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technical report and journal articles

Description: Objective: This project seeks to improve the application of noble gas isotope studies to multiphase fluid processes in the Earth's crust by (1) identifying the important noble gas carrier phases in sediments to address the processes that have led to the observed enrichment and depletion patterns in sedimentary rocks and fluids, (2) examine the mechanisms by which such noble gas patterns are acquired, trapped and subsequently released to mobile crustal fluids, and (3) evaluate the time and length scales for the transport of noble gas components, such as radiogenic 4He, through the continental crust.. Project Description: Sedimentary rocks and oil field gases typically are enriched in heavy noble gases: Xe/Ar ratios of ~10-10,000 times the ratio in air have been observed that cannot be explained by adsorption hypotheses. Laboratory experiments designed to isolate sedimentary phases for noble gas analysis are conducted to identify the carrier phase(s). It has been observed that radiogenic 4He accumulates in confined aquifer waters at rates that exceed the rate of local production and approaching the whole crustal production rate. A literature evaluation of 4He, 3He crustal fluxes is being conducted to evaluate crustal scale mass transport in terms of the rate, mechanisms, temporal and spatial variability and the role played by tectonic processes. Results: The laboratory study has concentrated on noble gas abundances in a variety of sedimentary silica samples. We have found that, in general, samples of inorganic silica have noble gas abundances that are consistent with occlusion of air-saturated water in fluid inclusions and lack requisite enrichment/depletion factors needed to explain the noble gas inventory in oil field fluids. However, numerous replicate analyses of noble gases extracted from silica spicules from live sponges (Calyxnicaeensis) show significantly enriched Ar, Kr, and Xe concentrations ([iNg]sample/[iNg]asw > 1), but with very little if any mass dependence ...
Date: March 25, 2011
Creator: Torgerson, Thomas & Kennedy, B. M.
Partner: UNT Libraries Government Documents Department

Inductively Coupled Plasma Etching of III-Nitrides in Cl(2)/Xe,Cl(2)/Ar and Cl(2)/He

Description: The role of additive noble gases He, Ar and Xe to C&based Inductively Coupled Plasmas for etching of GaN, AIN and InN were examined. The etch rates were a strong function of chlorine concentration, rf chuck power and ICP source power. The highest etch rates for InN were obtained with C12/Xe, while the highest rates for AIN and GaN were obtained with C12/He. Efficient breaking of the 111-nitrogen bond is crucial for attaining high etch rates. The InN etching was dominated by physical sputtering, in contrast to GaN and AIN. In the latter cases, the etch rates were limited by initial breaking of the III-nitrogen bond. Maximum selectivities of -80 for InN to GaN and InN to AIN were obtained.
Date: January 5, 1999
Creator: Abernathy, C.R.; Cho, H.; Donovan, S.M.; Hahn, Y.B.; Hays, D.C.; Jung, K.B. et al.
Partner: UNT Libraries Government Documents Department


Description: Separate abstracts were prepared for thirty-one of the thirty-three sections. Of the sections not abstracted, the one entitled Fission Product Transport'' contained no information, the other, Transport of Noble Gases in Graphite'' is available in a more complete form as ORNLTM-I35 (NSA 16: 9209) (J.R.D.)
Date: May 11, 1962
Partner: UNT Libraries Government Documents Department

Isotopic mass-dependence of noble gas diffusion coefficients inwater

Description: Noble gas isotopes are used extensively as tracers inhydrologic and paleoclimatic studies. These applications requireknowledge of the isotopic mass (m) dependence of noble gas diffusioncoefficients in water (D), which has not been measured but is estimatedusing experimental D-values for the major isotopes along with an untestedrelationship from kinetic theory, D prop m-0.5. We applied moleculardynamics methods to determine the mass dependence of D for four noblegases at 298 K, finding that D prop m-beta with beta<0.2, whichrefutes the kinetic theory model underlying all currentapplications.
Date: June 25, 2007
Creator: Bourg, I.C. & Sposito, G.
Partner: UNT Libraries Government Documents Department

