the dipole approximation. Due to different selection rules in ionization transitions, the circular polarization of photons causes some new features of the cross sections, PADs and angular correlation functions in comparison with the case of linearly polarized photons.

Rare gases systematics and mantle structure

NASA Technical Reports Server (NTRS)

Allegre, C. J.; Staudacher, T.

1994-01-01

The following points are emphasized: one of the most important ones is certainly the first set of experimental data on the solubility of noble gases in metal phases at intermediate pressures, since the core was certainly not formed at ultra high pressures, as emphasized by Ahrens and confirmed by trace elements systematics Wanke. The experimental data clearly show that the core can not be a major reservoir for terrestrial rare gases; the second point is a more elaborate reconsideration of the (40)K-(40)Ar budget of the Earth. This shows that (40)Ar contained in continental crust plus upper mantle plus atmosphere is at maximum half of the (40)Ar inventory of the whole earth. This implies the existence of a two layered mantle; the third point is the discovery by the Australian noble gases group of the existence of high (20)Ne/(22)Ne and low (21)Ne/(22)Ne isotopic ratios in Loihi seamount samples. This results which are different to the MORB ratios confirm the idea of a two layered model, but suggest the existence of a primordial solar type Ne reservoir. Several possibilities about the origin of this (20)Ne excess in the mantle will be discussed; The high (40)Ar/(36)Ar, (129)Xe/(130)Xe and (134) Xe/(130)Xe, (136)Xe/(130)Xe are confirmed by new data. The corresponding ratios for the lower mantle will be discussed. (40)Ar/(36)Ar ratios up to 6000 can be accepted and will not modify the general model of the mantle. They confirm the atmosphere chronology, about 85 percent of the atmosphere was formed in the first 50 My and 15 percent later on.

Kinetic Energy and Angular Distributions of He and Ar Atoms Evaporating from Liquid Dodecane.

PubMed

Patel, Enamul-Hasan; Williams, Mark A; Koehler, Sven P K

2017-01-12

We report both kinetic energy and angular distributions for He and Ar atoms evaporating from C 12 H 26 . All results were obtained by performing molecular dynamics simulations of liquid C 12 H 26 with around 10-20 noble gas atoms dissolved in the liquid and by subsequently following the trajectories of the noble gas atoms after evaporation from the liquid. Whereas He evaporates with a kinetic energy distribution of (1.05 ± 0.03) × 2RT (corrected for the geometry used in experiments: (1.08 ± 0.03) × 2RT, experimentally obtained value: (1.14 ± 0.01) × 2RT), Ar displays a kinetic energy distribution that better matches a Maxwell-Boltzmann distribution at the temperature of the liquid ((0.99 ± 0.04) × 2RT). This behavior is also reflected in the angular distributions, which are close to a cosine distribution for Ar but slightly narrower, especially for faster atoms, in the case of He. This behavior of He is most likely due to the weak interaction potential between He and the liquid hydrocarbon.

The Inherent Tracer Fingerprint of Captured CO2

NASA Astrophysics Data System (ADS)

Flude, Stephanie; Gyore, Domokos; Stuart, Finlay; Boyce, Adrian; Haszeldine, Stuart; Chalaturnyk, Rick; Gilfillan, Stuart

2017-04-01

Inherent tracers, the isotopic and trace gas composition of captured CO2 streams, are potentially powerful tracers for use in CCS technology [1,2]. Despite this potential, the inherent tracer fingerprint in captured CO2 streams has yet to be robustly investigated and documented [3]. Here, we will present the first high quality systematic measurements of the carbon and oxygen isotopic and noble gas fingerprints measured in anthropogenic CO2 captured from combustion power stations and fertiliser plants, using amine capture, oxyfuel and gasification processes, and derived from coal, biomass and natural gas feedstocks. We will show that δ13C values are mostly controlled by the feedstock composition, as expected. The majority of the CO2 samples exhibit δ18O values similar to atmospheric O2 although captured CO2 samples from biomass and gas feedstocks at one location in the UK are significantly higher. Our measured noble gas concentrations in captured CO2 are generally as expected [2], typically being two orders of magnitude lower in concentration than in atmospheric air. Relative noble gas elemental abundances are variable and often show an opposite trend to that of a water in contact with the atmosphere. Expected enrichments in radiogenic noble gases (4He and 40Ar) for fossil fuel derived CO2 were not always observed due to dilution with atmospheric noble gases during the CO2 generation and capture process. Many noble gas isotope ratios indicate that isotopic fractionation takes place during the CO2 generation and capture processes, resulting in isotope ratios similar to fractionated air. We conclude that phase changes associated with CO2 transport and sampling may induce noble gas elemental and isotopic fractionation, due to different noble gas solubilities between high (liquid or supercritical) and low (gaseous) density CO2. Data from the Australian CO2CRC Otway test site show that δ13C of CO2 will change once injected into the storage reservoir, but that this

