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PubMed2003

The 'zero charge' partitioning behaviour of noble gases during mantle melting.

Noble-gas geochemistry is an important tool for understanding planetary processes from accretion to mantle dynamics and atmospheric formation. Central to much of the modelling of such processes is the crystal-melt partitioning of noble gases during mantle melting, magma ascent and near-surface degassing. Geochemists have traditionally considered the 'inert' noble gases to be extremely incompatible elements, with almost 100 per cent extraction efficiency from the solid phase during melting processes. Previously published experimental data on partitioning between crystalline silicates and melts has, however, suggested that noble gases approach compatible behaviour, and a significant proportion should therefore remain in the mantle during melt extraction. Here we present experimental data to show that noble gases are more incompatible than previously demonstrated, but not necessarily to the extent assumed or required by geochemical models. Independent atomistic computer simulations indicate that noble gases can be considered as species of 'zero charge' incorporated at crystal lattice sites. Together with the lattice strain model, this provides a theoretical framework with which to model noble-gas geochemistry as a function of residual mantle mineralogy.

Journal Article↗

PubMed2001

Single-bubble sonoluminescence from noble gases.

Single-bubble sonoluminescence (SBSL) from noble gases in water is studied theoretically in order to clarify the reason of the distinguished feature that the luminescence is strong for all noble gases, while the other systems of cavitation luminescence are greatly enhanced by the presence of the heavy noble gas(xenon). It is clarified that in spite of the larger thermal conductivity of lighter noble gases the maximum temperature in a SBSL bubble of lighter noble gases is higher due both to the segregation of water vapor and noble gas inside a SBSL bubble and the stronger acoustic drive of a SBSL bubble of lighter noble gases.

Journal Article↗

PubMed1992

Possible cometary origin of heavy noble gases in the atmospheres of Venus, Earth and Mars

Models that trace the origin of noble gases in the atmospheres of the terrestrial planets (Venus, Earth and Mars) to the 'planetary component' in chondritic meteorites confront several problems. The 'missing' xenon in the atmospheres of Mars and Earth is one of the most obvious; this gas is not hidden or trapped in surface materials. On Venus, the absolute abundances of neon and argon per gram of rock are higher even than those in carbonaceous chondrites, whereas the relative abundances of argon and krypton are closer to solar than to chondritic values (there is only an upper limit on xenon). Pepin has developed a model that emphasizes hydrodynamic escape of early, massive hydrogen atmospheres to explain the abundances and isotope ratios of noble gases on all three planets. We have previously suggested that the unusual abundances of heavy noble gases on Venus might be explained by the impact of a low-temperature comet. Further consideration of the probable history of the martian atmosphere, the noble-gas data from the (Mars-derived) SNC meteorites and laboratory experiments on the trapping of noble gases in ice lead us to propose here that the noble gases in the atmospheres of all of the terrestrial planets are dominated by a mixture of an internal component and contribution from impacting icy planetesimals (comets). If true, this hypothesis illustrates the importance of impacts in determining the volatile inventories of these planets.

Argon↗

PubMed2000

Palaeotemperature reconstruction from noble gases in ground water taking into account equilibration with entrapped air

Noble-gas concentrations in ground water have been used as a proxy for past air temperatures, but the accuracy of this approach has been limited by the existence of a temperature-independent component of the noble gases in ground water, termed 'excess air' whose origin and composition is poorly understood. In particular, the evidence from noble gases in a Brazilian aquifer for a cooling of more than 5 C in tropical America during the Last Glacial Maximum has been called into question. Here we propose a model for dissolved gases in ground water, which describes the formation of excess air by equilibration of ground water with entrapped air in quasi-saturated soils. Our model predicts previously unexplained noble-gas data sets, including the concentration of atmospheric helium, and yields consistent results for the non-atmospheric helium isotopes that are used for dating ground water. Using this model of excess air, we re-evaluate the use of noble gases from ground water for reconstructing past temperatures. Our results corroborate the inferred cooling in Brazil during the Last Glacial Maximum, and indicate that even larger cooling took place at mid-latitudes.

Journal Article↗

PubMed1998

MRI using hyperpolarized noble gases.

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.

Adult↗

PubMed1998

[Magnetic resonance tomography with inhalation of polarized noble gases: new perspectives in functional imaging diagnosis of emphysema].

