Dislocation Loops in Proton Irradiated Uranium-Nitrogen-Oxygen System (original) (raw)

2021, Journal of Nuclear Materials

In this study, we investigated the dislocation loop types formed in the proton-irradiated uraniumnitrogen-oxygen (U-NO) system, which involves uranium mononitride (UN), uranium sesquinitride (-U2N3), and uranium dioxide (UO2) phases. The dislocation loop formation is examined using specimens irradiated at 400°C and 710°C. Based on the detailed transmissionbased electron microscopy characterization with i) the morphology-based on-zone and ii) the invisibility-criterion based two-beam condition imaging techniques, only a single type of dislocation loop in each phase is found: a/2 110 , a/2 111 , or a/3 111 dislocation loops in UN,-U2N3, and UO2 phases, respectively. Molecular statics calculations for the formation energy of perfect and faulted dislocation loops in UN phases indicate a critical loop size of ~ 6 nm, above which perfect loops are energetically favorable. This could explain the absence of faulted loops in the experimental observation of the irradiated UN phase at two temperatures. This work will enhance the understanding of irradiation induced microstructural evolution for uranium nitrides as advanced nuclear fuels for the next-generation nuclear reactors.

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In situ TEM observation of dislocation evolution in Kr-irradiated UO2 single crystal

Journal of Nuclear Materials, 2013

In situ transmission electron microscopy (TEM) observation of UO 2 single crystal irradiated with Kr ions at high temperatures was conducted to understand the dislocation evolution due to high-energy radiation. The dislocation evolution in UO 2 single crystal is shown to occur as nucleation and growth of dislocation loops at low-irradiation doses, followed by transformation to extended dislocation segments and networks at high doses, as well as shrinkage and annihilation of some loops and dislocations due to high temperature annealing. Generally the trends of dislocation evolution in UO 2 were similar under Kr irradiation at different ion energies and temperatures (150 keV at 600°C and 1 MeV at 800°C) used in this work. Interstitial-type dislocation loops with Burgers vector along h1 1 0i were observed in the Kr-irradiated UO 2. The irradiated specimens were denuded of dislocation loops near the surface.

Irradiation effects and micro-structural changes in large grain uranium dioxide fuel investigated by micro-beam X-ray diffraction

Journal of Nuclear Materials, 2014

Microstructural changes in a set of commercial grade UO 2 fuel samples have been investigated using synchrotron based micro-focused X-ray fluorescence (l-XRF) and X-ray diffraction (l-XRD) techniques. The results are associated with conventional UO 2 materials and relatively larger grain chromia-doped UO 2 fuels, irradiated in a commercial light water reactor plant (average burn-up: 40 MW d kg À1). The lattice parameters of UO 2 in fresh and irradiated specimens have been measured and compared with theoretical predictions. In the pristine state, the doped fuel has a somewhat smaller lattice parameter than the standard UO 2 as a result of chromia doping. Increase in micro-strain and lattice parameter in irradiated materials is highlighted. All irradiated samples behave in a similar manner with UO 2 lattice expansion occurring upon irradiation, where any Cr induced effect seems insignificant and accumulated lattice defects prevail. Elastic strain energy densities in the irradiated fuels are also evaluated based on the UO 2 crystal lattice strain and non-uniform strain. The l-XRD patterns further allow the evaluation of the crystalline domain size and sub-grain formation at different locations of the irradiated UO 2 pellets.

Athermal dislocation strengthening in UO2

Journal of Nuclear Materials, 2020

Understanding the mechanical behavior of uranium dioxide (UO2) at hightemperature is of great interest to predict the behavior of the nuclear fuel under incidental operating conditions. Here, strengthening elementary processes and dislocation hardening coefficients are studied by the mean of Dislocation Dynamics (DD) simulations in UO2. The three slip modes of the fluorite structure i.e., ½<110>{100}, ½<110>{110} and ½<110>{111} are modelled and all the possible dislocation configurations are analyzed and discussed. Averaged hardening coefficients are derived and their sensitivity to the sample orientation is discussed in the light of the seminal experimental work of Sawbridge and Sykes. This DD study gives rise to new insights about UO2 mechanical behavior at high-temperature.

Structural modifications in uranium dioxide irradiated with swift heavy ions

Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, 1997

An extensive knowledge of radiation damage in nuclear fuel elements is of considerable importance for technological applications. Ion bombardment and ion-beam analysis techniques provide efficient tools in order to simulate and characterize the structural modifications induced by irradiation. This paper deals with the study of radiation effects induced in UO, single crystals irradiated with 340-MeV Xe ions which simulate high electronic excitations sensed by the nuclear fuel during the slowing-down of fission fragments. Radiation damage was characterized by the RBS-channeling techniques. Resonant scattering '60(4He,4He)'60 occurring at 3.045 MeV was applied to the study of oxygen sublattice modifications. A strong disordering of both U and 0 sublattices was observed, even at very low ion irradiation fluence (-1013 cme2).