High order harmonic generation in rare gases

Description: The process of high order harmonic generation in atomic gases has shown great promise as a method of generating extremely short wavelength radiation, extending far into the extreme ultraviolet (XUV). The process is conceptually simple. A very intense laser pulse (I {approximately}10{sup 13}-10{sup 14} W/cm{sup 2}) is focused into a dense ({approximately}10{sup l7} particles/cm{sup 3}) atomic medium, causing the atoms to become polarized. These atomic dipoles are then coherently driven by the laser field and begin to radiate at odd harmonics of the laser field. This dissertation is a study of both the physical mechanism of harmonic generation as well as its development as a source of coherent XUV radiation. Recently, a semiclassical theory has been proposed which provides a simple, intuitive description of harmonic generation. In this picture the process is treated in two steps. The atom ionizes via tunneling after which its classical motion in the laser field is studied. Electron trajectories which return to the vicinity of the nucleus may recombine and emit a harmonic photon, while those which do not return will ionize. An experiment was performed to test the validity of this model wherein the trajectory of the electron as it orbits the nucleus or ion core is perturbed by driving the process with elliptically, rather than linearly, polarized laser radiation. The semiclassical theory predicts a rapid turn-off of harmonic production as the ellipticity of the driving field is increased. This decrease in harmonic production is observed experimentally and a simple quantum mechanical theory is used to model the data. The second major focus of this work was on development of the harmonic {open_quotes}source{close_quotes}. A series of experiments were performed examining the spatial profiles of the harmonics. The quality of the spatial profile is crucial if the harmonics are to be used as the source ...
Date: May 1, 1994
Creator: Budil, K.S.
Partner: UNT Libraries Government Documents Department

Mass- and temperature-dependent diffusion coefficients for lightnoble gases for the TOUGH2-EOSN Model

Description: This report describes modifications made to the EOSN module(Shan and Pruess, 2003) of the nonisothermal multiphase flow simulatorTOUGH2 (Pruess, et al., 1999). The EOSN fluid property module simulatestransport of water, brine, air, and noble gases or CO2 in the subsurface.In the standard version of the EOSN module, diffusion coefficients can bespecified by the user, but there is no allowance for liquid-phasediffusion coefficients to change with temperature. Furthermore, usersmust specify radiogenic sources of heat and helium for each element indata block GENER, which can be a time-consuming task for models withlarge numbers of elements. Our modifications seek to increase thefunctionality and efficiency of using TOUGH2-EOSN by allowing for mass-and temperature-dependent liquid-phase diffusion coefficients for heliumand neon and specification of radiogenic heat and helium production as aproperty of a material. The modified version is based on TOUGH2-EOSN andthus requires familiarity with the capabilities and input formats of theTOUGH2 code (Pruess, et al., 1999) and the EOSN module (Shan and Pruess,2003). This report only details our modifications and how to properlyutilize them.
Date: April 13, 2007
Creator: Andrews, J.L.; Finsterle, S. & Saar, M.O.
Partner: UNT Libraries Government Documents Department

EOSN: A TOUGH2 module for noble gases

Description: We developed a new fluid property module for TOUGH2, called EOSN, to simulate transport of noble gases in the subsurface. Currently, users may select any of five different noble gases as well as CO2, two at a time. For the three gas components (air and two user-specified noble gases) in EOSN, the Henry's coefficients and the diffusivities in the gas phase are no longer assumed constants, but are temperature dependent. We used the Crovetto et al. (1982) model to estimate Henry's coefficients, and the Reid et al. (1987) correlations to calculate gas phase diffusivities. The new module requires users to provide names of the selected noble gases, which properties are provided internally. There are options for users to specify any (non-zero) molecular weights and half-lives for the gas components. We provide two examples to show applications of TOUGH2IEOSN. While temperature effects are relatively insignificant for one example problem where advection is dominant, they cause almost an order of magnitude difference for the other case where diffusion becomes a dominant process and temperature variations are relatively large. It appears that thermodynamic effects on gas diffusivities and Henry's coefficients can be important for low-permeability porous media and zones with large temperature variations.
Date: March 7, 2003
Creator: Shan, Chao & Pruess, Karsten
Partner: UNT Libraries Government Documents Department