Field continuous measurement of dissolved gases with a CF-MIMS: Applications to the physics and biogeochemistry of groundwater flow

NASA Astrophysics Data System (ADS)

Chatton, Eliot; Labasque, Thierry; de La Bernardie, Jérôme; Guihéneuf, Nicolas; Bour, Olivier; Aquilina, Luc

2017-04-01

In the perspective of a temporal and spatial exploration of aquatic environments (surface and ground water), we developed a technique for precise field continuous measurements of dissolved gases (N2, O2, CO2, CH4, N2O, H2, He, Ne, Ar, Kr, Xe). With a large resolution (from 1×10-9 to 1×10-2 ccSTP/g) and a capability of high frequency analysis (1 measure every 2 seconds), the CF-MIMS (Continuous Flow Membrane Inlet Mass Spectrometer) is an innovative tool allowing the investigation of a large panel of hydrological and biogeochemical processes in aquatic systems. Based on the available MIMS technology, this study introduces the development of the CF-MIMS (conception for field experiments, membrane choices, ionisation) and an original calibration procedure allowing the quantification of mass spectral overlaps and temperature effects on membrane permeability. This study also presents two field applications of the CF-MIMS (Chatton et al, 2016) involving the well-logging of dissolved gases and the implementation of groundwater tracer tests with dissolved 4He. The results demonstrate the analytical capabilities of the CF-MIMS in the field. Therefore, the CF-MIMS is a valuable tool for the field characterisation of biogeochemical reactivity, aquifer transport properties, groundwater recharge, groundwater residence time and aquifer-river exchanges from few hours to several weeks experiments. Eliot Chatton, Thierry Labasque, Jérôme de La Bernardie, Nicolas Guihéneuf, Olivier Bour and Luc Aquilina; Field Continuous Measurement of Dissolved Gases with a CF-MIMS: Applications to the Physics and Biogeochemistry of Groundwater Flow; Environmental Science & Technology, in press, 2016.

Gaseous 83mKr generator for KATRIN

NASA Astrophysics Data System (ADS)

Sentkerestiová, J.; Dragoun, O.; Lebeda, O.; Ryšavý, M.; Sturm, M.; Vénos, D.

2018-04-01

Monoenergetic conversion electrons from the 83mKrKr isomeric state have been proven to be useful in the calibration of several tritium neutrino mass and dark matter experiments. In this paper the design and characteristics of the gaseous 83mKrKr generator, including the 83Rb/83mKrKr source behavior in tritium, for the KATRIN experiment are presented. Using Si(Li) and silicon drift detectors (SDD) detectors, the half-life of the 83mKrKr isomeric state was measured to be 1.8620 ± 0.0019 h.

Seasonal and geothermal production variations in concentrations of He and CO2 in soil gases, Roosevelt Hot Springs Known Geothermal Resource Area, Utah, U.S.A.

USGS Publications Warehouse

Hinkle, M.E.

1991-01-01

To increase understanding of natural variations in soil gas concentrations, CO2, He, O2 and N2 were measured in soil gases collected regularly for several months from four sites at the Roosevelt Hot Springs Known Geothermal Resource Area, Utah. Soil temperature, air temperature, per cent relative humidity, barometric pressure and amounts of rain and snowfall were also monitored to determine the effect of meteorological parameters on concentrations of the measured gases. Considerable seasonal variation existed in concentrations of CO2 and He. The parameters that most affected the soil-gas concentrations were soil and air temperatures. Moisture from rain and snow probably affected the soil-gas concentrations also. However, annual variations in meteorological parameters did not appear to affect measurements of anomalous concentrations in samples collected within a time period of a few days. Production from some of the geothermal wells probably affected the soil-gas concentrations. ?? 1990.

Spectral shapes of rovibrational lines of CO broadened by He, Ar, Kr and SF6: A test case of the Hartmann-Tran profile

NASA Astrophysics Data System (ADS)

Ngo, N. H.; Lin, H.; Hodges, J. T.; Tran, H.

2017-12-01

High signal-to-noise ratio spectra of the (3-0) band P(1) and P(17) lines of CO broadened by He, Ar, Kr and SF6 were measured with a frequency-stabilized cavity ring-down spectroscopy system. For each collision-partner and both lines, multiple spectra were measured over pressures spanning nearly three decades up to 130 kPa. These data were analyzed with a multispectrum fitting procedure. Line shapes were modeled using the Hartmann-Tran (HT) profile with first-order line mixing as well as several other simplified profiles. The results show that for all considered collision partners (with the exception of SF6), the HT profile captures the measured line shapes with maximum absolute residuals that are within 0.1% of the peak absorption. In the case of SF6, which is the heaviest perturber investigated here, the maximum residuals for the HT profile are twice as large as for the other collision partners.

