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Mitchell, Jeremy Neil

Publications and source records attributed to Mitchell, Jeremy Neil.

In Situ High-Temperature Raman Spectroscopy of UCl 3 : A Combined Experimental and Theoretical Study

Uranium trichloride (UCl 3 ) has received growing interest for its use in uranium-fueled molten salt reactors and in the pyrochemical processing of used fuel. In this paper, we report for the first time the experimentally determined Raman spectra of UCl 3 , at both ambient condition and in situ high temperatures up to 871 K. The frequencies of five of the Raman-active vibrational modes (v i ) of UCl 3 exhibit a negative temperature derivative ((∂ν i /∂T) P ) with increasing temperature. Here, this red-shift behavior is likely due to the elongation of U–Cl bonds. The average isobaric mode Grüneisen parameter (γ iP = 0.91 ± 0.02) of UCl 3 was determined through use of the coefficient of thermal expansion published in Vogel et al. (2021) and the (∂ νi /∂T) P values determined in this study. These results are in general agreement with those calculated here by density functional theory (DFT+U). Finally, a comparison of the ambient band positions of UCl 3 to those of isostructural lanthanide (La–Eu) and actinide chlorides (Am–Cf) has been made.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Defects and Mechanical Behavior of Plutonium [Slides]

Defects are important because they heavily influence material properties (e.g. strength, ductility, elasticity, conductivity, phase transformation temperatures (melting point), corrosion resistance, etc.). At LANL defects in plutonium are being characterized using many different methods (e.g. EXAFS, XRD, microscopy, RUS, DSC, dilatometry, density, etc.) My goal is to introduce a complimentary method of understanding defects in δ-Pu using the mechanical microscope concept. Using well-developed theories of first principles strengthening mechanisms (i.e. how defects influence strength) and carefully designed experiments, mechanical testing can compliment other defect characterization tools.

36 MATERIALS SCIENCE↗

Extended nuclear quadrupole resonance study of the heavy-fermion superconductor PuCoGa 5

PuCoGa 5 has emerged as a prototypical heavy-fermion superconductor, with its transition temperature (T c ≃ 18.5 K) being the highest amongst such materials. Nonetheless, a clear description as to what drives the superconducting pairing is still lacking, rendered complicated by the notoriously intricate nature of plutonium's 5f valence electrons. Here, we present a detailed 69,71 Ga nuclear quadrupole resonance (NQR) study of PuCoGa 5 , concentrating on the system's normal state properties near to T c and aiming to detect distinct signatures of possible pairing mechanisms. In particular, the quadrupole frequency and spin-lattice relaxation rate were measured for the two crystallographically inequivalent Ga sites and for both Ga isotopes, in the temperature range 1.6–300 K. No evidence of significant charge fluctuations is found from the NQR observables. On the contrary, the low-energy dynamics is dominated by anisotropic spin fluctuations with strong, nearly critical, in-plane character, which are effectively identical to the case of the sister compound PuCoIn 5 . Lastly, these findings are discussed within the context of different theoretical proposals for the unconventional pairing mechanism in heavy-fermion superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Heating-Cooling Asymmetry in the δ-γ Transformation in Plutonium: Clausius-Clapeyron Considerations

Slides discuss the subject under the following topics: Pu phase transformations and features of the γ-δ transformation (heating-cooling asymmetry, cooling rate, effect of impurities); pressure effects in γ-δ transformations; Clausius-Clapeyron analysis; and discussion of heating-cooling asymmetry in the γ-δ transformation. The following conclusions are reached: burst behavior and extended transformation range due to pressure arrest; low slope of P-T curve for γ-δ favors this transformation for pressure arrest; asymmetry w.r.t. direction of transformation likely due to defects.

36 MATERIALS SCIENCE↗

Superconductivity in plutonium compounds

Although the family of plutonium-based superconductors is relatively small, consisting of four compounds all of which crystallize in the tetragonal HoCoGa 5 structure, these materials serve as an important bridge between the known Ce- and U-based heavy fermion superconductors and the high-temperature cuprate superconductors. Additionally, the partial localization of 5f electrons that characterizes the novel electronic properties of elemental plutonium appears to be central to the relatively high superconducting transition temperatures that are observed in PuCoGa 5 , PuRhGa 5 , PuCoIn 5 , and PuRhIn 5 .

36 MATERIALS SCIENCE↗