Browsing by Author "Farnan, I"

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    Actinides in gology, energy, and the environment. Quantification of α-particle radiation damage in zircon.
    (GeoScienceWorld, 2014-10-01) Smye, KM; Brigden, C; Vance, ER; Farnan, I
    Analysis of radiation damage in natural mineral analogs such as zircon is important for the evaluation of the long-term behavior of nuclear waste forms and for geochronology. Here we present results of experiments to determine the partitioning of radiation damage due to the heavy nuclear recoil of uranium and thorium daughters and the α-particles ejected in an α-decay event in zircon. Synthetic polycrystalline zircon ceramics were doped with 10B and irradiated in a slow neutron flux for 1, 10, and 28 days to achieve the reaction 10B + n → 7Li + α (+2.79 MeV), creating an α event without a heavy nuclear recoil. The 7Li atoms produced in the nuclear reaction were directly detected by NMR “spin-counting”, providing a precise measurement of the α-dose applied to each sample. The amount of damage (number fraction and volume fraction) created by each α-event (one α-event being a 7Li + α-particle) has been quantified using radiological nuclear magnetic resonance and X-ray diffraction data. The number of permanently displaced atoms in the amorphous fraction was determined by 29Si NMR to be 252 ± 24 atoms for the 10B(n,α) event when the heavy recoil is absent, which is broadly in agreement with ballistic Monte Carlo calculations. The unit-cell swelling of the crystalline fraction, determined by X-ray diffraction, is small and anisotropic. The anisotropy is similar to that observed in ancient natural samples and implies an initial anisotropic swelling mechanism rather than an anisotropic recovery mechanism occurring over geological timescales. The small unit-cell volume swelling is only ~6% of the expansion frequently attributed to α-particles associated with an actinide α-decay event. The lattice parameters indicate a volume increase as α function of a dose of 0.21 A3/1018 α-events/g, which is significantly less than the increase of 3.55 A3/1018 α-events/g seen in Pu-doped zircon and 2.18 A3/1018 α-events/g seen in natural zircon. It is concluded that the heavy recoil plays a more important role in unit-cell swelling than previously predicted. The likely mechanism for such an effect is the rapid, and thus defect-rich, recrystallization of material initially displaced by the heavy recoil. © 2014, Mineralogical Society of America.
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    Positron annihilation lifetime study of radiation-damaged natural zircons
    (Elsevier B.V., 2016-04-01) Roberts, J; Gaugliardo, PR; Farnan, I; Zhang, M; Vance, ER; Davis, J; Karatchevtseva, I; Knott, RB; Mudie, ST; Buckman, J; Sullivan, JP
    Zircons are a well-known candidate waste form for actinides and their radiation damage behaviour has been widely studied by a range of techniques. In this study, well-characterised natural single crystal zircons have been studied using Positron Annihilation Lifetime Spectroscopy (PALS). In some, but not all, of the crystals that had incurred at least half of the alpha-event damage of ∼1019 α/g required to render them structurally amorphous, PALS spectra displayed long lifetimes corresponding to voids of ∼0.5 nm in diameter. The long lifetimes corresponded to expectations from published Small-Angle X-ray Scattering data on similar samples. However, the non-observation by PALS of such voids in some of the heavily damaged samples may reflect large size variations among the voids such that no singular size can be distinguished or. Characterisation of a range of samples was also performed using scanning electron microscopy, optical absorption spectroscopy, Raman scattering and X-ray scattering/diffraction, with the degree of alpha damage being inferred mainly from the Raman technique and X-ray diffraction. The observed void diameters and intensities of the long lifetime components were changed somewhat by annealing at 700 °C; annealing at 1200 °C removed the voids entirely. The voids themselves may derive from He gas bubbles or voids created by the inclusion of small quantities of organic and hydrous matter, notwithstanding the observation that no voidage was evidenced by PALS in two samples containing hydrous and organic matter. © 2016 Elsevier B.V.