Energy levels and radiative rates for transitions in B-like to F-like Kr ions (Kr XXXII XXVIII)

NASA Astrophysics Data System (ADS)

Aggarwal, K. M.; Keenan, F. P.; Lawson, K. D.

2008-05-01

Energy levels, radiative rates, oscillator strengths, line strengths, and lifetimes have been calculated for transitions in B-like to F-like Kr ions, Kr XXXIII-XXVIII. For the calculations, the fully relativistic GRASP code has been adopted, and results are reported for all electric dipole (E1), electric quadrupole (E2), magnetic dipole (M1), and magnetic quadrupole (M2) transitions among the lowest 125, 236, 272, 226, and 113 levels of Kr XXXII, Kr XXXI, Kr XXX, Kr XXIX, and Kr XXVIII, respectively, belonging to the n ⩽ 3 configurations. Comparisons are made with earlier available theoretical and experimental results, and some discrepancies have been noted and explained.

New Tracers of Gas Migration in the Continental Crust

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kurz, Mark D.

2015-11-01

Noble gases are exceptional tracers in continental settings due to the remarkable isotopic variability between the mantle, crust, and atmosphere, and because they are inert. Due to systematic variability in physical properties, such as diffusion, solubility, and production rates, the combination of helium, neon, and argon provides unique but under-utilized indices of gas migration. Existing noble gas data sets are dominated by measurements of gas and fluid phases from gas wells, ground waters and hot springs. There are very few noble gas measurements from the solid continental crust itself, which means that this important reservoir is poorly characterized. The centralmore » goal of this project was to enhance understanding of gas distribution and migration in the continental crust using new measurements of noble gases in whole rocks and minerals from existing continental drill cores, with an emphasis on helium, neon, argon. We carried out whole-rock and mineral-separate noble gas measurements on Precambrian basement samples from the Texas Panhandle. The Texas Panhandle gas field is the southern limb of the giant Hugoton-Panhandle oil and gas field; it has high helium contents (up to ~ 2 %) and 3He/4He of 0.21 (± 0.03) Ra. Because the total amount of helium in the Panhandle gas field is relatively well known, crustal isotopic data and mass balance calculations can be used to constrain the ultimate source rocks, and hence the helium migration paths. The new 3He/4He data range from 0.03 to 0.11 Ra (total), all of which are lower than the gas field values. There is internal isotopic heterogeneity in helium, neon, and argon, within all the samples; crushing extractions yield less radiogenic values than melting, demonstrating that fluid inclusions preserve less radiogenic gases. The new data suggest that the Precambrian basement has lost significant amounts of helium, and shows the importance of measuring helium with neon and argon. The 4He/40Ar values are

Cross-Section Measurements of the Kr86(γ,n) Reaction to Probe the s-Process Branching at Kr85

NASA Astrophysics Data System (ADS)

Raut, R.; Tonchev, A. P.; Rusev, G.; Tornow, W.; Iliadis, C.; Lugaro, M.; Buntain, J.; Goriely, S.; Kelley, J. H.; Schwengner, R.; Banu, A.; Tsoneva, N.

2013-09-01

We have carried out photodisintegration cross-section measurements on Kr86 using monoenergetic photon beams ranging from the neutron separation energy, Sn=9.86MeV, to 13 MeV. We combine our experimental Kr86(γ,n)Kr85 cross section with results from our recent Kr86(γ,γ') measurement below the neutron separation energy to obtain the complete nuclear dipole response of Kr86. The new experimental information is used to predict the neutron capture cross section of Kr85, an important branching point nucleus on the abundance flow path during s-process nucleosynthesis. Our new and more precise Kr85(n,γ)Kr86 cross section allows us to produce more precise predictions of the Kr86 abundance from s-process models. In particular, we find that the models of the s process in asymptotic giant branch stars of mass <1.5M⊙, where the C13 neutron source burns convectively rather than radiatively, represent a possible solution for the highest Kr86∶Kr82 ratios observed in meteoritic stardust SiC grains.

Cross-section measurements of the 86Kr(γ,n) reaction to probe the s-process branching at 85Kr.

