Intrinsic point defects and volume swelling in ZrSiO4 under irradiation

The effects of high concentration of point defects in crystalline ZrSiO4 as originated by exposure to radiation, have been simulated using first principles density functional calculations. Structural relaxation and vibrational studies were performed for a catalogue of intrinsic point defects, with different charge states and concentrations. The experimental evidence of a large anisotropic volume swelling in natural and artificially irradiated samples is used to select the subset of defects that give similar lattice swelling for the concentrations studied, namely interstitials of O and Si, and the anti-site Zr(Si), Calculated vibrational spectra for the interstitials show additional evidence for the presence of high concentrations of some of these defects in irradiated zircon.Comment: 9 pages, 7 (color) figure

Predicting the radiation tolerance of oxides

We have used atomistic computer simulations and ion beam irradiations to examine radiation damage accumulation in multicomponent oxides, We have developed contour energy maps via computer simulations to predict the effects of oxide structure and chemical composition on radiation-induced atomic disorder, defect migration, and swelling. Ion irradiation damage experiments have been perfonned on, pyrochlore and fluorite-structured oxide ceramics to test the predictions from computer models

In situ observation of defect growth beyond the irradiated region in yttria-stabilized zirconia induced by 400 keV xenon ion-beam at -90 and 30{degrees}C

Single crystals of yttria-stabilized zirconia were irradiated with 400 keV Xe ion-beam at room temperature and minus 90 degrees centigrade. Defect growth was monitored in situ with Rutherford Backscattering and ion channeling techniques using a 2 MeV He ion beam

Prediction of Irradiation Spectrum Effects in Pyrochlores

The final publication is available at Springer via http://dx.doi.org/10.1007/s11837-014-1158-xThe formation energy of cation antisites in pyrochlores (A2B2O7) has been correlated with the susceptibility to amorphize under irradiation, and thus, density functional theory calculations of antisite energetics can provide insights into the radiation tolerance of pyrochlores. Here, we show that the formation energy of antisite pairs in titanate pyrochlores, as opposed to other families of pyrochlores (B = Zr, Hf, or Sn), exhibits a strong dependence on the separation distance between the antisites. Classical molecular dynamics simulations of collision cascades in Er2Ti2O7 show that the average separation of antisite pairs is a function of the primary knock-on atom energy that creates the collision cascades. Together, these results suggest that the radiation tolerance of titanate pyrochlores may be sensitive to the irradiation conditions and might be controllable via the appropriate selection of ion beam parameters

Ion irradiation damage in ilmenite at 100 K

A natural single crystal of ilmenite (FeTiO{sub 3}) was irradiated at 100 K with 200 keV Ar{sup 2+}. Rutherford backscattering spectroscopy and ion channeling with MeV He{sup +} ions were used to monitor damage accumulation in the surface region of the implanted crystal. At an irradiation fluence of 1 {times} 10{sup 15} Ar{sup 2+} cm{sup {minus}2}, considerable near-surface He{sup +} ion dechanneling was observed, to the extent that ion yield from a portion of the aligned crystal spectrum reached the yield level of a random spectrum. This observation suggests that the near-surface region of the crystal was amorphized by the implantation. Cross-sectional transmission electron microscopy and electron diffraction on this sample confirmed the presence of a 150 nm thick amorphous layer. These results are compared to similar investigations on geikielite (MgTiO{sub 3}) and spinel (MgAl{sub 2}O{sub 4}) to explore factors that may influence radiation damage response in oxides

Point-detect production and migration in plutonium metal at ambient conditions

Modeling thermodynamics and defect production in plutonium (Pu) metal and its alloys, has proven to be singularly difficult. The multiplicity of phases and the small changes in temperature, pressure, and/or stress that can induce phase changes lie at the heart of this difficulty, In terms of radiation damage, Pu metal represents a unique situation because of the large volume changes that accompany the phase changes. The most workable form of the metal is the fcc (6.) phase, which in practice the 6 phase is stabilized by addition of alloying elements such as Ga or AI. The thermodynamically stable phase at ambient conditions is the between monoclinic (a-) phase, which, however, is approximately 20 % lower in volume than the 6 phase. In stabilized Pu metal, there is an interplay between the natural swelling tendencies of fcc metals and the volume-contraction tendency of the underlying phase transformation to the thermodynamically stable phase. This study explores the point defect production and migration properties that are necessary to eventually model the long-term outcome of this interplay

The Path to Sustainable Nuclear Energy. Basic and Applied Research Opportunities for Advanced Fuel Cycles

The objective of this report is to identify new basic science that will be the foundation for advances in nuclear fuel-cycle technology in the near term, and for changing the nature of fuel cycles and of the nuclear energy industry in the long term. The goals are to enhance the development of nuclear energy, to maximize energy production in nuclear reactor parks, and to minimize radioactive wastes, other environmental impacts, and proliferation risks. The limitations of the once-through fuel cycle can be overcome by adopting a closed fuel cycle, in which the irradiated fuel is reprocessed and its components are separated into streams that are recycled into a reactor or disposed of in appropriate waste forms. The recycled fuel is irradiated in a reactor, where certain constituents are partially transmuted into heavier isotopes via neutron capture or into lighter isotopes via fission. Fast reactors are required to complete the transmutation of long-lived isotopes. Closed fuel cycles are encompassed by the Department of Energy?s Advanced Fuel Cycle Initiative (AFCI), to which basic scientific research can contribute. Two nuclear reactor system architectures can meet the AFCI objectives: a ?single-tier? system or a ?dual-tier? system. Both begin with light water reactors and incorporate fast reactors. The ?dual-tier? systems transmute some plutonium and neptunium in light water reactors and all remaining transuranic elements (TRUs) in a closed-cycle fast reactor. Basic science initiatives are needed in two broad areas: ? Near-term impacts that can enhance the development of either ?single-tier? or ?dual-tier? AFCI systems, primarily within the next 20 years, through basic research. Examples: Dissolution of spent fuel, separations of elements for TRU recycling and transmutation Design, synthesis, and testing of inert matrix nuclear fuels and non-oxide fuels Invention and development of accurate on-line monitoring systems for chemical and nuclear species in the nuclear fuel cycle Development of advanced tools for designing reactors with reduced margins and lower costs ? Long-term nuclear reactor development requires basic science breakthroughs: Understanding of materials behavior under extreme environmental conditions Creation of new, efficient, environmentally benign chemical separations methods Modeling and simulation to improve nuclear reaction cross-section data, design new materials and separation system, and propagate uncertainties within the fuel cycle Improvement of proliferation resistance by strengthening safeguards technologies and decreasing the attractiveness of nuclear materials A series of translational tools is proposed to advance the AFCI objectives and to bring the basic science concepts and processes promptly into the technological sphere. These tools have the potential to revolutionize the approach to nuclear engineering R&D by replacing lengthy experimental campaigns with a rigorous approach based on modeling, key fundamental experiments, and advanced simulations