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Jacek Wasik

Publications and source records attributed to Jacek Wasik.

3 recordsLinked to original sources

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

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

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