Publications

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Metal hydrides can store hydrogen isotopes with high volumetric density. In metal tritides, tritium beta decay can result in accumulation of helium within the solid, in some cases exceeding 10 at.% helium after only 4 years of aging. Helium is insoluble in most materials, but often does not readily escape, and instead coalesces to form nanoscale bubbles when helium concentrations are near 1 at.%. Blistering or spallation often occurs at higher concentrations. Radioactive particles shed during this process present a potential safety hazard. This study investigates the effects of high helium concentrations on erbium deuteride (ErD₂), a non-radioactive surrogate material for erbium tritide (ErT₂). To simulate tritium decay in the surrogate, high doses of 120 keV helium ions were implanted into ErD₂ films at room temperature. Scanning and transmission electron microscopy indicated spherical helium bubble formation at a critical concentration of 1.5 at.% and bubble linkage leading to nanoscale crack formation at a concentration of 7.5 at.%. Additionally, crack propagation occurred through the nanocrack region, resulting in spallation extending from the implantation peak to the surface. Electron energy loss spectroscopy was utilized to confirm the presence of high-pressure helium in the nanocracks, suggesting that helium gas plays a predominant role in deformation. This work improves the overall understanding of helium behavior in ErD₂ by using modern characterization techniques to determine: the critical helium concentration required for bubble formation, the material failure mechanism at high concentration, and the nanoscale mechanisms responsible for material failure in helium implanted ErD₂.

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This report documents work done at the Sandia Ion Beam Laboratory to develop a capability to produce 14 Me neutrons at levels sufficient for testing radiation effects on electronic materials and components. The work was primarily enabled by a laboratory directed research and development (LDRD) project. The main elements of the work were to optimize target lifetime, test a new thin- film target design concept to reduce tritium usage, design and construct a new target chamber and beamline optimized for high-flux tests, and conduct tests of effects on electronic devices and components. These tasks were all successfully completed. The improvements in target performance and target chamber design have increased the flux and fluence of 14 MV neutrons available at the test location by several orders of magnitude. The outcome of the project is that a new capability for testing radiation-effects on electronic components from 14 MeV neutrons is now available at Sandia National Laboratories. This capability has already been extensively used for many qualification and component evaluation and development tests.

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Understanding the stability of the zircaloy-4 liner, which is used in the Tritium- Producing Burnable Absorber Rod, is important for predicting the maximium reasonable life time and failure mechanisms of this essential component for tritium production. In this year-long study, a combination of in-situ ion irradiation transmission electron microscopy and thermal desorption measurements were used to explore the structural stability of Zr-4 as a function of sequential and concurrent displacement damage, helium implantation, and molecular deuterium implantation at the temperature of interest for reactor operation. Under the limited conditions explored, the liner alloy appeared to be relatively stable based on the direct TEM observation of the microstructure.

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First-principles calculations are used to characterize the bulk elastic properties of cubic and tetragonal phase metal dihydrides, MH2 {M = Sc, Y, Ti, Zr, Hf, lanthanides} to gain insight into the mechanical properties that govern the aging behavior of rare-earth di-tritides as the constituent 3H, tritium, decays into 3He. As tritium decays, helium is inserted in the lattice, the helium migrates and collects into bubbles, that then can ultimately create sufficient internal pressure to rupture the material. The elastic properties of the materials are needed to construct effective mesoscale models of the process of bubble growth and fracture. Dihydrides of the scandium column and most of the rareearths crystalize into a cubic phase, while dihydrides from the next column, Ti, Zr, and Hf, distort instead into the tetragonal phase, indicating incipient instabilities in the phase and potentially significant changes in elastic properties. We report the computed elastic properties of these dihydrides, and also investigate the off-stoichiometric phases as He or vacancies accumulate. As helium builds up in the cubic phase, the shear moduli greatly soften, converting to the tetragonal phase. Conversely, the tetragonal phases convert very quickly to cubic with the removal of H from the lattice, while the cubic phases show little change with removal of H. The source and magnitude of the numerical and physical uncertainties in the modeling are analyzed and quantified to establish the level of confidence that can be placed in the computational results, and this quantified confidence is used to justify using the results to augment and even supplant experimental measurements.

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Here we investigated the microstructural response of various Pd physically vapor deposited films and Er and ErD₂ samples prepared from neutron Tube targets to implanted He via in situ ion irradiation transmission electron microscopy and subsequent in situ annealing experiments. Small bubbles formed in both systems during implantation, but did not grow with increasing fluence or a short duration room temperature aging (weeks). Annealing produced large cavities with different densities in the two systems. The ErD₂ showed increased cavity nucleation compared to Er. The spherical bubbles formed from high fluence implantation and rapid annealing in both Er and ErD₂ cases differed from microstructures of naturally aged tritiated samples. Further work is still underway to determine the transition in bubble shape in the Er samples, as well as the mechanism for evolution in Pd films.

