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A Determination of the Fine Structure Constant Using Precision Measurements of Helium Fine Structure

Description: Spectroscopic measurements of the helium atom are performed to high precision using an atomic beam apparatus and electro-optic laser techniques. These measurements, in addition to serving as a test of helium theory, also provide a new determination of the fine structure constant α. An apparatus was designed and built to overcome limitations encountered in a previous experiment. Not only did this allow an improved level of precision but also enabled new consistency checks, including an extremely useful measurement in 3He. I discuss the details of the experimental setup along with the major changes and improvements. A new value for the J = 0 to 2 fine structure interval in the 23P state of 4He is measured to be 31 908 131.25(30) kHz. The 300 Hz precision of this result represents an improvement over previous results by more than a factor of three. Combined with the latest theoretical calculations, this yields a new determination of α with better than 5 ppb uncertainty, α-1 = 137.035 999 55(64).
Date: August 2010
Creator: Smiciklas, Marc
Partner: UNT Libraries

Surface structure of CdSe Nanorods revealed by combined X-rayabsorption fine structure measurements and ab-initio calculations

Description: We report orientation-specific, surface-sensitive structural characterization of colloidal CdSe nanorods with extended X-ray absorption fine structure spectroscopy and ab-initio density functional theory calculations. Our measurements of crystallographically-aligned CdSe nanorods show that they have reconstructed Cd-rich surfaces. They exhibit orientation-dependent changes in interatomic distances which are qualitatively reproduced by our calculations. These calculations reveal that the measured interatomic distance anisotropy originates from the nanorod surface.
Date: January 27, 2006
Creator: Aruguete, Deborah A.; Marcus, Matthew A.; Li, Liang-shi; Williamson, Andrew; Fakra, Sirine; Gygi, Francois et al.
Partner: UNT Libraries Government Documents Department

A Variation of the F-Test for Determining Statistical Relevance ofParticular Parameters in EXAFS Fits

Description: A general problem when fitting EXAFS data is determining whether particular parameters are statistically significant. The F-test is an excellent way of determining relevancy in EXAFS because it only relies on the ratio of the fit residual of two possible models, and therefore the data errors approximately cancel. Although this test is widely used in crystallography (there, it is often called a 'Hamilton test') and has been properly applied to EXAFS data in the past, it is very rarely applied in EXAFS analysis. We have implemented a variation of the F-test adapted for EXAFS data analysis in the RSXAP analysis package, and demonstrate its applicability with a few examples, including determining whether a particular scattering shell is warranted, and differentiating between two possible species or two possible structures in a given shell.
Date: July 25, 2006
Creator: Downward, L.; Booth, C.H.; Lukens, W.W. & Bridges, F.
Partner: UNT Libraries Government Documents Department

Comparison of EXAFS Foil Spectra from Around the World

Description: The EXAFS spectra of Cu and Pd foil from many different beamlines and synchrotrons are compared to address the dependence of the amplitude reduction factor (S{sub 0}{sup 2}) on beamline specific parameters. Even though S{sub 0}{sup 2} is the same parameter as the EXAFS coordination number, the value for S{sub 0}{sup 2} is given little attention, and is often unreported. The S{sub 0}{sup 2} often differs for the same material due to beamline and sample attributes, such that no importance is given to S{sub 0}{sup 2}-values within a general range of 0.7 to 1.1. EXAFS beamlines have evolved such that it should now be feasible to use standard S{sub 0}{sup 2} values for all EXAFS measurements of a specific elemental environment. This would allow for the determination of the imaginary energy (Ei) to account for broadening of the EXAFS signal rather than folding these errors into an effective S{sub 0}{sup 2}-value. To test this concept, we model 11 Cu-foil and 6 Pd-foil EXAFS spectra from around the world to compare the difference in S{sub 0}{sup 2}- and Ei-values.
Date: July 16, 2010
Creator: Kelly, S. D.; Bare, S. R.; Greenlay, N.; Azevedo, G.; Balasubramanian, M.; Barton, D. et al.
Partner: UNT Libraries Government Documents Department

