Publications

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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.