arXiv subjects

Ross Springell

Publications and source records attributed to Ross Springell.

8 recordsLinked to original sources

arXiv2026

A Topotactic Phase Transition in the Uranium Oxide System

A topotactic phase transition involves the transformation of one crystalline solid to another, which may include the loss or gain of material, where the orientation of the parent crystal determines the orientation of the daughter. We set out an experimental approach, based on polyepitaxial thin film deposition, where the precise transformation mechanism in important physico-chemical processes can be revealed in brilliant detail. Here, we find a reversible topotactic transition from (001) cubic UO2 to a (130) orthorhombic U3O8 structure; a >35% expansion/contraction. This remarkable result solves a puzzle that has eluded researchers for decades, and presents a method for determining the mechanism of crystallographic transformation in many other compounds.

cond-mat.mtrl-sci↗

arXiv2026

Local Structure of Epitaxial Single Crystal UO$_{2+x}$ Thin Films

The influence of oxygen stoichiometry on the uranium local environment is explored in epitaxial single crystal uranium oxide thin films grown by DC magnetron sputtering. Through post-growth annealing, the stoichiometry of as-grown UO$_{2}$ films are tuned over an approximate stoichiometry range of $0.07 \leq x \leq 0.20$, estimated with X-ray photoelectron spectroscopy measurements of the U$-4f$ and O$-1s$ peaks. The local structure of the thin films are then probed using extended X-ray absorption fine structure measurements at the U $L_{3}$ absorption edge. We observe both the evolution of the U local environment of as a function of oxidation in UO$_{2+x}$, and that the near stoichiometric UO$_{2}$ film replicates the local structure of bulk UO$_{2}$ material standards well. The series of stoichiometrically varied samples highlights the non-trivial transitional behaviour of the UO$_{2+x}$ oxygen sublattice with increasing oxygen content in this stoichiometric regime, while also demonstrating the efficacy of this thin film synthesis route for actinide studies beyond their established use as idealised surfaces, which could be readily adapted for further stoichiometrically tailored material studies and UO$_{2+x}$ device fabrication.

cond-mat.mtrl-sci↗

arXiv2024

Polyepitaxial grain matching to study the oxidation of uranium dioxide

Although the principal physical behaviour of a material is inherently connected to its fundamental crystal structure, the behaviours observed in the real-world are often driven by the microstructure, which for many polycrystalline materials, equates to the size and shape of the constituent crystal grains. Here we highlight a cutting edge synthesis route to the controlled engineering of grain structures in thin films and the simplification of associated 3-dimensional problems to less complex 2D ones. This has been applied to the actinide ceramic, uranium dioxide, to replicate structures typical in nuclear fission fuel pellets, in order to investigate the oxidation and subsequent transformation of cubic UO$_{2}$ to orthorhombic U$_{3}$O$_{8}$. This article shows how this synthesis approach could be utilised to investigate a range of phenomena, affected by grain morphology, and highlights some unusual results in the oxidation behaviour of UO$_{2}$, regarding the phase transition to U$_{3}$O$_{8}$.

cond-mat.mtrl-sci↗

arXiv2024

Absence of Induced Ferromagnetism in Epitaxial Uranium Dioxide Thin Films

Recently, Sharma et al. [Adv. Sci. 9, 2203473 (2022)] claimed that thin films (around 20 nm) of UO2 deposited on perovskite substrates exhibit strongly enhanced paramagnetism (called induced ferromagnetism by the authors). Moments of up to 3 Bohr magneton/U atom were claimed in magnetic fields of 6 T. We have reproduced such films and, after characterisation, have examined them with X-ray circular magnetic dichroism (XMCD) at the uranium M edges, a technique that is element specific. We do not confirm the published results. We find a small increase, as compared to the bulk, in the magnetic susceptibility of UO2 in such films, but the magnetisation versus field curves, measured by XMCD, are linear with field and there is no indication of any ferromagnetism. The absence of any anomaly around 30 K (the antiferromagnetic ordering temperature of bulk UO2) in the XMCD signal suggests the films do not order magnetically.

cond-mat.mtrl-sci↗

arXiv2022

Structure and Phase Transitions of Metastable Hexagonal Uranium Thin Films

We report a simple technique for the synthesis of uniaxially textured, metastable hexagonal close-packed-like uranium thin films with thicknesses between 175-2800 \r{A}. The initial structure and texture of the layers have been studied via X-ray diffraction and reflectivity and the time-dependent transitions of the samples into various orientations of orthorhombic ${\alpha}$-U have been mapped by similar techniques. The final crystallographic orientations of each system and the timescales on which the transitions occur are found to depend on the lattice parameters of the original layer. The absence of the ${\alpha}$-U (001) orientation in the transition products suggests that the transitions in these layers are mediated by mechanisms other than the [110] transverse acoustic phonon mode previously suggested for the cubic ${\gamma}$-U(110) to hcp-U(00.1) to ${\alpha}$-U(001) displacive phase transition. Alternative transition pathways are discussed.

cond-mat.mtrl-sci↗

arXiv2021

A geometrical model to describe the alpha dose rates from particulates of UO$_2$ in water

A model investigating the role of geometry on the alpha dose rate of spent nuclear fuel has been developed. This novel approach utilises a new piecewise function to describe the probability of alpha escape as a function of particulate radius, decay range within the material, and position from the surface. The alpha dose rates were produced for particulates of radii 1 $\mu$m to 10 mm, showing considerable changes in the 1 $\mu$m to 50 $\mu$m range. Results indicate that for decreasing particulate sizes, approaching radii equal to or less than the range of the $\alpha$-particle within the fuel, there is a significant increase in the rate of energy emitted per unit mass of fuel material. The influence of geometry is more significant for smaller radii, showing clear differences in dose rate curves below 50 $\mu$m. These considerations are essential for any future accurate prediction of the dissolution rates and hydrogen gas release, driven by the radiolytic yields of particulate spent nuclear fuel.

nucl-th↗

arXiv2021

A mathematical model to describe the alpha dose rate from a UO2 surface

A model to determine the dose rate of a planar alpha-emitting surface, has been developed. The approach presented is a computationally efficient mathematical model using stopping range data from the Stopping Ranges of Ions in Matter (SRIM) software. The alpha dose rates as a function of distance from irradiated UO2 spent fuel surfaces were produced for bench-marking with previous modelling attempts. This method is able to replicate a Monte Carlo (MCNPX) study of an irradiated UO2 fuel surface within 0.6 % of the resulting total dose rate and displays a similar dose profile.

nucl-th↗

arXiv2015

Moderate Positive Spin Hall Angle in Uranium

We report measurements of spin pumping and the inverse spin Hall effect in Ni80Fe20/Uranium bilayers designed to study the efficiency of spin-charge interconversion in a super-heavy element. We employ broad-band ferromagnetic resonance on extended films to inject a spin current from the Ni80Fe20 (permalloy) into the uranium layer, which is then converted into an electric field by the inverse spin Hall effect. Surprisingly, our results suggest a spin mixing conductance of order 2x10 e19 m-2 and a positive spin Hall angle of 0.004, which are both merely comparable to those of several transition metals. These results thus support the idea that the electronic configuration may be at least as important as the atomic number in governing spin pumping across interfaces and subsequent spin Hall effects. In fact, given that both the magnitude and the sign are unexpected based on trends in d-electron systems, materials with unfilled f-electron orbitals may hold additional exploration avenues for spin physics.

cond-mat.mes-hall↗