First-principles study of defect behavior in irradiated uranium monocarbide

International audienceAb initio electron theory based on the projector-augmented-wave method in the generalized gradient approximation of the density functional theory is used for calculating formation and migration energies of point defects in uranium monocarbide (UC). The use of the Hubbard term to describe the 5f electrons of uranium is discussed on the basis of the density of states and cohesive energies. A formalism allowing the "raw" calculated energies to be normalized is proposed to take into account the compositional dependence of defective crystals. Such formation energies are then used to determine the population of predominant defects as a function of nonstoichiometry. We identify the most stable defects as uranium antisites and carbon vacancies for UC(1-x), and dimers C(2) for UC(1+ x). The most stable thermal defects are obtained, in turn, by formation of complex defects associating dimer C(2) and carbon vacancies whereas carbon Frenkel pairs and Schottky defects require larger formation energies. The migration energies are also calculated for different mechanisms, using as diffusion vectors both thermal vacancy sources and preexisting constitutional defects in the case of off-stoichiometric alloys. We compare the calculated diffusion paths with available experimental data proposed by Matzke [J. Less-Common Met. 121, 537 (1986)]