Physics Commons^™

Oral Presentation: Next Generation Nuclear Fuels, Douglas Hanks

Festival of Communities: UG Symposium (Posters)

Zirconium carbide has been proposed as a coating layer for next generation (“TRISO”) nuclear fuel, and is intended as a diffusion barrier to contain fission products (e.g., Pd). To study the chemical interaction between Pd and ZrC, their interface was investigated using X-ray Photoelectron Spectroscopy (XPS). Pd was step-wise deposited onto ZrC in ultra-high vacuum, and the chemical interaction at the interface was monitored, also as a function of temperature (up to 1000 C). In the presentation, details of the chemical interaction and changes in the chemical environment of Pd and their relevance for TRISO fuel will be discussed.

Hipsec X-Ray Diffraction And Infrared Spectroscopy Studies On Energetic Materials Under Extreme Conditions, Mai Huong Bausch, Yu Liu

Festival of Communities: UG Symposium (Posters)

We conducted a series of experiments on the decompositions of the energetic materials NaBH4, NH3BH3, HMX, and RDX under different pressures using the x-ray diffraction (XRD) technique; we also studied the lesser known but high-performance explosive FOX-7’s behaviors under high pressures using the infrared spectroscopy (IR) technique. For the chemical decomposition of NaBH4 and NH3BH3 we discovered possible x-ray induced hydrogen gas generation; for the decomposition of HMX and RDX, we discovered that the decay rates of these two materials vary with pressure respectively; for the study of FOX-7’s high pressure behaviors we discovered potential phase changes and pressure induced …

X-Ray Diffraction On The Thermoelectric Silicides At High Pressure, Deep Patel, Ravhi S. Kumar, Andrew Cornelius

Festival of Communities: UG Symposium (Posters)

Cobalt Silicide (CoSi2) is a transition metal disilicide that has gathered scientific interest due to its interesting thermoelectric properties and applications in silicon-based devices because of their high temperature stability. It has been reported that CoSi2 undergoes a phase transition at around 0.4 GPa and again at 13 GPa. Furthermore, at 13 GPa the material changes from a cubic cell to an orthorhombic cell, but details of the phase transition at 0.4 GPa could not be determined. To further study the properties of CoSi2 and understand its pressure induced phase changes, we recorded the structural behavior of CoSi2 under pressure.

Investigation Of Structural And Magnetic Properties Of Iron Clusters Encapsulated In Carbon, Andrew Mohrland, Eunja Kim, Phillipe Weck, Pang Tao, Kenneth Czerwinski

Festival of Communities: UG Symposium (Posters)

Our goal is to investigate and predict the properties of iron-carbon nanostructures by performing numerical calculations using the density-functional theory. We are interested in which nanostructures are most stable, and in how they are likely to form. We have a particular interest in the magnetic properties of carbon "buckyballs" containing iron particles. These structures have potential for biomedical application, including use in anti-cancer treatment. Lone iron clusters have potential for use as a catalyst designed to reduce vehicle emissions.

Speciation And Spectroscopy Of The Uranyl And Tetravalent Plutonium Nitrate Systems: Fundamental Studies And Applications To Used Fuel Reprocessing, Nicholas A. Smith

UNLV Theses, Dissertations, Professional Papers, and Capstones

This dissertation explores the use of UV-Visible spectroscopy and Time Resolved Laser Induced Fluorescence spectroscopy as near real time process monitors of uranium and plutonium concentrations in aqueous reprocessing trains. The molar absorptivities and linear ranges of these metals were investigated under total nitrate and acid concentrations similar to those found in current reprocessing systems. Concurrent to this, a new multiple wavelength monitor was derived that is capable of determining the total nitrate concentration spectroscopically. This method uses the uranium absorbance spectrum to calculate the nitrate concentration in solution. When used as part of an Advanced Safeguard suite, this technique …

Full Multiple Scattering Analysis Of Xanes At The Cd L 3- And O K- Edges In Cdo Films Combined With A Soft-X-Ray Emission Investigation, I. N. Demchenko, J. D. Denlinger, M. Chernyshova, K. M. Yu, D. T. Speaks, P. Olalde-Velasco, Oliver Hemmers, W. Walukiewicz, A. Derkachova, K. Lawniczak-Jablonska