Description: The research outlined below established theoretical proof-of-concept using ab initio calculations that {sup 3}He can be separated from {sup 4}He by taking advantage of weak van der Waals interactions with other higher molecular weight rare gases such as xenon. To the best of our knowledge, this is the only suggested method that exploits the physical differences of the isotopes using a chemical interaction.
Date: September 4, 2012
Creator: Roy, L.; Nigg, H. & Watson, H.
Partner: UNT Libraries Government Documents Department

Pulse Radiolysis in Supercritical Rare Gas Fluids

Description: Recently, supercritical fluids have become quite popular in chemical and semiconductor industries for applications in chemical synthesis, extraction, separation processes, and surface cleaning. These applications are based on: the high dissolving power due to density build-up around solute molecules, and the ability to tune the conditions of a supercritical fluid, such as density and temperature, that are most suitable for a particular reaction. The rare gases also possess these properties and have the added advantage of being supercritical at room temperature. Information about the density buildup around both charged and neutral species can be obtained from fundamental studies of volume changes in the reactions of charged species in supercritical fluids. Volume changes are much larger in supercritical fluids than in ordinary solvents because of their higher compressibility. Hopefully basic studies, such as discussed here, of the behavior of charged species in supercritical gases will provide information useful for the utilization of these solvents in industrial applications.
Date: January 1, 2007
Creator: Holroyd, R.
Partner: UNT Libraries Government Documents Department

Helium measurements of pore-fluids obtained from SAFOD drillcore

Description: {sup 4}He accumulated in fluids is a well established geochemical tracer used to study crustal fluid dynamics. Direct fluid samples are not always collectable; therefore, a method to extract rare gases from matrix fluids of whole rocks by diffusion has been adapted. Helium was measured on matrix fluids extracted from sandstones and mudstones recovered during the San Andreas Fault Observatory at Depth (SAFOD) drilling in California, USA. Samples were typically collected as subcores or from drillcore fragments. Helium concentration and isotope ratios were measured 4-6 times on each sample, and indicate a bulk {sup 4}He diffusion coefficient of 3.5 {+-} 1.3 x 10{sup -8} cm{sup 2}s{sup -1} at 21 C, compared to previously published diffusion coefficients of 1.2 x 10{sup -18} cm{sup 2}s{sup -1} (21 C) to 3.0 x 10{sup -15} cm{sup 2}s{sup -1} (150 C) in the sands and clays. Correcting the diffusion coefficient of {sup 4}He{sub water} for matrix porosity ({approx}3%) and tortuosity ({approx}6-13) produces effective diffusion coefficients of 1 x 10{sup -8} cm{sup 2}s{sup -1} (21 C) and 1 x 10{sup -7} (120 C), effectively isolating pore fluid {sup 4}He from the {sup 4}He contained in the rock matrix. Model calculations indicate that &lt;6% of helium initially dissolved in pore fluids was lost during the sampling process. Complete and quantitative extraction of the pore fluids provide minimum in situ porosity values for sandstones 2.8 {+-} 0.4% (SD, n=4) and mudstones 3.1 {+-} 0.8% (SD, n=4).
Date: April 15, 2010
Creator: Ali, S.; Stute, M.; Torgersen, T.; Winckler, G. & Kennedy, B.M.
Partner: UNT Libraries Government Documents Department

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

Description: Gold Basin is a large L4 chondrite shower, that was recently discovered in the Mojave Desert, Arizona [1]. Based on {sup 109}Be and {sup 14}C concentrations in several fragments, the pre-atmospheric radius of this shower was estimated to be 3-4 meters [2]. Among chondrites, Gold Basin is one of the largest, thus providing a unique opportunity for comparing measured cosmogenic nuclide concentrations with model calculations for large objects. Noble gas measurements combined with {sup 10}Be data of most Gold Basin samples suggest a single-stage exposure of 15-30 Myr, although a few samples may require a complex exposure history [3]. We selected eight samples of the Gold Basin shower that were analyzed for noble gases; these samples represent a wide range of shielding depths.
Date: April 30, 2001
Creator: Welten, K.C.; Nishiizumi, K.; Caffee, M.; Masarik, J. & Wieler, R.
Partner: UNT Libraries Government Documents Department