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Hydriding of metals can be routinely performed at high temperature in a rich hydrogen atmosphere. Prior to the hydrogen loading process, a thermal activation procedure is required to promote facile hydrogen sorption into the metal. Despite the wide spread utilization of this activation procedure, little is known about the chemical and electronic changes that occur during activation and how this thermal pretreatment leads to increased rates of hydrogen uptake. This study utilized variable kinetic energy X-ray photoelectron spectroscopy to interrogate the changes during in situ thermal annealing of erbium films, with results confirmed by time-of-flight secondary ion mass spectrometry and low energy ion scattering. Activation can be identified by a large increase in photoemission between the valence band edge and the Fermi level and appears to occur over a two stage process. The first stage involves desorption of contaminants and recrystallization of the oxide, initially impeding hydrogen loading. Further heating overcomes the first stage and leads to degradation of the passive surface oxide leading to a bulk film more accessible for hydrogen loading. © 2011 American Institute of Physics.

Erbium is known to effectively load with hydrogen when held at high temperature in a hydrogen atmosphere. To make the storage of hydrogen kinetically feasible, a thermal activation step is required. Activation is a routine practice, but very little is known about the physical, chemical, and/or electronic processes that occur during Activation. This work presents in situ characterization of erbium Activation using variable energy photoelectron spectroscopy at various stages of the Activation process. Modification of the passive surface oxide plays a significant role in Activation. The chemical and electronic changes observed from core-level and valence band spectra will be discussed along with corroborating ion scattering spectroscopy measurements.

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In an effort to better understand the structural changes occurring during hydrogen loading of erbium target materials, we have performed in situ D{sub 2} loading of erbium metal (powder) at temperature (450 C) with simultaneous neutron diffraction analysis. This experiment tracked the conversion of Er metal to the {alpha} erbium deuteride (solid-solution) phase and then into the {beta} (fluorite) phase. Complete conversion to ErD{sub 2.0} was accomplished at 10 Torr D{sub 2} pressure with deuterium fully occupying the tetrahedral sites in the fluorite lattice.

Erbium is known to effectively load with hydrogen when held at high temperature in a hydrogen atmosphere. To make the storage of hydrogen kinetically feasible, a thermal activation step is required. Activation is a routine practice, but very little is known about the physical, chemical, and/or electronic processes that occur during Activation. This work presents in situ characterization of erbium Activation using variable energy photoelectron spectroscopy at various stages of the Activation process. Modification of the passive surface oxide plays a significant role in Activation. The chemical and electronic changes observed from core-level and valence band spectra will be discussed along with corroborating ion scattering spectroscopy measurements.

Erbium metal thin-films have been deposited on molybdenum-on-silicon substrates and then converted to erbium dideuteride (ErD2). Here, we study the effects of deposition temperature (≈300 or 723 K) and deposition rate (1 or 20 nm/s) upon the initial Er metal microstructure and subsequent ErD2 microstructure. We find that low deposition temperature and low deposition rate lead to small Er metal grain sizes, and high deposition temperature and deposition rate led to larger Er metal grain sizes, consistent with published models of metal thin-film growth. ErD2 grain sizes are strongly influenced by the prior-metal grain size, with small metal grains leading to large ErD2 grains. A novel sample preparation technique for electron backscatter diffraction of air-sensitive ErD2 was developed, and allowed the quantitative measurement of ErD2 grain size and crystallographic texture. Finer-grained ErD2 showed a strong (1 1 1) fiber texture, whereas larger grained ErD2 had only weak texture. We hypothesize that this inverse correlation may arise from improved hydrogen diffusion kinetics in the more defective fine-grained metal structure or due to improved nucleation in the textured large-grain Er. © 2010 Elsevier B.V. All rights reserved.

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Erbium metal thin-films have been deposited on molybdenum-on-silicon substrates and then converted to erbium dideuteride (ErD{sub 2}). Here, we study the effects of deposition temperature ({approx}300 or 723 K) and deposition rate (1 or 20 nm/s) upon the initial Er metal microstructure and subsequent ErD{sub 2} microstructure. We find that low deposition temperature and low deposition rate lead to small Er metal grain sizes, and high deposition temperature and deposition rate led to larger Er metal grain sizes, consistent with published models of metal thin-film growth. ErD{sub 2} grain sizes are strongly influenced by the prior-metal grain size, with small metal grains leading to large ErD{sub 2} grains. A novel sample preparation technique for electron backscatter diffraction of air-sensitive ErD{sub 2} was developed, and allowed the quantitative measurement of ErD{sub 2} grain size and crystallographic texture. Finer-grained ErD{sub 2} showed a strong (1 1 1) fiber texture, whereas larger grained ErD{sub 2} had only weak texture. We hypothesize that this inverse correlation may arise from improved hydrogen diffusion kinetics in the more defective fine-grained metal structure or due to improved nucleation in the textured large-grain Er.