Environmental Studies Faculty Publications

X-ray absorption near edge structure (XANES) at the cadmium L3 and oxygen K edges for CdO thin films grown by pulsed laser deposition method, is interpreted within the real-space multiple scattering formalism, FEFF code. The features in the experimental spectra are well reproduced by calculations for a cluster of about six and ten coordination shells around the absorber for L3 edge of Cd and K edge of O, respectively. The calculated projected electronic density of states is found to be in good agreement with unoccupied electronic states in experimental data and allows to conclude that the orbital character of the …

Vibrational Spectroscopic Study Of The 1,3,5,7-Cyclooctatetraene At High Static Pressures, Edward Romano

UNLV Theses, Dissertations, Professional Papers, and Capstones

1,3,5,7-cyclooctatetraene (COT) is a single-ringed hydrocarbon that has not been studied extensively under high static pressures. It was the intent of this study to reveal its high-pressure behavior through its vibrational spectra. To this end, its infrared spectra as a function of pressure were collected at the National Synchrotron Light Source (NSLS) U2A beamline, as well as its Raman spectra over pressure using a micro-Raman spectrometer.

The spectra show the typical stiffening of force constants with increasing pressure for most peaks, particularly those which would theoretically exhibit a mode-softening behavior under hypotheses of molecular planarization and aromatization. Additionally, the data …

Partial Phonon Density Of States Of 57-Iron And 161-Dysprosium In Dyfe3 By Nuclear Resonant Inelastic X-Ray Scattering Under High Pressure, Elizabeth Anne Tanis

UNLV Theses, Dissertations, Professional Papers, and Capstones

The dual partial phonon density of states (DOS) from two different Mossbauer isotopes (161Dy and 57Fe) in the same material (DyFe3) was successfully measured using the nuclear resonant inelastic x-ray scattering (NRIXS) technique at high pressure. Nuclear inelastic scattering measurements yield an in-depth understanding of the element-specific dynamic properties. The Debye temperatures , the Lamb-Mossbauer factor, and the vibrational contributions to the Helmholtz free energy, specific heat , entropy and internal energy are calculated directly from the phonon density of states.

Sulfur K-Edge Photo-Fragmentation Of Ethylene Sulfide, Wayne C. Stolte, Gunnar Ohrwall

Chemistry and Biochemistry Faculty Research

We have investigated the photofragmentation properties of the three-membered ring heterocyclic molecule ethylene sulfide or thiirane, C₂H₄S, by time-of-flight mass spectroscopy. Positive ions have been collected as a function of photon energy around the S K ionization threshold. Branching ratios were derived for all detected ions, which are informative of the decay dynamics and photofragmentation patterns of the core-excited species. We present a new assignment of the spectral features around the S K-edge.

Fragmentation Properties Of Three-Membered Ring Heterocyclic Molecules By Partial Ion Yield Spectroscopy: C2h4o And C2h4s, Wayne C. Stolte, I. Dumitriu, S-W Yu, Gunnar Ohrwall, Maria Novella Piancastelli, Dennis W. Lindle

Chemistry and Biochemistry Faculty Research

We investigated the photofragmentation properties of two three-membered ring heterocyclic molecules, C₂H₄O and C₂H₄S, by total and partial ion yield spectroscopy. Positive and negative ions have been collected as a function of photon energy around the C 1s and O 1s ionization thresholds in C₂H₄O, and around the S 2p and C 1s thresholds in C₂H₄S. We underline similarities and differences between these two analogous systems. We present a new assignment of the spectral features around the C K-edge and the sulfur L_{2 …}

Experimental And Theoretical Investigation Of Molecular Field Effects By Polarization-Resolved Resonant Inelastic X-Ray Scattering, Stephane Carniato, Renaud Guillemin, Wayne C. Stolte, Loic Journel, Richard Taieb, Dennis W. Lindle, Marc Simon