Microstructure evolution in Xe-irradiated UO2 at room temperature

Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, 2014

In situ Transmission Electron Microscopy was conducted for single crystal UO 2 to understand the microstructure evolution during 300 keV Xe irradiation at room temperature. The dislocation microstructure evolution was shown to occur as nucleation and growth of dislocation loops at low irradiation doses, followed by transformation to extended dislocation segments and tangles at higher doses. Xe bubbles with dimensions of 1-2 nm were observed after room-temperature irradiation. Electron Energy Loss Spectroscopy indicated that UO 2 remained stoichiometric under room temperature Xe irradiation.

Impact of homogeneous strain on uranium vacancy diffusion in uranium dioxide

Physical Review B, 2015

We present a detailed mechanism of, and the effect of homogeneous strains on, the migration of uranium vacancies in UO2. Vacancy migration pathways and barriers are identified using density functional theory (DFT) and the effect of uniform strain fields are accounted for using the dipole tensor approach. We report complex migration pathways and non-cubic symmetry associated with the uranium vacancy in UO2 and show that these complexities need to be carefully accounted for to predict the correct diffusion behavior of uranium vacancies. We show that under homogeneous strain fields, only the dipole tensor of the saddle with respect to the minimum is required to correctly predict the change in the energy barrier between the strained and the unstrained case. Diffusivities are computed using kinetic Monte Carlo (KMC) simulations for both neutral and fully charged state of uranium single and di-vacancies. We calculate the effect of strain on migration barriers in the temperature range 800-1800 K for both vacancy types. Homogeneous strains as small as 2% have a considerable effect on diffusivity of both single and di-vacancies of uranium, with the effect of strain being more pronounced for single vacancies than di-vacancies. In contrast, the response of a given defect to strain is less sensitive to changes in the charge state of the defect. Further, strain leads to anisotropies in the mobility of the vacancy and the degree of anisotropy is very sensitive to the nature of the applied strain field for strain of equal magnitude. Our results suggest that the influence of strain on vacancy diffusivity will be significantly greater when single vacancies dominate the defect structure, such as sintering, while the effects will be much less substantial under irradiation conditions where di-vacancies dominate.

Energetics of intrinsic point defects in uranium dioxide from electronic-structure calculations

Journal of Nuclear Materials, 2009

The stability range of intrinsic point defects in uranium dioxide is determined as a function of temperature, oxygen partial pressure, and non-stoichiometry. The computational approach integrates high accuracy ab initio electronic-structure calculations and thermodynamic analysis supported by experimental data. In particular, the density functional theory calculations are performed at the level of the spin polarized, generalized gradient approximation and includes the Hubbard U term; as a result they predict the correct anti-ferromagnetic insulating ground state of uranium oxide. The thermodynamic calculations enable the effects of system temperature and partial pressure of oxygen on defect formation energy to be determined. The predicted equilibrium properties and defect formation energies for neutral defect complexes match trends in the experimental literature quite well. In contrast, the predicted values for charged complexes are lower than the measured values. The calculations predict that the formation of oxygen interstitials becomes increasingly difficult as higher temperatures and reducing conditions are approached.

Atomic-scale effects of chromium-doping on defect behaviour in uranium dioxide fuel

Journal of Nuclear Materials, 2017

The effects of doping conventional UO 2 fuel with chromium are studied through atomistic simulations using empirical force field methods. We first analyse the stable structures of unirradiated doped fuel by determining the preferred lattice configuration of chromium ions and oxygen vacancies within the matrix. In order to understand the physical effects of the dopants, we investigate the energy change upon inserting isolated defects and Frenkel pairs in the vicinity of chromium. The behaviour of point defects is then studied with collision cascade simulations and relaxation of doped simulation cells containing Frenkel pairs. The defective structures are analysed using an in-house tool named ASTRAM. Results indicate definite effects of chromium-doping on the ease with which defects are formed. Moreover, the extent of Cr effects on the residual damage following a displacement cascade is dependent on the dopant distribution and concentration in the fuel matrix.

Structures of Dislocation Loops in Some Ceramics Induced by Fast Neutron Irradiation

Journal of the Ceramic Society of Japan, 2003

HAEåw´qFHw¤C1528550 sÚaeåªR 2121 Fast neutron emitted from the ssion or fusion nuclear reactions induces various kinds of crystalline defects into ceramics. These defects can cause degradation of material properties. Dislocation loops are frequently formed in crystalline materials after high uence fast neutron irradiation. These structures have been ana lyzed based on highresolution electron microscopy and image simulations based on defects models. Local atomic congurations of interstitial loops formed in SiC, AlN and Si 3 N 4 are reviewed. These loops are com monly formed on the closest packing plane in each crystal, and more than one layer is arranged to form specic atomic congurations in spite of an extra thickness corresponding only one tetrahedral layer. Physi cal property changes of these materials are discussed based on the presence of these defects.

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