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Energetic radiation can cause dramatic changes in the physical and chemical properties of actinide materials, degrading their performance in fission-based energy systems. As advanced nuclear fuels and wasteforms are developed, fundamental understanding of the processes controlling radiation damage accumulation is necessary. Here we report oxidation state(More)
High-pressure and high-temperature phases show unusual physical and chemical properties, but they are often difficult to 'quench' to ambient conditions. Here, we present a new approach, using bombardment with very high-energy, heavy ions accelerated to relativistic velocities, to stabilize a high-pressure phase. In this case, Gd(2)Zr(2)O(7), pressurized in(More)
In many solids, heavy ions of high kinetic energy (MeV-GeV) produce long cylindrical damage trails with diameters of order 10 nm. Up to now, no information was available how solids cope with the simultaneous exposure to these energetic projectiles and to high pressure. We report the first experiments where relativistic uranium and gold ions from the SIS(More)
Tracks formed by swift-heavy ion irradiation, 2.2 GeV Au, of isometric Gd2Ti2O7 pyrochlore and orthorhombic Gd2TiO5 were modeled using the thermal-spike model combined with a molecular-dynamics simulation. The thermal-spike model was used to calculate the energy dissipation over time and space. Using the time, space, and energy profile generated from the(More)
Ab initio total-energy calculations and X-ray diffraction measurements have been combined to study the phase stability of zirconate pyrochlores (A(2)Zr(2)O(7); A = La, Nd and Sm) under pressures up to 50 GPa. Phase transformations to the defect-cotunnite structure are theoretically predicted at pressures of 22, 20 and 18 GPa, in excellent agreement with the(More)
There has been an increased focus on understanding the energetics of structures with unconventional ordering (for example, correlated disorder that is heterogeneous across different length scales). In particular, compounds with the isometric pyrochlore structure, A2B2O7, can adopt a disordered, isometric fluorite-type structure, (A, B)4O7, under extreme(More)
Bulk ZrO(2) polymorphs generally have an extremely high amorphization tolerance upon low energy ion and swift heavy ion irradiation in which ballistic interaction and ionization radiation dominate the ion-solid interaction, respectively. However, under very high-energy irradiation by 1.33 GeV U-238, nanocrystalline (40-50 nm) monoclinic ZrO(2) can be(More)
We report dramatically different behaviors between isostructural Gd2Ti2O7 and Gd2Zr2O7 pyrochlore at pressures up to 44 GPa, in which the substitution of Ti for Zr significantly increases structural stability. Upon release of pressure, the Gd2Ti2O7 becomes amorphous. In contrast, the high-pressure phase of Gd2Zr2O7 transforms to a disordered defect-fluorite(More)
Swift heavy-ion irradiations of a wide variety of materials have been used to modify and manipulate the properties of solids at the nanoscale. Recently, these high-energy irradiations have been successfully combined with high-pressure experiments. Based on results obtained for zircon (ZrSiO(4)), this paper introduces this new experimental approach involving(More)
Pressure-induced cation and anion disordering in La2Zr2O7 pyrochlore is quantitatively analyzed by Rietveld refinement of in situ x-ray diffraction patterns, Raman, and infrared measurements. An anomalous lattice expansion and obvious change of the pressure dependence of the vibrational modes occur at ∼10  GPa. The pressure-induced water incorporation in(More)