Chemistry and Biochemistry Faculty Research

We present a combined theoretical and experimental study of molecular field effects on molecular core levels. Polarization-dependent resonant inelastic x-ray scattering is observed experimentally after resonant K-shell excitation of CF₃Cl and HCl. We explain the linear dichroism observed in spin-orbit level intensities as due to molecular field effects, including singlet-triplet exchange, and interpret this behavior in terms of population differences in the 2p_x,y,z inner-shell orbitals. We investigate theoretically the different factors that can affect the electronic populations and the dynamical R dependence of the spin-orbit ratio. Finally, the results obtained are used to interpret the L-shell …

Pressure-Driven Transport Of Particles Through A Converging-Diverging Microchannel, Ye Ai, Sang W. Joo, Yingtao Jiang, Xiangchun Xuan, Shizhi Qian

Mechanical Engineering Faculty Research

Pressure-driven transport of particles through a symmetric converging-diverging microchannel is studied by solving a coupled nonlinear system, which is composed of the Navier–Stokes and continuity equations using the arbitrary Lagrangian–Eulerian finite-element technique. The predicted particle translation is in good agreement with existing experimental observations. The effects of pressure gradient, particle size, channel geometry, and a particle’s initial location on the particle transport are investigated. The pressure gradient has no effect on the ratio of the translational velocity of particles through a converging-diverging channel to that in the upstream straight channel. Particles are generally accelerated in the converging region and then …

Partial Ion Yield Sspectroscopy Around The Cl 2p And C 1s Ionization Thresholds In Cf3cl, D. Ceolin, Maria Novella Piancastelli, Wayne C. Stolte, Dennis W. Lindle

Chemistry and Biochemistry Faculty Research

We present a partial ion yield experiment on freon 13, CF₃Cl, excited in the vicinity of the C 1s and Cl 2p ionization thresholds. We have collected a large amount of cationic fragments and a few anionic fragments at both edges. We have observed a strong intensity dependence of Rydberg transitions with ion fragment size for the CF_nCl⁺ and CF_n⁺/F⁺ (n=0–3) series at both the Cl 2p and C 1s ionization edges. Selectivity in the fragmentation processes involving the C–Cl and C–F bonds are highlighted by the intensities of the C …

Yttrium And Hydrogen Superstructure And Correlation Of Lattice Expansion And Proton Conductivity In The Bazr0.9y0.1o2.95 Proton Conductor, A. Braun, A. Ovalle, V. Pomjakushin, A. Cervellino, S. Erat, Wayne C. Stolte, T. Graule

Chemistry and Biochemistry Faculty Research

Bragg reflections in Y-resonant x-ray diffractograms of BaZr_0.9Y_0.1O_2.95 (BZY10) reveal that Y is organized in a superstructure. Comparison with neutron diffraction superstructure reflections in protonated/deuterated BZY10 suggests that both superstructures are linked, and that protons move in the landscape imposed by the Y. The thermal lattice expansion decreases abruptly for protonated BZY10 at T≥648±20 K, coinciding with the onset of lateral proton diffusion and suggesting a correlation of structural changes and proton conductivity. The chemical shift in the Y L₁-shell x-ray absorption spectra reveals a reduction from Y³⁺ toward Y²⁺ upon …

Linear Dichroism In Resonant Inelastic X-Ray Scattering To Molecular Spin-Orbit States, Renaud Guillemin, Stephane Carniato, Wayne C. Stolte, Loic Journel, Richard Taieb, Dennis W. Lindle, Marc Simon

Chemistry and Biochemistry Faculty Research

Polarization-dependent resonant inelastic x-ray scattering (RIXS) is shown to be a new probe of molecular-field effects on the electronic structure of isolated molecules. A combined experimental and theoretical analysis explains the linear dichroism observed in Cl 2p RIXS following Cl 1s excitation in HCl and CF₃Cl as due to molecular-field effects, including singlet-triplet exchange, indicating polarized-RIXS provides a direct probe of spin-orbit-state populations applicable to any molecule.