A moving target: responding to magnetic and structural disorder in lanthanide- and actinide-based superconductors

Description: The effects of various chemical substitutions and induced lattice disorder in the Ce- and Pu-based 115 superconductors are reviewed, with particular emphasis on results from x-ray absorption fine structure (XAFS) measurements. The PuCoGa{sub 5} system offers the opportunity to follow changes in magnetic and electronic properties due to lattice disorder as a function of time in the same samples, in addition to the more traditional approach of perturbing the superconducting state through chemical substitutions. The reviewed work establishes a baseline for such future studies by determining the intrinsic lattice order in the 115 system, successfully understanding disorder as introduced through chemical substitutions in the Ce-based 115s, and beginning to explore the surprisingly large role of self-irradiation damage directly on the PuCoGa{sub 5} lattice. These studies lay the foundation for the harder future work toward measuring chemical substitutions in PuCoGa{sub 5}, correlating effects with non-Fermi liquid behavior, and obtaining a better structural picture of the distortions induced by {alpha}-decay of the plutonium nucleus.
Date: February 10, 2010
Creator: Booth, Corwin H.; Bauer, Eric D. & Mitchel, Jeremy N.
Partner: UNT Libraries Government Documents Department

Is U3Ni3Sn4 best described as near a quantum critical point?

Description: Although most known non-Fermi liquid (NFL) materials are structurally or chemically disordered, the role of this disorder remains unclear. In particular, very few systems have been discovered that may be stoichiometric and well ordered. To test whether U{sub 3}Ni{sub 3}Sn{sub 4} belongs in this latter class, we present measurements of the x-ray absorption fine structure (XAFS) of polycrystalline and single-crystal U{sub 3}Ni{sub 3}Sn{sub 4} samples that are consistent with no measurable local atomic disorder. We also present temperature-dependent specific heat data in applied magnetic fields as high as 8 T that show features that are inconsistent with the antiferromagnetic Griffiths' phase model, but do support the conclusion that a Fermi liquid/NFL crossover temperature increases with applied field. These results are inconsistent with theoretical explanations that require strong disorder effects, but do support the view that U{sub 3}Ni{sub 3}Sn{sub 4} is a stoichoiometric, ordered material that exhibits NFL behavior, and is best described as being near an antiferromagnetic quantum critical point.
Date: April 8, 2003
Creator: Booth, C. H.; Shlyk, L.; Nenkov, K.; Huber, J. G. & De Long, L. E.
Partner: UNT Libraries Government Documents Department

FOURIER ANALYSIS OF EXTENDED FINE STRUCTURE WITH AUTOREGRESSIVE PREDICTION

Description: Autoregressive prediction is adapted to double the resolution of Angle-Resolved Photoemission Extended Fine Structure (ARPEFS) Fourier transforms. Even with the optimal taper (weighting function), the commonly used taper-and-transform Fourier method has limited resolution: it assumes the signal is zero beyond the limits of the measurement. By seeking the Fourier spectrum of an infinite extent oscillation consistent with the measurements but otherwise having maximum entropy, the errors caused by finite data range can be reduced. Our procedure developed to implement this concept applies autoregressive prediction to extrapolate the signal to an extent controlled by a taper width. Difficulties encountered when processing actual ARPEFS data are discussed. A key feature of this approach is the ability to convert improved measurements (signal-to-noise or point density) into improved Fourier resolution.
Date: January 1, 1985
Creator: Barton, J. & Shirley, D.A.
Partner: UNT Libraries Government Documents Department

Molecular conformation changes in alkylthiols ligands as afunction of size in gold nanoparticles