PubMed

Raut, R; Tonchev, A P; Rusev, G; Tornow, W; Iliadis, C; Lugaro, M; Buntain, J; Goriely, S; Kelley, J H; Schwengner, R; Banu, A; Tsoneva, N

2013-09-13

We have carried out photodisintegration cross-section measurements on 86Kr using monoenergetic photon beams ranging from the neutron separation energy, S(n) = 9.86  MeV, to 13 MeV. We combine our experimental 86Kr(γ,n)85Kr cross section with results from our recent 86Kr(γ,γ') measurement below the neutron separation energy to obtain the complete nuclear dipole response of 86Kr. The new experimental information is used to predict the neutron capture cross section of 85Kr, an important branching point nucleus on the abundance flow path during s-process nucleosynthesis. Our new and more precise 85Kr(n,γ)86Kr cross section allows us to produce more precise predictions of the 86Kr abundance from s-process models. In particular, we find that the models of the s process in asymptotic giant branch stars of mass <1.5M⊙, where the 13C neutron source burns convectively rather than radiatively, represent a possible solution for the highest 86Kr:82Kr ratios observed in meteoritic stardust SiC grains.

A comparative study on the frequency effects of the electrical characteristics of the pulsed dielectric barrier discharge in He/O{sub 2} and in Ar/O{sub 2} at atmospheric pressure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pan, Guangsheng; Tan, Zhenyu, E-mail: tzy@sdu.edu.cn; Pan, Jie

In this work, a comparative study on the frequency effects of the electrical characteristics of the pulsed dielectric barrier discharges in He/O{sub 2} and in Ar/O{sub 2} at atmospheric pressure has been performed by means of the numerical simulation based on a 1-D fluid model at frequencies below 100 kHz. The frequency dependences of the characteristic quantities of the discharges in the two gases have been systematically calculated and analyzed under the oxygen concentrations below 2%. The characteristic quantities include the discharge current density, the averaged electron density, the electric field, and the averaged electron temperature. Especially, the frequency effects onmore » the averaged particle densities of the reactive species have also been calculated. This work gives the following significant results. For the two gases, there are two bipolar discharges in one period of applied voltage pulse under the considered frequency range and oxygen concentrations, as occurred in the pure noble gases. The frequency affects the two discharges in He/O{sub 2}, but in Ar/O{sub 2}, it induces a strong effect only on the first discharge. For the first discharge in each gas, there is a characteristic frequency at which the characteristic quantities reach their respective minimum, and this frequency appears earlier for Ar/O{sub 2}. For the second discharge in Ar/O{sub 2}, the averaged electron density presents a slight variation with the frequency. In addition, the discharge in Ar/O{sub 2} is strong and the averaged electron temperature is low, compared to those in He/O{sub 2.} The total averaged particle density of the reactive species in Ar/O{sub 2} is larger than those in He/O{sub 2} by about one order of magnitude.« less

Optimizing detection of noble gas emission at a former UNE site: sample strategy, collection, and analysis

NASA Astrophysics Data System (ADS)

Kirkham, R.; Olsen, K.; Hayes, J. C.; Emer, D. F.

2013-12-01

Underground nuclear tests may be first detected by seismic or air samplers operated by the CTBTO (Comprehensive Nuclear-Test-Ban Treaty Organization). After initial detection of a suspicious event, member nations may call for an On-Site Inspection (OSI) that in part, will sample for localized releases of radioactive noble gases and particles. Although much of the commercially available equipment and methods used for surface and subsurface environmental sampling of gases can be used for an OSI scenario, on-site sampling conditions, required sampling volumes and establishment of background concentrations of noble gases require development of specialized methodologies. To facilitate development of sampling equipment and methodologies that address OSI sampling volume and detection objectives, and to collect information required for model development, a field test site was created at a former underground nuclear explosion site located in welded volcanic tuff. A mixture of SF-6, Xe127 and Ar37 was metered into 4400 m3 of air as it was injected into the top region of the UNE cavity. These tracers were expected to move towards the surface primarily in response to barometric pumping or through delayed cavity pressurization (accelerated transport to minimize source decay time). Sampling approaches compared during the field exercise included sampling at the soil surface, inside surface fractures, and at soil vapor extraction points at depths down to 2 m. Effectiveness of various sampling approaches and the results of tracer gas measurements will be presented.

Terrestrial nitrogen and noble gases in lunar soils.

PubMed

Ozima, M; Seki, K; Terada, N; Miura, Y N; Podosek, F A; Shinagawa, H

2005-08-04

The nitrogen in lunar soils is correlated to the surface and therefore clearly implanted from outside. The straightforward interpretation is that the nitrogen is implanted by the solar wind, but this explanation has difficulties accounting for both the abundance of nitrogen and a variation of the order of 30 per cent in the 15N/14N ratio. Here we propose that most of the nitrogen and some of the other volatile elements in lunar soils may actually have come from the Earth's atmosphere rather than the solar wind. We infer that this hypothesis is quantitatively reasonable if the escape of atmospheric gases, and implantation into lunar soil grains, occurred at a time when the Earth had essentially no geomagnetic field. Thus, evidence preserved in lunar soils might be useful in constraining when the geomagnetic field first appeared. This hypothesis could be tested by examination of lunar farside soils, which should lack the terrestrial component.