Photofragmentation Of Sif4 Upon Si 2p And F 1s Core Excitation: Cation And Anion Yield Spectroscopy, Maria Novella Piancastelli, Wayne C. Stolte, Renaud Guillemin, A. Wolska, Dennis W. Lindle

Chemistry and Biochemistry Faculty Research

We have studied the fragmentation dynamics of core-excited SiF₄ by means of soft-x-ray photoexcitation and partial positive and negative ion yield measurements around the Si L_2,3-shell and F K-shell ionization thresholds. All detectable ionic fragments are reported and we observe significant differences between the various partial ion yields near the Si 2p threshold. The differences are similar to our previous results from CH₃Cl showing more extended fragmentation in correspondence to transitions to Rydberg states. At variance with smaller systems, we observe negative ion production in the shape resonance region. This can be related …

Design And Performance Of A Curved-Crystal X-Ray Emission Spectrometer, A. C. Hudson, Wayne C. Stolte, Dennis W. Lindle, Renaud Guillemin

Chemistry and Biochemistry Faculty Research

A curved-crystal x-ray emission spectrometer has been designed and built to measure 2–5 keV x-ray fluorescence resulting from a core-level excitation of gas phase species. The spectrometer can rotate 180°, allowing detection of emitted x rays with variable polarization angles, and is capable of collecting spectra over a wide energy range (20 eV wide with 0.5 eV resolution at the Cl K edge) simultaneously. In addition, the entire experimental chamber can be rotated about the incident-radiation axis by nearly 360° while maintaining vacuum, permitting measurements of angular distributions of emitted x rays.

Low-Energy Nondipole Effects In Molecular Nitrogen Valence-Shell Photoionization, Oliver Hemmers, Renaud Guillemin, D. Rolles, A. Wolska, Dennis W. Lindle, E. P. Kanter, B. Krassig, S. H. Southworth, R. Wehlitz, B. Zimmermann, V. Mckoy, P. W. Langhoff

Environmental Studies Faculty Publications

Observations are reported for the first time of significant nondipole effects in the photoionization of the outer-valence orbitals of diatomic molecules. Measured nondipole angular-distribution parameters for the 3σ_g, 1π_u, and 2σ_u shells of N₂ exhibit spectral variations with incident photon energies from thresholds to ∼200  eV which are attributed via concomitant calculations to particular final-state symmetry waves arising from (E1)⊗(M1,E2) radiation-matter interactions first-order in photon momentum. Comparisons with previously reported K-edge studies in N₂ verify linear scaling with photon momentum, accounting in part for the significantly enhanced nondipole behavior observed in inner-shell ionization …

Femtosecond Nuclear Motion Of Hcl Probed By Resonant X-Ray Raman Scattering In The Cl 1s Region, Marc Simon, Loic Journel, Stephane Carniato, Richard Taieb, I. Minkov, Faris Gel'mukhanov, P. Salek, H. Agren, Renaud Guillemin, Wayne C. Stolte, A. C. Hudson, Dennis W. Lindle

Chemistry and Biochemistry Faculty Research

Femtosecond dynamics are observed by resonant x-ray Raman scattering (RXS) after excitation along the dissociative Cl 1s→6ơ* resonance of gas-phase HCl. The short core-hole lifetime results in a complete breakdown of the common nondispersive behavior of soft-x-ray transitions between parallel potentials. We evidence a general phenomenon of RXS in the hard-x-ray region: a complete quenching of vibrational broadening. This opens up a unique opportunity for superhigh resolution x-ray spectroscopy beyond vibrational and lifetime limitations.

Anion And Cation-Yield Spectroscopy Of Core-Excited Sf6, Maria Novella Piancastelli, Wayne C. Stolte, Renaud Guillemin, A. Wolska, M. M. Sant'anna, Dennis W. Lindle

Chemistry and Biochemistry Faculty Research

We report an extensive study on total and partial-ion-yield spectroscopy around both the S 2p and F 1s thresholds in SF₆. All positive and negative single-ion channels have been measured. Below the F 1s threshold we detect a large variation in relative intensity of the resonant structures according to the specific channel monitored, indicating selective fragmentation. Above threshold, at variance with previous cases described by us, we detect high-intensity structures related to shape resonances not only in the cation channels but also for the anions. We discuss the applicability and limits of a model we …

Fragmentation Dynamics Of H2s Following S 2p Photoexcitation, Renaud Guillemin, S-W Yu, Wayne C. Stolte, Dennis W. Lindle

Chemistry and Biochemistry Faculty Research

The fragmentation dynamics of core-excited H₂S has been studied by means of partial anion and cation yield measurements around the S L_2,3-subshell ionization thresholds. All detectable ionic fragments are reported, and significant differences between partial ion yields are observed. Possible dissociation pathways are discussed by comparison to previous studies of electron spectra.

