PNNL

Abstract

The present paper reviews recent results on radiation resistance of lanthanum pyrozirconate obtained using empirical potentials molecular dynamic simulations. First, displacement cascades (DCs) with a 6 keV U4+ cation representing the a- recoil nucleus have been performed in the lanthanum pyrozirconate La2Zr2O7. Only point defects are observed after each DC. They represent on average only 10% of the total number of displaced atoms during the cascade, with two times more cation anti-sites than Frenkel pairs. These calculations indicate that amorphization does not occur by a direct impact mechanism in pyrozirconate. Second, consequences of point defects accumulation have been simulated by introducing different types – either cation anti-sites or Frenkel pairs – and concentrations of point defects in pyrochlore. Results show that cation Frenkel pairs accumulation is the driving force for lanthanum zirconate amorphization. Under cation Frenkel pair accumulation, the crystal transits first from the pyrochlore to the disordered fluorite structure, with the oxygen atoms simply rearranging around cations. Amorphization occurs as a second step. These results consequently provide atomic-level interpretation to experimental irradiation observations of a two-step phase transition.