Hydrocarbon-Rich Groundwater above Shale-Gas Formations: A Karoo Basin Case Study.

PubMed

Eymold, William K; Swana, Kelley; Moore, Myles T; Whyte, Colin J; Harkness, Jennifer S; Talma, Siep; Murray, Ricky; Moortgat, Joachim B; Miller, Jodie; Vengosh, Avner; Darrah, Thomas H

2018-03-01

Horizontal drilling and hydraulic fracturing have enhanced unconventional hydrocarbon recovery but raised environmental concerns related to water quality. Because most basins targeted for shale-gas development in the USA have histories of both active and legacy petroleum extraction, confusion about the hydrogeological context of naturally occurring methane in shallow aquifers overlying shales remains. The Karoo Basin, located in South Africa, provides a near-pristine setting to evaluate these processes, without a history of conventional or unconventional energy extraction. We conducted a comprehensive pre-industrial evaluation of water quality and gas geochemistry in 22 groundwater samples across the Karoo Basin, including dissolved ions, water isotopes, hydrocarbon molecular and isotopic composition, and noble gases. Methane-rich samples were associated with high-salinity, NaCl-type groundwater and elevated levels of ethane, 4 He, and other noble gases produced by radioactive decay. This endmember displayed less negative δ 13 C-CH 4 and evidence of mixing between thermogenic natural gases and hydrogenotrophic methane. Atmospheric noble gases in the methane-rich samples record a history of fractionation during gas-phase migration from source rocks to shallow aquifers. Conversely, methane-poor samples have a paucity of ethane and 4 He, near saturation levels of atmospheric noble gases, and more negative δ 13 C-CH 4 ; methane in these samples is biogenic and produced by a mixture of hydrogenotrophic and acetoclastic sources. These geochemical observations are consistent with other basins targeted for unconventional energy extraction in the USA and contribute to a growing data base of naturally occurring methane in shallow aquifers globally, which provide a framework for evaluating environmental concerns related to unconventional energy development (e.g., stray gas). © 2018, National Ground Water Association.

Post-Hartree-Fock studies of the He/Mg(0001) interaction: Anti-corrugation, screening, and pairwise additivity

NASA Astrophysics Data System (ADS)

de Lara-Castells, María Pilar; Fernández-Perea, Ricardo; Madzharova, Fani; Voloshina, Elena

2016-06-01

The adsorption of noble gases on metallic surfaces represents a paradigmatic case of van-der-Waals (vdW) interaction due to the role of screening effects on the corrugation of the interaction potential [J. L. F. Da Silva et al., Phys. Rev. Lett. 90, 066104 (2003)]. The extremely small adsorption energy of He atoms on the Mg(0001) surface (below 3 meV) and the delocalized nature and mobility of the surface electrons make the He/Mg(0001) system particularly challenging, even for state-of-the-art vdW-corrected density functional-based (vdW-DFT) approaches [M. P. de Lara-Castells et al., J. Chem. Phys. 143, 194701 (2015)]. In this work, we meet this challenge by applying two different procedures. First, the dispersion-corrected second-order Möller-Plesset perturbation theory (MP2C) approach is adopted, using bare metal clusters of increasing size. Second, the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)] is applied at coupled cluster singles and doubles and perturbative triples level, using embedded cluster models of the metal surface. Both approaches provide clear evidences of the anti-corrugation of the interaction potential: the He atom prefers on-top sites, instead of the expected hollow sites. This is interpreted as a signature of the screening of the He atom by the metal for the on-top configuration. The strong screening in the metal is clearly reflected in the relative contribution of successively deeper surface layers to the main dispersion contribution. Aimed to assist future dynamical simulations, a pairwise potential model for the He/surface interaction as a sum of effective He-Mg pair potentials is also presented, as an improvement of the approximation using isolated He-Mg pairs.

The helium flux from the continents and ubiquity of low-3He/4He recycled crust and lithosphere

NASA Astrophysics Data System (ADS)

Day, James M. D.; Barry, Peter H.; Hilton, David R.; Burgess, Ray; Pearson, D. Graham; Taylor, Lawrence A.