Nuclear magnetic resonance imaging with hyper-polarized noble gases

Description: This is the final report of a six-month, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). The nuclei of noble gases can be hyper polarized through a laser-driven spin exchange to a degree many orders of magnitude larger than that attainable by thermal polarization without requiring a strong magnetic field. The increased polarization from the laser pumping enables a good nuclear magnetic resonance (NMR) signal from a gas. The main goal of this project was to demonstrate diffusion-weighted imaging of such hyper-polarized noble gas with magnetic resonance imaging (MRI). Possible applications include characterizing porosity of materials and dynamically imaging pressure distributions in biological or acoustical systems.
Date: October 1, 1997
Creator: Schmidt, D.M.; George, J.S.; Penttila, S.I. & Caprihan, A.
Partner: UNT Libraries Government Documents Department

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

Description: 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 permit 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.
Date: December 1, 1999
Creator: Goodson, Boyd M.
Partner: UNT Libraries Government Documents Department

The Potential for Dating Groundwater Using Radiogenic Noble Gases

Description: The accumulation in groundwater of products from the radioactive decay of elements naturally found in rocks offers a potential for measuring the time that the groundwater has been contact with the rock. This dating method has an advantage over using decay products from the atmosphere in that the amount of decay products increases with age rather than decreases. However, different decay products accumulate at different rates and, thus, have a different potential usefulness in age determinations. The most useful decay product is helium, produced from uranium and thorium. The use of Ar-40 produced from potassium is limited because Ar-40 is abundant in meteoric water. Neon, xenon and krypton are useful with great difficulty because they are produced in extremely small quantities. In general, the potential for error increases when a long time is required to produce a small quantity of the dating nuclide.
Date: March 23, 2001
Creator: Cornman, W.R.
Partner: UNT Libraries Government Documents Department

Observation of Optical Pulse and Material Dynamics on the Femtosecond Time-Scale

Description: The widespread availability of lasers that generate pulses on the femtosecond scale has opened new realms of investigation in the basic and applied sciences, rendering available excitations delivering intensities well in excess of 10{sup 21} W/cm{sup 2}, and furnishing probes capable of resolving molecular relaxation timescales. As a consequence and a necessity, sophisticated techniques to examine the pulse behavior on the femtosecond scale have been developed and are of crucial importance to gain insight on the behavior of physical systems. These techniques will be discussed with specific application to guided pulse propagation and ionization dynamics of noble gases.
Date: September 13, 1999
Creator: Omenetto, F.; Luce, B.; Siders, C.W. & Taylor, A.J.
Partner: UNT Libraries Government Documents Department

Low-field magnetic resonance imaging of gases

Description: This is the final report of a six-month, Laboratory-Directed Research and Development (LDRD) project at the Los Alamos National Laboratory (LANL). The main goal of this project was to develop the capability to conduct low-field magnetic resonance imaging of hyper-polarized noble gas nuclei and of thermally polarized protons in water. The authors constructed a versatile low-field NMR system using a SQUID gradiometer detector inside a magnetically shielded room. This device has sufficient low-field sensitivity to detect the small signals associated with NMR at low magnetic fields.
Date: November 1, 1998
Creator: Schmidt, D.M. & Espy, M.A.
Partner: UNT Libraries Government Documents Department

Diffusive separation of noble gases and noble gas abundance patterns in sedimentary rocks

