Search

International audience; The main purpose of this paper is to summarize our results obtained during research on the radiation behavior of oxides. The paper presents various methods of damage accumulation in irradiated oxides with the special emphasis on correlations between channeling, luminescence and Raman spectroscopy measurements as well as the possibility to obtain quantitative data on polycrystalline materials. The results are interpreted in terms of Multi Step Damage Accumulation model. Without pretending to give a full review of the current trends concerning these studies, we intend to present both a reflection about recent results and a few options for next investigations. This article can thus be regarded as the opening of a discussion on further directions of the research to be conducted on the topic of radiation damage formation in advanced materials for nuclear applications.

Microstructural changes in a set of commercial grade UO 2 fuel samples have been investigated using synchrotron based micro-focused X-ray fluorescence (μ-XRF) and X-ray diffraction (μ-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 −1 ). 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 μ-XRD patterns further allow the evaluation of the crystalline domain size and sub-grain formation at different locations of the irradiated UO 2 pellets.

Synchrotron-based microprobe x-ray absorption spectroscopy (XAS) has been used to study the local atomic structure of chromium in chromia-doped uranium dioxide (UO2) grains. The specimens investigated were a commercial grade chromia-doped UO2 fresh fuel pellet, and materials from a spent fuel pellet of the same batch, irradiated with an average burnup of ~40 MW d kg(-1). Uranium L3-edge and chromium K-edge XAS have been measured, and the structural environments of central uranium and chromium atoms have been elucidated. The Fourier transform of uranium L3-edge extended x-ray absorption fine structure shows two well-defined peaks of U-O and U-U bonds at average distances of 2.36 and 3.83 Å. Their coordination numbers are determined as 8 and 11, respectively. The chromium Fourier transform extended x-ray absorption fine structure of the pristine UO2 matrix shows similar structural features with the corresponding spectrum of the irradiated spent fuel, indicative of analogous chromium environments in the two samples studied. From the chromium XAS experimental data, detectable next neighbor atoms are oxygen and uranium of the cation-substituted UO2 lattice, and two distinct subshells of chromium and oxygen neighbors, possibly because of undissolved chromia particles present in the doped fuels. Curve-fitting analyses using theoretical amplitude and phase-shift functions of the closest Cr-O shell and calculations with ab initio computer code FEFF and atomic clusters generated from the chromium-dissolved UO2 structure have been carried out. There is a prominent reduction in the length of the adjacent Cr-O bond of about 0.3 Å in chromia-doped UO2 compared with the ideal U-O bond length in standard UO2 that would be expected because of the change in effective Coulomb interactions resulting from replacing U(4+) with Cr(3+) and their ionic size differences. The contraction of shortest Cr-U bond is ~0.1 Å relative to the U-U bond length in bulk UO2. The difference in the local chromium environment between fresh and irradiated UO2 is discussed based on the comparison of quantitative structural information obtained from the two chromia-doped fuel samples analyzed.