Description: The bonding of hexanethiols to gold nanoparticles of 1.5, 2.0 and 3 nm was studied using X-ray Absorption Near Edge Spectroscopy (XANES) and Extended X-ray Absorption Fine Structure (EXAFS). The XANES spectra revealed that a substantial fraction of hexanethiol molecules were weakly bound, in addition to the molecules forming covalent bonds with Au surface atoms. The weakly bound molecules could be easily removed by washing in dichloromethane. After removal of the weakly bound molecules the S K-edge XANES spectrum reveals peaks due to S-Au and S-C bonds with intensities that change as a function of particle size. We explain this as the result of distortions occurring in the molecules adsorbed on the smaller particles. The distortions arise from the poor packing due to the high curvature of the particles. In addition, EXAFS results show that the smaller particles bind more molecules per Au atom than the larger ones, which is again interpreted as a result of the curved nature of the surface.
Date: January 9, 2006
Creator: Ramallo-Lopez, J.M.; Giovanetti, L.J.; Requejo, F.G.; Isaacs,S.R.; Shon, Y.S. & Salmeron, M.
Partner: UNT Libraries Government Documents Department

Lattice disorder and size-induced Kondo behavior in CeAl2 andCePt2+x

Description: When the particle size of CeAl{sub 2} and CePt{sub 2+x} samples is reduced to the nanometer scale, antiferromagnetism is suppressed and Kondo behavior dominates. We find that the Kondo temperature T{sub K} can either decrease (CeAl{sub 2}) or increase (CePt{sub 2+x}) in the nanoparticles relative to the bulk. Extended x-ray absorption fine-structure data show that the Ce-Al and Ce-Pt environments are significantly distorted in the nanoparticles. While such distortions should strongly affect magnetic and electronic properties, we find they cannot explain the observed changes in T{sub K}. Changes in the conduction density of states or other parameters must, therefore, play a significant role.
Date: March 14, 2006
Creator: Han, S.-W.; Booth, C.H.; Bauer, E.D.; P.H., Huang; Chen, Y.Y. & Lawrence, J.M.
Partner: UNT Libraries Government Documents Department

Examination of the local structure in composite and lowdimensional semiconductor by X-ray Absorption Spectroscopy

Description: X-ray absorption methods have been successfully used to obtain quantitative information about local atomic composition of two different materials. X-ray Absorption Near Edge Structure analysis and X-Ray Photoelectron Spectroscopy allowed us to determine seven chemical compounds and their concentrations in c-BN composite. Use of Extended X-ray Absorption Fine Structure in combination with Transmission Electron Microscopy enabled us to determine the composition and size of buried Ge quantum dots. It was found that the quantum dots consisted out of pure Ge core covered by 1-2 monolayers of a layer rich in Si.
Date: September 25, 2006
Creator: Lawniczak-Jablonska, K.; Demchenko, I.N.; Piskorska, E.; Wolska,A.; Talik, E.; Zakharov, D.N. et al.
Partner: UNT Libraries Government Documents Department

HIGH RESOLUTION FOURIER ANALYSIS WITH AUTO-REGRESSIVE LINEAR PREDICTION

Description: Auto-regressive linear prediction is adapted to double the resolution of Angle-Resolved Photoemission Extended Fine Structure (ARPEFS) Fourier transforms. Even with the optimal taper (weighting function), the commonly used taper-and-transform Fourier method has limited resolution: it assumes the signal is zero beyond the limits of the measurement. By seeking the Fourier spectrum of an infinite extent oscillation consistent with the measurements but otherwise having maximum entropy, the errors caused by finite data range can be reduced. Our procedure developed to implement this concept adapts auto-regressive linear prediction to extrapolate the signal in an effective and controllable manner. Difficulties encountered when processing actual ARPEFS data are discussed. A key feature of this approach is the ability to convert improved measurements (signal-to-noise or point density) into improved Fourier resolution.
Date: April 1, 1984
Creator: Barton, J. & Shirley, D.A.
Partner: UNT Libraries Government Documents Department

Effects of self-irradiation on local crystal structure and 5flocalization in PuCoGa5