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Erbium dihydride Er(H,D,T){sub 2} is a fluorite structure rare-earth dihydride useful for the storage of hydrogen isotopes in the solid state. However, thermodynamic predictions indicate that erbium oxide formation will proceed readily during processing, which may detrimentally contaminate Er(H,D,T){sub 2} films. In this work, transmission electron microscopy (TEM) techniques including energy-dispersive x-ray spectroscopy, energy-filtered TEM, selected area electron diffraction, and high-resolution TEM are used to examine the manifestation of oxygen contamination in ErD{sub 2} thin films. An oxide layer {approx}30-130 nm thick was found on top of the underlying ErD{sub 2} film, and showed a cube-on-cube epitaxial orientation to the underlying ErD{sub 2}. Electron diffraction confirmed the oxide layer to be Er{sub 2}O{sub 3}. While the majority of the film was observed to have the expected fluorite structure for ErD{sub 2}, secondary diffraction spots suggested the possibility of either nanoscale oxide inclusions or hydrogen ordering. In situ heating experiments combined with electron diffraction ruled out the possibility of hydrogen ordering, so epitaxial oxide nanoinclusions within the ErD{sub 2} matrix are hypothesized. TEM techniques were applied to examine this oxide nanoinclusion hypothesis.

X-ray powder diffraction data for ErH2-x Dx formed by hydrogen (i.e., protium)-deuterium loading of Er metal are reported. Lattice parameters for the varying hydrogen-deuterium compositions followed Vergard's law behavior. The cubic lattice parameter at room temperature for ErH2-x Dx obeys a linear relationship according to the formula a=5.1287-1.1120× 10-4 x, where a is the lattice parameter of the fluorite-type structure and x is the mole percent of deuterium. Microstrain measurements suggest a possible ordering of hydrogen and deuterium in the composition ErH1 D1. © 2008 International Centre for Diffraction Data.

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In an effort to better understand the structural changes occurring during hydrogen loading of erbium target materials, we have performed D{sub 2} loading of erbium metal (powder) with simultaneous neutron diffraction analysis. This experiment tracked the conversion of Er metal to the {alpha} erbium deuteride (solid-solution) phase and then on to the {beta} (fluorite) phase. Complete conversion to ErD{sub 2.0} was accomplished at 10 Torr D{sub 2} pressure with deuterium fully occupying the tetrahedral sites in the fluorite lattice. Increased D{sub 2} pressure (up to 500 Torr at 450 C) revealed {approx}10 % deuterium occupation of the octahedral sites. Subsequent vacuum pumping of the sample at 450 C removed octahedral site occupancy while maintaining tetrahedral deuterium occupancy, thereby yielding stoichiometric ErD{sub 2.0} {beta} phase.

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Sandia National Laboratories has cradle to grave responsibility for all neutron generators in the US nuclear weapons stockpile. As such, much research effort is exerted to develop a comprehensive understanding of all the major components of a neutron generator. One of the key components is the tritium containing target. The target is a thin metal tritide film. Sandia's research into metal tritides began in the early 1960's with a collaboration with the Denver Research Institute (DRI) and continues to this day with a major in house research effort. This document is an attempt to briefly summarize what is known about the aging of erbium tritide and to review the major publications conducted at Sandia in FY 07. First, a review of our knowledge of helium in erbium tritide will be presented. Second, executive summaries of the six major SAND reports regarding neutron tube targets published in FY07 by Department 2735, the Applied Science and Technology Maturation Department, and research partners are presented.

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Er(D,T){sub 2-x} {sup 3}He{sub x}, erbium di-tritide, films of thicknesses 500 nm, 400 nm, 300 nm, 200 nm, and 100 nm were grown and analyzed by Transmission Electron Microscopy, X-Ray Diffraction, and Ion Beam Analysis to determine variations in film microstructure as a function of film thickness and age, due to the time-dependent build-up of {sup 3}He in the film from the radioactive decay of tritium. Several interesting features were observed: One, the amount of helium released as a function of film thickness is relatively constant. This suggests that the helium is being released only from the near surface region and that the helium is not diffusing to the surface from the bulk of the film. Two, lenticular helium bubbles are observed as a result of the radioactive decay of tritium into {sup 3}He. These bubbles grow along the [111] crystallographic direction. Three, a helium bubble free zone, or 'denuded zone' is observed near the surface. The size of this region is independent of film thickness. Four, an analysis of secondary diffraction spots in the Transmission Electron Microscopy study indicate that small erbium oxide precipitates, 5-10 nm in size, exist throughout the film. Further, all of the films had large erbium oxide inclusions, in many cases these inclusions span the depth of the film.

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