2015-03-01

geological timescales (>0.1 Ga), and that U and Th contents vary between cratonic lithosphere and non-cratonic lithosphere, calculations yield a 3He flux of 0.25-2.2 atoms/s/cm2 for the continental lithospheric mantle. These estimates differ by a factor of ten from non-cratonic lithospheric mantle and are closer to the observed 3He flux from the continents (<1 atoms/s/cm2). Pyroxenites and eclogites from the continental regions are all characterized by 3He/4He (0.03-5.6 RA) less than the depleted upper mantle, and relatively high U and Th contents. Together with oceanic and continental lithospheric peridotites, these materials represent reservoirs with low time-integrated 3He/(U + Th) in the mantle. Pyroxenites and eclogites are also characterized by higher Fe/Mg, more radiogenic Os-Pb isotope compositions, and more variable δ18O values (∼3‰ to 7‰), compared with peridotitic mantle. These xenoliths are widely interpreted to be the metamorphic/metasomatic equivalents of recycled oceanic crustal protoliths. The low-3He/4He values of these reservoirs and their distinctive compositions make them probable end-members to explain the compositions of some low-3He/4He OIB, and provide an explanation for the low-3He/4He measured in most HIMU lavas. Continental lithospheric mantle and recycled oceanic crust protoliths are not reservoirs for high-3He/4He and so alternative, volumetrically significant, He-rich reservoirs, such as less-degassed (lower?) mantle, are required to explain high-3He/4He signatures measured in some intraplate lavas. Recycling of oceanic crust represents a fundamental process for the generation of radiogenic noble gases in the mantle, and can therefore be used effectively as tracers for volatile recycling.

Understanding Bright 13 keV Kr K-shell X-ray Sources at the NIF

NASA Astrophysics Data System (ADS)

May, M. J.; Colvin, J. D.; Kemp, G. E.; Fournier, K. B.; Scott, H.; Patel, M.; Barrios, Widmann; Widmann, K.

2015-11-01

High x-ray conversion efficiency (CE) K-shell Kr sources are being investigated for High Energy Density experiments. These sources are 4.1 mm in diameter 4.4 mm tall hollow epoxy tubes having a 40 μm thick wall holding either 1.2 or 1.5 atm of Kr gas. The CE of K-shell Kr is dependent upon the peak electron temperature in the radiating plasma. In the NIF experiments, the available energy heats the source to Te = 6-7 keV, well below the temperature of Te ~25 keV needed to optimize the Kr CE. The CE is a steep function of the peak electron temperature. A spatially averaged electron temperature can be estimated from measured He(α) and Ly(α) line ratios. Some disagreement has been observed in the simulated and measured line ratios for some of these K-shell sources. Disagreements have been observed between the simulated and measured line ratios for some of these K-shell sources. To help understand this issue, Kr gas pipes have been shot with 3 ω light at ?750 kJ at ~210, ~140 TW and ~120 TW power levels with 3.7, 5.2 and 6.7 ns pulses, respectively. The power and pulse length scaling of the measured CE and K-shell line ratios and their comparison to simulations will be discussed. This work was performed under the auspic

Noble metal superparticles and methods of preparation thereof

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sun, Yugang; Hu, Yongxing

A method comprises heating an aqueous solution of colloidal silver particles. A soluble noble metal halide salt is added to the aqueous solution which undergoes a redox reaction on a surface of the silver particles to form noble metal/silver halide SPs, noble metal halide/silver halide SPs or noble metal oxide/silver halide SPs on the surface of the silver particles. The heat is maintained for a predetermined time to consume the silver particles and release the noble metal/silver halide SPs, the noble metal halide/silver halide SPs or the noble metal oxide/silver halide SPs into the aqueous solution. The aqueous solution ismore » cooled. The noble metal/silver halide SPs, the noble metal halide/silver halide SPs or noble metal oxide/silver halide SPs are separated from the aqueous solution. The method optionally includes adding a soluble halide salt to the aqueous solution.« less

Cosmogenic He and Ne in chondrules from clastic matrix and a lithic clast of Murchison: No pre-irradiation by the early sun

NASA Astrophysics Data System (ADS)

Riebe, My E. I.; Huber, Liliane; Metzler, Knut; Busemann, Henner; Luginbuehl, Stefanie M.; Meier, Matthias M. M.; Maden, Colin; Wieler, Rainer