Near-Edge X-Ray Absorption Fine Structure Study Of Ion-Beam-Induced Phase Transformation In Gd2(Ti1-Yzry)2o7, Ponnusamy Nachimuthu, S. Thevuthasan, V. Shutthanandan, E. M. Adams, W. J. Weber, B. D. Begg, D. K. Shuh, Dennis W. Lindle, Eric M. Gullikson, Rupert C. Perera

Chemistry and Biochemistry Faculty Research

The structural and electronic properties of Gd₂(Ti_1−yZr_y)₂O₇ (y=0–1) pyrochlores following a 2.0-MeV Au²⁺ ion-beam irradiation (~5.0 X 10¹⁴ Au²⁺/cm²) have been investigated by Ti 2p and O 1s near-edge x-ray absorption fine structure (NEXAFS). The irradiation of Gd₂(Ti_1−yZr_y)₂O₇ leads to the phase transformation from the ordered pyrochlore structure (Fd3m) to the defect fluorite structure (Fm3m) regardless of Zr concentration. Irradiated Gd₂(Ti_{1−y …}

Nondipole Effects In The Photoionization Of Xe 4d5/2 And 4d3/2: Evidence For Quadrupole Satellites, Oliver Hemmers, Renaud Guillemin, D. Rolles, A. Wolska, Dennis W. Lindle, K. T. Cheng, W. R. Johnson, H. L. Zhou, S. T. Manson

Environmental Studies Faculty Publications

Measurements of nondipole parameters in spin-orbit-resolved Xe 4d photoionization demonstrate dynamical differences arising from relativistic effects. The experimental data do not agree with relativistic random-phase approximation calculations of single ionization dipole and quadrupole channels. It is suggested that the discrepancy is due to the omission of multiple-excitation quadrupole channels, i.e., quadrupole satellite transitions.

Probing Cation Antisite Disorder In Gd2ti2o7 Pyrochlore By Site-Specific Nexafs And Xps, Ponnusamy Nachimuthu, S. Thevuthasan, Mark H. Engelhard, W. J. Weber, D. K. Shuh, N. M. Hamdan, B. S. Mun, E. M. Adams, D. E. Mccready, V. Shutthanandan, Dennis W. Lindle, G. Balakrishnan, R. C. Ewing

Chemistry and Biochemistry Faculty Research

Disorder in Gd₂Ti₂O₇ is investigated by near-edge x-ray-absorption fine structure (NEXAFS) and x-ray photoelectron spectroscopy (XPS). NEXAFS shows Ti⁴⁺ ions occupy octahedral sites with a tetragonal distortion induced by vacant oxygen sites. O 1s XPS spectra obtained with a charge neutralization system from Gd₂Ti₂O₇(100) and the Gd₂Ti₂O₇ pyrochlore used by Chen et al. [Phys. Rev. Lett. 88, 105901 (2002)], both yielded a single peak, unlike the previous result on the latter that found two peaks. The current results give no evidence for …

Nearest-Neighbor-Atom Core-Hole Transfer In Isolated Molecules, Renaud Guillemin, Oliver Hemmers, D. Rolles, S. W. Yu, A. Wolska, I. Tran, A. C. Hudson, J. Baker, Dennis W. Lindle

Environmental Studies Faculty Publications

A new phenomenon sensitive only to next-door-neighbor atoms in isolated molecules is demonstrated using angle-resolved photoemission of site-selective core electrons. Evidence for this interatomic core-to-core electron interaction is observable only by measuring nondipolar angular distributions of photoelectrons. In essence, the phenomenon acts as a very fine atomic-scale sensor of nearest-neighbor elemental identity.