Description: The mechanisms responsible for noble gas concentrations, abundance patterns, and strong retentivity in sedimentary lithologies remain poorly explained. Diffusion-controlled fractionation of noble gases is modeled and examined as an explanation for the absolute and relative abundances of noble gases observed in sediments. Since the physical properties of the noble gases are strong functions of atomic mass, the individual diffusion coefficients, adsorption coefficients and atomic radii combine to impede heavy noble gas (Xe) diffusion relative to light noble gas (Ne) diffusion. Filling of lithic grains/half-spaces by diffusive processes thus produces Ne enrichments in the early and middle stages of the filling process with F(Ne) values similar to that observed in volcanic glasses. Emptying lithic grains/half-spaces produces a Xe-enriched residual in the late (but not final) stages of the process producing F(Xe) values similar to that observed in shales. 'Exotic but unexceptional' shales that exhibit both F(Ne) and F(Xe) enrichments can be produced by incomplete emptying followed by incomplete filling. This mechanism is consistent with literature reported noble gas abundance patterns but may still require a separate mechanism for strong retention. A system of labyrinths-with-constrictions and/or C-, Si-nanotubes when combined with simple adsorption can result in stronger diffusive separation and non-steady-state enrichments that persist for longer times. Enhanced adsorption to multiple C atoms inside C-nanotubes as well as dangling functional groups closing the ends of nanotubes can provide potential mechanisms for 'strong retention'. We need new methods of examining noble gases in rocks to determine the role and function of angstrom-scale structures in both the diffusive enrichment process and the 'strong retention' process for noble gas abundances in terrestrial rocks.
Date: June 14, 2004
Creator: Torgersen, T.; Kennedy, B.M. & van Soest, M.C.
Partner: UNT Libraries Government Documents Department

EOSN - A new TOUGH2 module for simulating transport of noble gases in the subsurface

Description: Noble gases widely exist in nature, and except for radon, they are stable. Modern techniques can detect noble gases to relatively low concentrations and with great precision. These factors suggest that noble gases can be useful tracers for subsurface characterization. Their applications, however, require an appropriate transport model for data analyses. A new fluid property module, EOSN, was developed for TOUGH2 to simulate transport of noble gases in the subsurface. Currently any of five different noble gases (except radon) as well as CO{sub 2} can be selected, two at a time. For the two selected gas components, the Crovetto et al. (1982) model is used to calculate the Henry's law coefficients; and the Reid et al. (1987) correlation is used to calculate the gas phase diffusivities. Like most other sister modules, TOUGH2/EOSN can simulate nonisothermal multiphase flow and fully coupled transport in fractured porous media. Potential applications of the new module include, but are not limited to: (a) study of different reservoir processes such as recharge, boiling, condensation, and fracture-matrix fluid exchange; (b) characterization of reservoir geometry such as fracture spacing; and (c) analysis of CO{sub 2} sequestration.
Date: April 2, 2003
Creator: Shan, Chao & Pruess, Karsten
Partner: UNT Libraries Government Documents Department

CANCELLED Molecular dynamics simulations of noble gases in liquidwater: Solvati on structure, self-diffusion, and kinetic isotopeeffect

Description: Despite their great importance in low-temperaturegeochemistry, self-diffusion coefficients of noble gas isotopes in liquidwater (D) have been measured only for the major isotopes of helium, neon,krypton and xenon. Data on the self-diffusion coefficients of minor noblegas isotopes are essentially non-existent and so typically are estimatedby a kinetic theory model in which D varies as the inverse square root ofthe isotopic mass (m): D proportional to m-0.5. To examine the validityof the kinetic theory model, we performed molecular dynamics (MD)simulations of the diffusion of noble gases in ambient liquid water withan accurate set of noble gas-water interaction potentials. Our simulationresults agree with available experimental data on the solvation structureand self-diffusion coefficients of the major noble gas isotopes in liquidwater and reveal for the first time that the isotopic mass-dependence ofall noble gas self-diffusion coefficients has the power-law form Dproportional to m-beta with 0<beta<0.2. Thus our results callinto serious question the widespread assumption that the square rootmodel can be applied to estimate the kinetic fractionation of noble gasisotopes caused by diffusion in ambient liquid water.
Date: May 25, 2007
Creator: Bourg, I.C. & Sposito, G.
Partner: UNT Libraries Government Documents Department