Ab initio energetics of some fission products (Kr, I, Cs, Sr and He) in uranium dioxide

A computational study of some fission products (FP) energetics in uranium dioxide is presented. Krypton, iodine, caesium, strontium and helium are considered. Calculations are made within the density functional theory in the local density approximation with the plane wave pseudopotential method. Three insertion sites are considered: the octahedral interstitial position and the oxygen and uranium substitution sites. The importance of atomic relaxations is estimated on the He and Kr cases. They prove quantitatively important but can be neglected to draw qualitative trends. For each fission product incorporation and solution energies are calculated. The obtained values of the solutions energies of the various FP are in good agreement with their experimental behaviour: Kr, Cs and I atoms are insoluble in uranium dioxide, Sr solubility depends on the stoichiometry of mania. He atoms are found to have little interaction with their environment in uranium doxide. (C) 2002 Elsevier Science B.V. All rights reserved.