In-Situ Monitoring of Microstructural Features in PuGa Alloys at Non-Ambient Conditions
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Publications and source records attributed to Smith, Alice Iulia.
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An in-situ high-pressure neutron diffraction experiment was conducted on a δ-phase stabilized plutonium alloy with isotope 242 Pu. Upon room-temperature compression, neither of the previously reported pressure-induced transformation paths, δ → α' or δ → γ’ → α', was observed up to 1.2 GPa. Instead, a drastic reduction in the diffraction intensity of the δ phase was observed when the pressure was above 0.8 GPa. At the highest pressure of the experiment (1.2 GPa), the diffraction data appear to be characteristic of an amorphous state, manifested by the diminishing intensities of all diffraction lines. Additionally, no evidence was found to support the transformation to a body-centered tetragonal structure (δ’), which was previously inferred from the diffraction line broadening during initial compression to 0.1 GPa. The discrepancies between the present and previous experiments suggest a substantial strain-induced stabilization of the δ-phase and is presumably attributed to the different stress states in the high-pressure environments. From the pressure - volume measurements, the determined isothermal bulk modulus for the δ-phase is in the range of 31.9 ± 1.3–34.8 ± 1.8 GPa using different pressure scales, comparable to those obtained from the resonant ultrasound spectroscopy measurements of the alloys of similar composition. Finally, the pressure-induced elastic softening is neither convinced in the present work, nor can it be resolved from the diffraction experiments if it is intrinsically weak.
The coating of nuclear fuel kernels with pyrolytic carbon (PyC) is a well-understood practice dating back over half a century. In spite of decades of studies related to these coatings, no study has yet investigated the effect of the PyC deposition coating process on the kernels themselves. In this study, the composition and crystallographic phase of kernel materials were observed to change after exposure to the thermal and chemical environment of PyC coating process. Specifically, the coating process increased the fraction of high carbon content phase within carbide microsphere kernels, with W 2 C containing microspheres driven towards WC, and UC containing microspheres driven towards UC 2 . Oxide microspheres consisted of a mixture of two crystalline phases. The monoclinic phase within yttria-stabilized zirconia microspheres was eliminated by the coating process resulting in a purely tetragonal phase. Hafnium oxide microspheres were more stable showing no detectable change in composition or crystal structure after coating.
Here, we report on observations of structural and chemical differences between samples of UBe 13 that were synthesised using two different methods. Unexplained discrepancies in properties between samples with differing synthesis had previously been found in this heavy fermion superconductor. A polycrystalline UBe 13 sample was made by arc-melting the constituents. Single crystals were grown using an aluminium flux and had a consistently slightly larger lattice parameter than the polycrystals, which merited further study. Neutron diffraction data were collected at the Lujan Center at LANSCE on the HIPPO diffractometer. Aluminium was detected by inductively coupled plasma mass spectrometry (ICP-MS) in the flux-grown single crystal (0.803 wt%), and small amounts (~0.2 wt%) of thorium were detected in the UBe 13 polycrystalline sample. In order to probe the implications of the presence of Al, calculations by spin-polarised DFT-GGA+U show that the incorporation of Al onto the 96i site (the lowest symmetry site in the structure) is energetically more favourable than on other sites. In general, the trends calculated by DFT for bond lengths and lattice parameter increases are consistent with bond lengths experimentally observed by neutron diffraction, but specific percentage changes with aluminium incorporation may be obscured by the unexpected thorium in the polycrystalline sample. The aggregate of our initial observations suggests that incorporation of aluminium from the flux into single crystal UBe 13 is significant.
This is a review of the Rigaku Smartlab project.
[Full Text] Plutonium metal is a highly unusual element, exhibiting six allotropes at ambient pressure, from room temperature to its melting point. Many phases of plutonium metal are unstable with temperature, pressure, chemical additions, and time. This strongly affects structure and properties, and becomes of high importance, particularly when considering effects on structural integrity over long time periods. The fcc δ-phase deserves additional attention, not only in the context of understanding the electronic structure of Pu, but also as one of the few high-symmetry actinide phases that can be stabilized down to ambient pressure and room temperature by alloying it with trivalent elements. We will present results on recent work on aging of Pu-2at.%Ga and Pu-7at.%Ga alloys
We report the formation of plutonium hydride in 2 at % Ga-stabilized δ-Pu, with 1 atomic % H charging. We show that magnetization measurements are a sensitive, quantitative measure of ferromagnetic plutonium hydride against the nonmagnetic background of plutonium. It was previously shown that at low hydrogen concentrations, hydrogen forms super-abundant vacancy complexes with plutonium, resulting in a bulk lattice contraction. Here we use magnetization, X-ray and neutron diffraction measurements to show that in addition to forming vacancy complexes, at least 30% of the H atoms bond with Pu to precipitate PuH x , largely on the surface of the sample with x ~ 1.9. We observe magnetic hysteresis loops below 40 K with magnetic remanence, consistent with precipitates of ferromagnetic PuH 1.9 .
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