Diffusion of helium in the perfect and non perfect uranium dioxide crystals and their local structures

Local nano structures and their changes relevant with the diffusion of helium was determined by applying the density functional theory (DFT). With its help we calculated deformation of the crystal lattice while wandering helium atoms between octahedral sites. The optimal mutual coordinates of the atoms were determined by minimizing the Hellman-Feyman forces, allowing at the same time precisely specify dynamic height and the shape of the potential barrier. For a crystal containing single oxygen or uranium vacancies, has been described both the deformation associated with the presence of vacancy, as well as additional deformation related to the migration of the helium atom in the lattice. It was found that in the case of vacancies, the migration of helium atoms between the octahedral sites is not along a straight line but along a polyline. In addition, the presence of uranium vacancy causes that helium atoms in the octahedral sites, situated in the I and II coordination shell of uranium vacancy, have different energies. Migration between such positions must be carried out with the participation of the emission-absorption of phonons. Applying two site - model we evaluated the time for an over-barrier jump and diffusion of interstitial He. The obtained values for diffusion coefficient are compared with the experimentally obtained values and with the theoretical values of other authors.