2017-09-01

Whether or not some meteorites retain a record of irradiation by a large flux of energetic particles from the early sun in the form of excesses of cosmic-ray produced noble gases in individual crystals or single chondrules is a topic of ongoing debate. Here, we present He and Ne isotopic data for individual chondrules in Murchison, a chondritic regolith breccia of the CM group. We separated 27 chondrules from a clastic matrix portion and 26 chondrules from an adjacent single so-called "primary accretionary rock" (Metzler et al., 1992). All chondrules from the primary rock fragment are expected to share a common irradiation history, whereas chondrules from the clastic matrix were stirred in the regolith independently of each other. All "primary rock chondrules" and 23 of the "matrix chondrules" have very similar concentrations of cosmogenic 3He and 21Ne, corresponding to a cosmic-ray exposure age to galactic cosmic rays (GCR) of ∼1.3-1.9 Ma, in the range of Murchison's meteoroid exposure age determined with cosmogenic radionuclides. Four clastic matrix chondrules contain excesses of cosmogenic 3He and 21Ne, corresponding to nominal 4π exposure ages of ∼4-∼29 Ma, with a Ne isotopic composition as expected for production by GCR. If the fraction of excess cosmogenic gas bearing chondrules in the primary rock and clastic matrix were the same, we would expect this result with a statistical probability of only 0.5 - 2.7%. Therefore, the exposure age distributions for Murchison chondrules in primary rock and clastic matrix are very likely different. Such a difference is expected if the excess cosmogenic gas was acquired by some of the matrix chondrules in the regolith, but not if chondrules were irradiated in the solar nebula by the early sun before they accreted on the Murchison parent body. Therefore, Murchison does not provide evidence for irradiation by a high fluence of energetic particles from the early sun. By inference, this statement likely holds for the

Neutron capture cross sections of Kr

NASA Astrophysics Data System (ADS)

Fiebiger, Stefan; Baramsai, Bayarbadrakh; Couture, Aaron; Krtička, Milan; Mosby, Shea; Reifarth, René; O'Donnell, John; Rusev, Gencho; Ullmann, John; Weigand, Mario; Wolf, Clemens

2018-01-01

Neutron capture and β- -decay are competing branches of the s-process nucleosynthesis path at 85Kr [1], which makes it an important branching point. The knowledge of its neutron capture cross section is therefore essential to constrain stellar models of nucleosynthesis. Despite its importance for different fields, no direct measurement of the cross section of 85Kr in the keV-regime has been performed. The currently reported uncertainties are still in the order of 50% [2, 3]. Neutron capture cross section measurements on a 4% enriched 85Kr gas enclosed in a stainless steel cylinder were performed at Los Alamos National Laboratory (LANL) using the Detector for Advanced Neutron Capture Experiments (DANCE). 85Kr is radioactive isotope with a half life of 10.8 years. As this was a low-enrichment sample, the main contaminants, the stable krypton isotopes 83Kr and 86Kr, were also investigated. The material was highly enriched and contained in pressurized stainless steel spheres.

Constraints on the thermosteric component of Last Interglacial sea level

NASA Astrophysics Data System (ADS)

Shackleton, S. A.; Severinghaus, J. P.; Petrenko, V. V.; Dyonisius, M.; Hmiel, B.

2016-12-01

With global temperatures 1 to 2°C above preindustrial, but sea level exceeding current levels by upwards of 8 meters, the Last Interglacial (LIG) period at 125 ka may provide valuable insight into Earth system constraints under future global warming. The relative contributions of thermal expansion and ice sheet loss to sea level rise over this period are of particular interest in seeking to improve sea level projections in the upcoming decades and beyond. Here we quantify this thermosteric component from a reconstruction of global ocean temperature over the LIG from atmospheric noble gases trapped in glacial ice. With no major sources or sinks outside of the ocean-atmosphere system, the relative changes in the atmospheric content of krypton, xenon, and nitrogen reflect changes in ocean gas storage. This storage is primarily governed by solubility and ocean temperature, making dKr/N2, dXe/N2­, and dXe/Kr unique tracers of globally integrated oceanic heat content. However, processes within the firn can fractionate these gases, and firn effects on these tracers must be removed to derive an ocean temperature. We present high precision measurements of these gas ratios along with isotopes of argon, krypton, and xenon in firn air withdrawn from the snowpack at Summit, Greenland. We use these isotopes to identify sources of fractionation within the firn and quantify their effects on the noble gas tracers, enabling a reconstruction of Last Interglacial ocean temperature.

Rare gases in cyclosilicates and cogenetic minerals

NASA Technical Reports Server (NTRS)

Saito, K.; Alexander, E. C., Jr.; Dragon, J. C.; Zashu, S.

1984-01-01

The cyclosilicate minerals, beryl, tourmaline, and cordierite, typically contain large amounts of He-4 and Ar-40 which are not in situ radiogenic products. In the study of excess rare gases in cyclosilicates, one of the most enigmatic observations is the age effect, a qualitative tendency for geologically older samples to contain more excess He-4 and Ar-40 than younger samples. The present investigation is concerned with measurements regarding the abundance and isotopic composition of all five rare gases in a number of cyclosilicates as well as in their cogenetic minerals. The significance of the obtained data is discussed. The data indicate that cyclosilicates sample the rare gases present in the environment in which they crystallize. This 'sampling' involves major elemental fractionations which are variable but mineral specific. Cyclosilicates can, therefore, be used to probe the isotopic ratios and elemental compositions.