Description: The 18.5 K superconductor PuCoGa{sub 5} has many unusual properties, including those due to damage induced by self-irradiation. The superconducting transition temperature decreases sharply with time, suggesting a radiation-induced Frenkel defect concentration much larger than predicted by current radiation damage theories. Extended x-ray absorption fine-structure measurements demonstrate that while the local crystal structure in fresh material is well ordered, aged material is disordered much more strongly than expected from simple defects, consistent with strong disorder throughout the damage cascade region. These data highlight the potential impact of local lattice distortions relative to defects on the properties of irradiated materials and underscore the need for more atomic-resolution structural comparisons between radiation damage experiments and theory.
Date: October 20, 2006
Creator: Booth, C.H.; Daniel, M.; Wilson, R.E.; Bauer, E.D.; Mitchell,J.N.; Moreno, N.O. et al.
Partner: UNT Libraries Government Documents Department

Hydrogenic and Screened Self-Energies for d-States

Description: The one-loop self-energy is evaluated for d{sub 3/2} and d{sub 5/2} states in hydrogenic ions, and good agreement found with previous calculations. Results are compared to what is known of the Z{alpha} expansion and higher-order binding corrections inferred for these states as well as for their fine structures. Screened Kohn-Sham potentials are then used to evaluate the one-loop self-energy corrections to n = 2 states of lithiumlike ions for Z = 10 - 100, n = 3 states of sodiumlike ions for Z = 20 - 100, and n = 4 states of copperlike ions for Z = 40 - 100. The importance of these screened calculations for the interpretation of recent high accuracy experiments is emphasized.
Date: October 17, 2005
Creator: Sapirstein, J & Cheng, K T
Partner: UNT Libraries Government Documents Department

Hydrocarbon-free resonance transition 795-nm rubidium laser

Description: An optical resonance transition rubidium laser (5{sup 2}P{sub 1/2} {yields} 5{sup 2}S{sub 1/2}) is demonstrated with a hydrocarbon-free buffer gas. Prior demonstrations of alkali resonance transition lasers have used ethane as either the buffer gas or a buffer gas component to promote rapid fine-structure mixing. However, our experience suggests that the alkali vapor reacts with the ethane producing carbon as one of the reaction products. This degrades long term laser reliability. Our recent experimental results with a 'clean' helium-only buffer gas system pumped by a Ti:sapphire laser demonstrate all the advantages of the original alkali laser system, but without the reliability issues associated with the use of ethane.
Date: January 9, 2008
Creator: Wu, S Q; Soules, T F; Page, R H; Mitchell, S C; Kanz, V K & Beach, R J
Partner: UNT Libraries Government Documents Department

Resonance transition 795-nm Rubidium laser using 3He buffer gas

Description: We report the first demonstration of a 795-nm Rubidium resonance transition laser using a buffer gas consisting of pure {sup 3}He. This follows our recent demonstration of a hydrocarbon-free 795-nm Rubidium resonance laser which used naturally-occurring He as the buffer gas. Using He gas that is isotopically enriched with {sup 3}He yields enhanced mixing of the Rb fine-structure levels. This enables efficient lasing at reduced He buffer gas pressure, improving thermal management in high average power Rb lasers and enhancing the power scaling potential of such systems.
Date: August 2, 2007
Creator: Wu, S S; Soules, T F; Page, R H; Mitchell, S C; Kanz, V K & Beach, R J
Partner: UNT Libraries Government Documents Department

Developments toward a reliable diode-pumped hydrocarbon-free 795-nm rubidium laser

Description: We report a 795-nm diode-pumpable Rb laser using a buffer gas of pure {sup 3}He. {sup 3}He gas enhances mixing of the Rb fine-structure levels. This enables efficient lasing at reduced He pressures and improved thermal management.
Date: May 7, 2008
Creator: Wu, S S; Soules, T F; Page, R H; Mitchell, S C; Kanz, V K & Beach, R J
Partner: UNT Libraries Government Documents Department

Effect of temperature on the complexation of Uranium(VI) with fluoride in aqueous solutions