PURPOSE: Based on a review of the background of MRI using inhaled hyperpolarized noble gases first experiences and perspectives for functional imaging in emphysema patients are presented. MATERIAL AND METHODS: In vonventional MRI, the spin density of protons, which is defined by the Boltzmann equilibrium, is the source of the imaging signal. Since proton density in the lungs is low and multiple air-tissue interfaces exist, MRI of the lung parenchyma is unsatisfactory. The possibility to artificially enrich the spin density (hyperpolarization) in noble gases (H3-3, Xe-129) by optical pumping results in a non-equilibrium polarization five orders of magnitude higher than the Boltzmann equilibrium. Hyperpolarized noble gases can then be applied as "inhaled contrast media" using a dedicated application device. At the MR unit several prerequisites must also be fulfilled: transmit-receive coil, boradband amplifier and fast sequences with low flip angles. These are essential for dynamic scans in breath-hold tecnique of the highly diffusible He-3 or the well soluble Xe-129. RESULTS: He-3 and Xe-129 have been successfully applied for imaging of the ventilated airspaces. Besides the well-known narcotic effects of Xenon no adverse effects were observed. A homogeneous distribution of signal intensity can be regarded as a normal findings in people without lung disease. Obstructive diseases and emphysematous changes lead to generalized or localized signal inhomogeneities. Most likely they are caused by disorders of the distribution of ventilation bases on a different functional vehavior of different alveolar regions. By making use of the paramagenetic properties of oxygen, He-3 can also be used for local measurements of oxygen partial pressure in the lung. Xe-129 exhibits a different chemical shift within alveoli, interstitial space and vessels which can be measured by MRI. CONCLUSIONS: MRI using inhaled hyperpolarized noble gases is a functional imaging modality with high spatial and/or temporal resolution. First studies for early detection of obstructive lung diseases and disorders of distribution of ventilation in emphysema are promising.

Administration, Inhalation↗

PubMed1966

Growth responses of Neurospora crassa to increased partial pressures of the noble gases and nitrogen.

Buchheit, R. G. (Union Carbide Corp., Tonawanda, N.Y.), H. R. Schreiner, and G. F. Doebbler. Growth responses of Neurospora crassa to increased partial pressures of the noble gases and nitrogen. J. Bacteriol. 91:622-627. 1966.-Growth rate of the fungus Neurospora crassa depends in part on the nature of metabolically "inert gas" present in its environment. At high partial pressures, the noble gas elements (helium, neon, argon, krypton, and xenon) inhibit growth in the order: Xe > Kr> Ar >> Ne >> He. Nitrogen (N(2)) closely resembles He in inhibitory effectiveness. Partial pressures required for 50% inhibition of growth were: Xe (0.8 atm), Kr (1.6 atm), Ar (3.8 atm), Ne (35 atm), and He ( approximately 300 atm). With respect to inhibition of growth, the noble gases and N(2) differ qualitatively and quantitatively from the order of effectiveness found with other biological effects, i.e., narcosis, inhibition of insect development, depression of O(2)-dependent radiation sensitivity, and effects on tissue-slice glycolysis and respiration. Partial pressures giving 50% inhibition of N. crassa growth parallel various physical properties (i.e., solubilities, solubility ratios, etc.) of the noble gases. Linear correlation of 50% inhibition pressures to the polarizability and of the logarithm of pressure to the first and second ionization potentials suggests the involvement of weak intermolecular interactions or charge-transfer in the biological activity of the noble gases.

Argon↗

PubMed2000

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

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 of small ligands within proteins, the detection of water molecules within apolar cavities and the determination of crystallographic phases.

Amino Acid Substitution↗

PubMed2002

MRI of the lungs using hyperpolarized noble gases.

The nuclear spin polarization of the noble gas isotopes (3)He and (129)Xe can be increased using optical pumping methods by four to five orders of magnitude. This extraordinary gain in polarization translates directly into a gain in signal strength for MRI. The new technology of hyperpolarized (HP) gas MRI holds enormous potential for enhancing sensitivity and contrast in pulmonary imaging. This review outlines the physics underlying the optical pumping process, imaging strategies coping with the nonequilibrium polarization, and effects of the alveolar microstructure on relaxation and diffusion of the noble gases. It presents recent progress in HP gas MRI and applications ranging from MR microscopy of airspaces to imaging pulmonary function in patients and suggests potential directions for future developments.

Animals↗

PubMed2003

Selling candles in a post-Edison world: phasing with noble gases bound within engineered sites.

The utility of noble gases for phase determination has been limited by the lack of naturally occurring binding sites in proteins. Wild-type T4 lysozyme contains one such binding site. By mutating large hydrophobic residues to alanine, additional noble-gas binding sites have been successfully introduced into this protein. Using data from xenon derivatives of the wild type, two single mutants and the corresponding double mutant, experimental phases for T4 lysozyme have been determined using standard multiple isomorphous replacement (MIR) techniques. These phases, which were obtained from room-temperature data collected on a rotating-anode source, are comparable in quality with phases calculated using selenomethionine-based multiwavelength anomalous dispersion (MAD) methods on frozen crystals at a synchrotron. In addition, this method of introducing noble-gas binding sites near specific residues should provide useful information for determining the register of amino acids within electron-density maps and the positions of molecules within the unit cell.

Binding Sites↗

PubMedDate not supplied

[A possible molecular mechanism of the narcotic action of noble gases].

