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A new understanding of the damage formation mechanisms in Si is developed and investigated over an extended range of ion energy, dose, and irradiation temperature. A simple model for dealing with ion-induced damage is proposed, which is shown to be applicable over the range of implantation conditions. In particular the concept of defect "excesses" will be discussed. An excess exists in the lattice when there is a local surplus of one particular type of defect, such as an interstitial, over its complimentary defect (i.e., a vacancy). Mechanisms for producing such excesses by implantation will be discussed. The basis of this model specifies that accumulation of stable lattice damage during implantation depends upon the excess defects and not the total number of defects. The excess defect model is validated by fundamental damage studies involving ion implantation over a range of conditions. Confirmation of the model is provided by comparing damage profiles after implantation with computer simulation results. It will be shown that transport of ions in matter (TRIM) can be used effectively to model the ion-induced damage profile, i.e. excess defect distributions, by a simple subtraction process in which the spatially correlated defects are removed, thereby simulating recombination. Classic defect studies illuminate defect interactions from concomitant implantation of high- and medium-energy Si+-self ions. Also, the predictive quality of the excess defect model was tested by applying the model to develop several experiments to engineer excess defect concentrations to substantially change the nature and distribution of the defects. Not only are the excess defects shown to play a dominant role in defect-related processing issues, but their manipulation is demonstrated to be a powerful tool in tailoring the implantation process to achieve design goals. Pre-amorphization and dual implantation of different energetic ions are two primary investigative tools used in this work. Various analyses, including XTEM, RBS/channeling, PAS, and SIMS, provided experimental verification of the excess defect model disseminated within this dissertation.

The evolution of electrical resistance as function of defect concentration is examined for the unipolar n-conducting oxides CdO, β-Ga 2 O 3 , In 2 O 3 , SnO 2 and ZnO in order to explore the predictions of the amphoteric defect model. Intrinsic defects are introduced by ion irradiation at cryogenic temperatures, and the resistance is measured in-situ by current–voltage sweeps as a function of irradiation dose. Temperature dependent Hall effect measurements are performed to determine the carrier concentration and mobility of the samples before and after irradiation. After the ultimate irradiation step, the Ga 2 O 3 and SnO2 samples have both turned highly resistive. In contrast, the In 2 O 3 and ZnO samples are ultimately found to be less resistive than prior to irradiation, however, they both show an increased resistance at intermediate doses. Based on thermodynamic defect charge state transitions computed by hybrid density functional theory, a model expanding on the current amphoteric defect model is proposed.

Fundamental understanding of the behaviour of nuclear fuel has been of great importance. Enhancing this knowledge not only by means of experimental observations, but also via multi-scale modelling is of current interest. The overall goal of this thesis is to understand the impact of atomic interactions on the nuclear fuel material properties. Two major topics are tackled in this thesis. The first topic deals with non-stoichiometry in uranium dioxide (UO2) to be addressed by empirical potential (EP) studies. The second fundamental question to be answered is the effect of the atomic fraction of americium (Am), neptunium (Np) containing uranium (U) and plutonium (Pu) mixed oxide (MOX) on the material properties.UO2 has been the reference fuel for the current fleet of nuclear reactors (Gen-II and Gen-III); it is also considered today by the Gen-IV International Forum for the first cores of the future generation of nuclear reactors on the roadmap towards minor actinide (MA) based fuel technology. The physical properties of UO2 highly depend on material stoichiometry. In particular, oxidation towards hyper stoichiometric UO2 – UO2+x – might be encountered at various stages of the nuclear fuel cycle if oxidative conditions are met; the impact of physical property changes upon stoichiometry should therefore be properly assessed to ensure safe and reliable operations. These physical properties are intimately linked to the arrangement of atomic defects in the crystalline structure. The first paper evaluates the evolution of defect concentration with environment parameters – oxygen partial pressure and temperature by means of a point defect model, with reaction energies being derived from EP based atomic scale simulations. Ultimately, results from the point defect model are discussed, and compared to experimental measurements of stoichiometry dependence on oxygen partial pressure and temperature. Such investigations will allow for future discussions about the solubility of different fission products and dopants in the UO2 matrix at EP level.While the first paper answers the central question regarding the dominating defects in non-stoichiometry in UO2, the focus of the second paper was on the EP prediction of the material properties, notably the lattice parameter of Am, Np containing U and Pu MOX as a function of atomic fractions.The configurational space of a complex U1-y-y’-y’’PuyAmy’Npy’’O2 system, was assessed via Metropolis-Monte Carlo techniques. From the predicted configuration, the relaxed lattice parameter of Am, Np bearing MOX fuel was investigated and compared with available literature data. As a result, a linear behaviour of the lattice parameter as a function of Am, Np content was observed, as expected for an ideal solid solution. These results will allow to support and increase current knowledge on Gen-IV fuel properties, such as melting temperature, for which preliminary results are presented in this thesis, and possibly thermal conductivity in the future. / Doctorat en Sciences de l'ingénieur et technologie / info:eu-repo/semantics/nonPublished