Description: Complexation of U(VI) with fluoride at elevated temperatures in aqueous solutions was studied by spectrophotometry. Four successive complexes, UO{sub 2}F{sup +}, UO{sub 2}F{sub 2}(aq), UO{sub 2}F{sub 3}{sup -}, and UO{sub 2}F{sub 4}{sup 2-}, were identified, and the stability constants at 25, 40, 55, and 70 C were calculated. The stability of the complexes increased as the temperature was elevated. The enthalpies of complexation at 25 C were determined by microcalorimetry. Thermodynamic parameters indicate that the complexation of U(VI) with fluoride in aqueous solutions at 25 to 70 C is slightly endothermic and entropy-driven. The Specific Ion Interaction (SIT) approach was used to obtain the thermodynamic parameters of complexation at infinite dilution. Structural information on the U(VI)/fluoride complexes was obtained by extended X-ray absorption fine structure spectroscopy.
Date: May 18, 2009
Creator: Tian, Guoxin & Rao, Linfeng
Partner: UNT Libraries Government Documents Department

Formation of Zn-rich phyllosilicate, Zn-layered double hydroxide and hydrozincite in contaminated calcareous soils

Description: Recent studies demonstrated that Zn-phyllosilicate- and Zn-layered double hydroxide-type (Zn-LDH) precipitates may form in contaminated soils. However, the influence of soil properties and Zn content on the quantity and type of precipitate forming has not been studied in detail so far. In this work, we determined the speciation of Zn in six carbonate-rich surface soils (pH 6.2 to 7.5) contaminated by aqueous Zn in the runoff from galvanized power line towers (1322 to 30090 mg/kg Zn). Based on 12 bulk and 23 microfocused extended X-ray absorption fine structure (EXAFS) spectra, the number, type and proportion of Zn species were derived using principal component analysis, target testing, and linear combination fitting. Nearly pure Zn-rich phyllosilicate and Zn-LDH were identified at different locations within a single soil horizon, suggesting that the local availabilities of Al and Si controlled the type of precipitate forming. Hydrozincite was identified on the surfaces of limestone particles that were not in direct contact with the soil clay matrix. With increasing Zn loading of the soils, the percentage of precipitated Zn increased from {approx}20% to {approx}80%, while the precipitate type shifted from Zn-phyllosilicate and/or Zn-LDH at the lowest studied soil Zn contents over predominantly Zn-LDH at intermediate loadings to hydrozincite in extremely contaminated soils. These trends were in agreement with the solubility of Zn in equilibrium with these phases. Sequential extractions showed that large fractions of soil Zn ({approx}30% to {approx}80%) as well as of synthetic Zn-kerolite, Zn-LDH, and hydrozincite spiked into uncontaminated soil were readily extracted by 1 M NH{sub 4}NO{sub 3} followed by 1 M NH{sub 4}-acetate at pH 6.0. Even though the formation of Zn precipitates allows for the retention of Zn in excess to the adsorption capacity of calcareous soils, the long-term immobilization potential of these precipitates is limited.
Date: October 15, 2007
Creator: Jacquat, Olivier; Voegelin, Andreas; Villard, Andre; Marcus, Matthew A. & Kretzschmar, Ruben
Partner: UNT Libraries Government Documents Department

X-ray absorption spectroscopy at the Ni-K edge in Stackhousia tryonii Bailey hyperaccumulator

Description: Young plants of Stackhousia tryonii Bailey were exposed to 34 mM Ni kg-1 in the form of NiSO4- 6H2O solution and grown under controlled glasshouse conditions for a period of 20 days. Fresh leaf, stem and root samples were analysed in vivo by micro x-ray absorption spectroscopy (XAS) at the Ni-K edge.Both x-ray absorption near edge structure and extended x-ray absorption fine structure spectra were analysed, and theresulting spectra were compared with spectra obtained from nine biologically important Ni-containing model compounds. The results revealed that themajority of leaf, stem and root Ni in the hyperaccumulator was chelated by citrate.Our results also suggest that in leavesNi is complexed by phosphate and histidine, and in stems and roots, phytate and histidine. The XAS results provide an important physiological insightinto transport, detoxification and storage of Ni in S. tryonii plants.
Date: October 8, 2007
Creator: Ionescu, Mihail; Bhatia, Naveen P.; Cohen , David D.; Siegele, R.; Marcus, Matthew A.; Fakra, Sirine C. et al.
Partner: UNT Libraries Government Documents Department