Rare Gases Inserted into Biological Building Blocks: A Theoretical Study of Glycine - Rg Compounds (Rg-Xe, Kr, Ar)

NASA Technical Reports Server (NTRS)

Chaban, Galina M.

2005-01-01

Compounds formed by insertion of rare-gas atoms (Xe, Kr, and Ar) into glycine molecule are investigated using accurate ab initio computational methods. Identification of such insertion compounds may open new frontiers in the field of rare-gas chemistry, such as possible existence of biological molecules that include chemically bound rare gas atoms. The most stable glycine-Rg configuration is found to correspond to insertion of Rg atoms into the 0-H bond of glycine. These NH2CH2COORgH compounds are metastable , but separated by sizable potential barriers from the Rg + glycine dissociation products. Preliminary calculations show that NH2CH2COOXeH compound is energetically stable with respect to another (3-body) dissociation channel (NH2CH2COO + Rg + H), while the corresponding Ar species is not stable in this respect. The compound with the inserted Kr is a borderline case, with the 3-body dissociation products being close in energy to the NH2CH2COOKrH minimum.

U.S. Geological Survey Noble Gas Laboratory’s standard operating procedures for the measurement of dissolved gas in water samples

USGS Publications Warehouse

Hunt, Andrew G.

2015-08-12

This report addresses the standard operating procedures used by the U.S. Geological Survey’s Noble Gas Laboratory in Denver, Colorado, U.S.A., for the measurement of dissolved gases (methane, nitrogen, oxygen, and carbon dioxide) and noble gas isotopes (helium-3, helium-4, neon-20, neon-21, neon-22, argon-36, argon-38, argon-40, kryton-84, krypton-86, xenon-103, and xenon-132) dissolved in water. A synopsis of the instrumentation used, procedures followed, calibration practices, standards used, and a quality assurance and quality control program is presented. The report outlines the day-to-day operation of the Residual Gas Analyzer Model 200, Mass Analyzer Products Model 215–50, and ultralow vacuum extraction line along with the sample handling procedures, noble gas extraction and purification, instrument measurement procedures, instrumental data acquisition, and calculations for the conversion of raw data from the mass spectrometer into noble gas concentrations per unit mass of water analyzed. Techniques for the preparation of artificial dissolved gas standards are detailed and coupled to a quality assurance and quality control program to present the accuracy of the procedures used in the laboratory.

Venus, Earth, Xenon

NASA Astrophysics Data System (ADS)

Zahnle, K. J.

2013-12-01

Xenon has been regarded as an important goal of many proposed missions to Venus. This talk is intended to explain why. Despite its being the heaviest gas found in natural planetary atmospheres, there is more evidence that Xe escaped from Earth than for any element apart from helium: (i) Atmospheric Xe is very strongly mass fractionated (at about 4% per amu) from any known solar system source. This suggests fractionating escape that preferentially left the heavy Xe isotopes behind. (ii) Xe is underabundant compared to Kr, a lighter noble gas that is not strongly mass fractionated in air. (iii) Radiogenic Xe is strongly depleted by factors of several to ~100 compared to the quantities expected from radioactive decay of primordial solar system materials. In these respects Xe on Mars is similar to Xe on Earth, but with one key difference: Xe on Mars is readily explained by a simple process like hydrodynamic escape that acts on an initially solar or meteoritic Xe. This is not so for Earth. Earth's Xe cannot be derived by an uncontrived mass fractionating process acting on any known type of Solar System Xe. Earth is a stranger, made from different stuff than any known meteorite or Mars or even the Sun. Who else is in Earth's family? Comets? We know nothing. Father Zeus? Data from Jupiter are good enough to show that jovian Xe is not strongly mass-fractionated but not good enough to determine whether Jupiter resembles the Earth or the Sun. Sister Venus? Noble gas data from Venus are incomplete, with Kr uncertain and Xe unmeasured. Krypton was measured by several instruments on several spacecraft. The reported Kr abundances are discrepant and were once highly controversial. These discrepancies appear to have been not so much resolved as forgotten. Xenon was not detected on Venus. Upper limits were reported for the two most abundant xenon isotopes 129Xe and 132Xe. From the limited data it is not possible to tell whether Venus's affinities lie with the solar wind, or with

21 CFR 872.3060 - Noble metal alloy.

Code of Federal Regulations, 2011 CFR

2011-04-01

... 21 Food and Drugs 8 2011-04-01 2011-04-01 false Noble metal alloy. 872.3060 Section 872.3060 Food... DEVICES DENTAL DEVICES Prosthetic Devices § 872.3060 Noble metal alloy. (a) Identification. A noble metal alloy is a device composed primarily of noble metals, such as gold, palladium, platinum, or silver, that...

21 CFR 872.3060 - Noble metal alloy.

Code of Federal Regulations, 2010 CFR