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

Holweck Type Mollecular Pump

The general design of a Holweck-type molecular pump is considered. The design consists of a stationary helical pumping groove cut inside a cylindrical bore and a closely fitting smooth cylindrical rotor spinning concentrically inside this housing. Approximate analytical expressions were obtained for the pumping speed and ultimate pressure ratio of this type pump. (J.R.D.

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

Spatial distribution and interaction of defects in spinel, based on optical studies of x-ray irradiation induced processes

Kinetic studies of optical center accumulation and decay, together with the growth and decay of radioluminescence (RL) in magnesium aluminate spinel MgAl{sub 2}O{sub 4}, were performed at room temperature. We observed two stages of defect accumulation during prolonged X-ray irradiation, as evidenced by changes in absorption bands at 3.78 and 4.15 eV related to antisite defects, and bands at 4.75 and 5.3 eV due to F-type centers. A correlation was found between optical absorption band growth and the intensities of RL bands at 4.86 and 5.02 eV, the latter of which originate: from electron-hole recombination processes. The rate of decay of absorption centers and RL intensities is dependent on time after X-ray irradiation. Also both decay rates could be described by a two-stage exponential law. Results are discussed using a model that includes tunneling and recombination of electron and hole centers on spatially correlated defects located at different distances from one another

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

Glass Ceramic Waste Forms for Combined CS+LN+TM Fission Products Waste Streams

In this study, glass ceramics were explored as an alternative waste form for glass, the current baseline, to be used for immobilizing alkaline/alkaline earth + lanthanide (CS+LN) or CS+LN+transition metal (TM) fission-product waste streams generated by a uranium extraction (UREX+) aqueous separations type process. Results from past work on a glass waste form for the combined CS+LN waste streams showed that as waste loading increased, large fractions of crystalline phases precipitated upon slow cooling.[1] The crystalline phases had no noticeable impact on the waste form performance by the 7-day product consistency test (PCT). These results point towards the development of a glass ceramic waste form for treating CS+LN or CS+LN+TM combined waste streams. Three main benefits for exploring glass ceramics are: (1) Glass ceramics offer increased solubility of troublesome components in crystalline phases as compared to glass, leading to increased waste loading; (2) The crystalline network formed in the glass ceramic results in higher heat tolerance than glass; and (3) These glass ceramics are designed to be processed by the same melter technology as the current baseline glass waste form. It will only require adding controlled canister cooling for crystallization into a glass ceramic waste form. Highly annealed waste form (essentially crack free) with up to 50X lower surface area than a typical High-Level Waste (HLW) glass canister. Lower surface area translates directly into increased durability. This was the first full year of exploring glass ceramics for the Option 1 and 2 combined waste stream options. This work has shown that dramatic increases in waste loading are achievable by designing a glass ceramic waste form as an alternative to glass. Table S1 shows the upper limits for heat, waste loading (based on solubility), and the decay time needed before treatment can occur for glass and glass ceramic waste forms. The improvements are significant for both combined waste stream options in terms of waste loading and/or decay time required before treatment. For Option 1, glass ceramics show an increase in waste loading of 15 mass % and reduction in decay time of 24 years. Decay times of {approx}50 years or longer are close to the expected age of the fuel that will be reprocessed when the modified open or closed fuel cycle is expected to be put into action. Option 2 shows a 2x to 2.5x increase in waste loading with decay times of only 45 years. Note that for Option 2 glass, the required decay time before treatment is only 35 years because of the waste loading limits related to the solubility of MoO{sub 3} in glass. If glass was evaluated for similar waste loadings as those achieved in Option 2 glass ceramics, the decay time would be significantly longer than 45 years. These glass ceramics are not optimized, but already they show the potential to dramatically reduce the amount of waste generated while still utilizing the proven processing technology used for glass production

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