A molecular mechanism of the narcotic action of noble gases is suggested, which is based on the fact that noble gas atoms change the orientation of water molecules absorbed on the surface of axon membrane. The resulting change in the transmembrane potential deteriorates the propagation of nerve pulse.

Animals↗

PubMed1998

Signal dynamics in magnetic resonance imaging of the lung with hyperpolarized noble gases.

The nonequilibrium bulk magnetic moment of hyperpolarized (HP) noble gases generated by optical pumping has unique characteristics. Based on the Bloch equations, a model was developed describing the signal dynamics of HP gases used in magnetic resonance imaging (MRI) of the lung with special consideration to the breathing cycle. Experimental verification included extensive investigations with HP 3He and 129Xe during both inspiration and held breath in live guinea pigs. Radial acquisition was used to investigate the view variations with a temporal resolution of 5 ms. Agreement between theoretical predictions and in vivo results was excellent. Additionally, information about effects from noble gas diffusion and spin-lattice relaxation was obtained. In vivo results for T1 were 28.8 +/- 1.8 s for 3He and 31.3 +/- 1.8 s for 129Xe. Comparison with in vitro data indicated that relaxation in the pulmonary gas space is dominated by dipolar coupling with molecular oxygen. The results provide a quantitative basis for optimizing pulse sequence design in HP gas MRI of the lung.

Animals↗

PubMed2002

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

The sensitivity of conventional nuclear magnetic resonance (NMR) techniques is fundamentally limited by 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 review describes the principles and magnetic resonance applications of laser-polarized noble gases. The enormous sensitivity enhancement afforded by optical pumping can be exploited to permit a variety of novel NMR experiments across numerous 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, NMR sensitivity enhancement via polarization transfer, and low-field NMR and MRI.

Chemical Phenomena↗

PubMed2000

Fullerenes: an extraterrestrial carbon carrier phase for noble gases.

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.

Carbon↗

PubMed2006

Examination of (e,2e) scattering models by comparison of momentum profiles of noble gases between experiment and theory.

Momentum profiles have been measured for the two outermost atomic orbitals of noble gases, Ar, Kr and Xe, at incident electron energy of about 2 keV using a newly developed multichannel (e,2e) spectrometer. The experimental results exhibit significantly improved statistics compared with those achieved in previous studies while covering a wide range of momenta up to 3.6 a.u. The results are compared with theoretical calculations using four (e,2e) scattering models, the plane-wave impulse and Born approximations (PWIA and PWBA), and the distorted-wave impulse and Born approximations (DWIA and DWBA). The DWIA and DWBA scattering models have been found to satisfactorily reproduce the experimental momentum profiles in terms of both shape and intensity over the entire momentum range covered, indicating the importance of distorted wave effects for quantitatively describing (e,2e) reaction.

Computer Simulation↗

PubMed1999

Primordial noble gases from Earth's mantle: identification of a primitive volatile component

Carbon dioxide well gases in Colorado, New Mexico, and South Australia show excesses of (124-128)Xe correlated with (129)I-derived (129)Xe and (20)Ne/(22)Ne ratios that are higher than the atmospheric (20)Ne/(22)Ne ratio. The xenon isotopic data indicate the presence of a solarlike component deep within Earth. The presence of this component in crustal and upper mantle reservoirs may be explained by a steady-state transport of noble gases from the lower mantle, which still retains much of its juvenile volatile inventory. These measurements also indicate that the mantle source of these noble gases in the carbon dioxide well gases cannot be the source of Earth's present atmosphere. The variations observed in (129)Xe/(130)Xe between solar wind xenon, Earth's atmosphere, and mantle samples may be generated by variations of iodine/xenon in terrestrial reservoirs, as opposed to rapid early degassing.

Journal Article↗

PubMed1999

Sensitivity and resolution in 3D NMR microscopy of the lung with hyperpolarized noble gases.

Three-dimensional magnetic resonance images of the guinea pig lung were acquired in vivo using hyperpolarized (HP) noble gases and radial projection encoding (PE). Results obtained with 3He (voxel size 17 microl) demonstrated high image quality showing airway structure down to the 5th or 6th generations. Signal-to-noise ratios (SNRs) of 129Xe images (voxel size 40 microl) were lower by about 1 order of magnitude as a consequence of the smaller gyromagnetic ratio, a more rapid relaxation in the gas reservoir, and lower polarization and isotope abundance. Comparison between experimentally obtained SNRs and results from calculations based on a model that accounts for the three-dimensional PE acquisition scheme and the non-equilibrium situation in HP gas imaging yielded excellent agreement for small flip angles. A theoretical examination of the potential resolution in HP gas MR microscopy of the lungs suggests that in vivo visualization of alveolar clusters distal to respiratory bronchioles may be possible.

Animals↗

PubMed2000

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

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 overcome the unfavorable binding entropy.

Amino Acid Substitution↗