Physics based calculation of the fine structure constant

Description: We assume that the coupling between particles and photons is defined by a surface area and a temperature, and that the square of the temperature is the inverse of the surface area ({Dirac_h}=c= 1). By making assumptions regarding stimulated emission and effects associated with the finite length of a string that forms the particle surface, the fine structure constant is calculated to be {approx}1/137.04. The corresponding calculated fundamental unit of charge is 1.6021 x 10{sup -19} C.
Date: January 1, 2009
Creator: Lestone, John Paul
Partner: UNT Libraries Government Documents Department

EXAFS Signatures of Structural Zn at Trace Levels in Layered Minerals

Description: Many in situ XAFS studies have shown that zinc incorporated in layered minerals is a major form of zinc in Zn-contaminated soils. Quantitative information on the local structural environment(s) and ordering of Zn in these minerals is required to better understand its behavior in soils. In this study, EXAFS spectroscopy was used to assess the structural environment of zinc incorporated at trace levels (40 ppm to 4,000 ppm) within the octahedral sheets of various natural and synthetic layered minerals. Results indicate that EXAFS data analyzed using ab initio FEFF calculations (FEFF 8.10) can unambiguously distinguish between zinc incorporation within the octahedral sheet of dioctahedral versus trioctahedral layered minerals and can determine the distribution (random or ordered) of zinc cations within the octahedral sheets of these minerals.
Date: December 13, 2006
Creator: Juillot, Farid; Morin, Guillaume; Hazemann, Jean-Louis; Proux, Olivier; Belin, Stephanie; Briois, Valerie et al.
Partner: UNT Libraries Government Documents Department

Promoting Uranium Immobilization by the Activities of Microbial Phosphatases

Description: The overall objective of this project is to examine the activity of nonspecific phosphohydrolases present in naturally occurring subsurface microorganisms for the purpose of promoting the immobilization of radionuclides through the production of uranium [U(VI)] phosphate precipitates. Specifically, we hypothesize that the precipitation of U(VI) phosphate minerals may be promoted through the microbial release and/or accumulation of PO4 3- as a means to detoxify radionuclides and heavy metals. An experimental approach was designed to determine the extent of phosphatase activity in bacteria previously isolated from contaminated subsurface soils collected at the ERSP Field Research Center (FRC) in Oak Ridge, TN. Screening of 135 metal resistant isolates for phosphatase activity indicated the majority (75 of 135) exhibited a phosphatase-positive phenotype. During this phase of the project, a PCR based approach has also been designed to assay FRC isolates for the presence of one or more classes of the characterized non-specific acid phophastase (NSAP) genes likely to be involved in promoting U(VI) precipitation. Testing of a subset of Pb resistant (Pbr) Arthrobacter, Bacillus and Rahnella strains indicated 4 of the 9 Pbr isolates exhibited phosphatase phenotypes suggestive of the ability to bioprecipitate U(VI). Two FRC strains, a Rahnella sp. strain Y9602 and a Bacillus sp. strain Y9-2, were further characterized. The Rahnella sp. exhibited enhanced phosphatase activity relative to the Bacillus sp. Whole-cell enzyme assays identified a pH optimum of 5.5, and inorganic phosphate accumulated in pH 5.5 synthetic groundwater (designed to mimic FRC conditions) incubations of both strains in the presence of a model organophosphorus substrate provided as the sole C and P source. Kinetic experiments showed that these two organisms can grow in the presence of 200 μM dissolved uranium and that Rahnella is much more efficient in precipitating U(VI) than Bacillus sp. The precipitation of U(VI) must be mediated ...
Date: April 19, 2007
Creator: Martinez, Robert J.; Beazley, Melanie J.; Webb, Samuel M.; Taillefert, Martial & Sobecky, Patricia A.
Partner: UNT Libraries Government Documents Department