Performance Characteristics Of Beamline 6.3.1 From 200 Ev To 2000 Ev At The Advanced Light Source, Ponnusamy Nachimuthu, J. H. Underwood, C. D. Kemp, Eric M. Gullikson, Dennis W. Lindle, David K. Shuh, Rupert C. Perera

Chemistry and Biochemistry Faculty Research

Bend magnet beamline 6.3.1 at the Advanced Light Source operates from 200 eV to 2000 eV, primarily used for x-ray absorption fine structure investigations. The beamline optics consist of a compact, entrance-slitless, Hettrick-Underwood type variable-line-spacing plane-grating monochromator and refocusing mirrors to provide a 25 μm × 500 μm spot at the focal point in the reflectometer end station. Wavelength is scanned by the simple rotation of the grating and illuminates a fixed exit slit. The LabView based beamline control and data acquisition computer code has been implemented to provide a convenient interface to the user. The dedicated end station is …

Dramatic Nondipole Effects In Low-Energy Photoionization: Experimental And Theoretical Study Of Xe 5s, Oliver Hemmers, Renaud Guillemin, E. P. Kanter, B. Krassig, Dennis W. Lindle, S. H. Southworth, R. Wehlitz, J. Baker, A. C. Hudson, M. Lotrakul, D. Rolles, Wayne C. Stolte, I. Tran, A. Wolska, S. Yu, M. Ya Amusia, K. T. Cheng, L. V. Chernysheva, W. R. Johnson, S. T. Manson

Environmental Studies Faculty Publications

The Xe 5s nondipole photoelectron parameter γ is obtained experimentally and theoretically from threshold to ∼200  eV photon energy. Significant nondipole effects are seen even in the threshold region of this valence shell photoionization. In addition, contrary to previous understanding, clear evidence of interchannel coupling among quadrupole photoionization channels is found.

Photofragmentation Dynamics Of Core-Excited Water By Anion-Yield Spectroscopy, Wayne C. Stolte, M. M. Sant'anna, Gunnar Ohrwall, Maria Novella Piancastelli, I. Dominguez-Lopez, Dennis W. Lindle

Chemistry and Biochemistry Faculty Research

Partial-anion and- cation yields from H₂O are presented for photon energies near the oxygen K edge. The O^- yield exhibits a feature above threshold attributed to doubly excited states, in contrast to the H^- and cation yields, which are nearly featureless above threshold. Additionally, the lack of the OH^- fragment indicates radiative decay and provides a negligible amount of anion formation.

E1-E2 Interference In The Vuv Photoionization Of He, E. P. Kanter, B. Krassig, S. H. Southworth, Renaud Guillemin, Oliver Hemmers, Dennis W. Lindle, R. Wehlitz, M. Ya Amusia, L. V. Chernysheva, N. L. S. Martin

Environmental Studies Faculty Publications

We have measured the forward-backward asymmetry of photoelectron angular distributions produced in the vacuum ultraviolet photoionization of helium. This asymmetry, a consequence of the breakdown of the dipole approximation, measures the real part of the ratio of the quadrupole and dipole matrix elements. In the autoionization region, the strong energy dependence of the asymmetry permits an experimental separation of the ratio of those magnitudes from their phase difference. We experimentally determined the Fano parameters of the 2p²¹D₂ quadrupole resonance, and report improved values of the width Γ and line profile parameter q from those previously available …

Investigation Of The Corrosion Of Steel By Lead-Bismuth Eutectic (Lbe) Using Scanning Electron Microscopy And X-Ray Photoelectron Spectroscopy, Daniel Koury

UNLV Theses, Dissertations, Professional Papers, and Capstones

Lead Bismuth Eutectic (LBE) has been proposed for use in programs for accelerator transmutation of waste. LBE is the leading candidate material as a spallation target and an option for the sub-critical blanket coolant. The corrosion of 316 and 316L stainless steels by LBE has been studied using UNLV's facilities for Scanning Electron Microscopy (SEM) and X-ray Photoelectron Spectroscopy (XPS). We have compared exposed and unexposed samples and studied the differences. Some amount of surface contamination is present on the samples and has been removed by ionbeam etching. The unexposed samples reveal typical stainless steel characteristics: a chromium oxide passivation …