Analysis of the Structure of Heavy Ion Irradiated LaFeO3 Using Grazing Angle X-ray Absorption Spectroscopy.

Abstract

Crystalline ceramics are candidate materials for the immobilization of radionuclides, particularly transuranics (such as U, Pu, and Am), arising from the nuclear fuel cycle. Due to the α-decay of transuranics and the associated recoil of the parent nucleus, crystalline materials may eventually be rendered amorphous through changes to the crystal lattice caused by these recoil events. Previous work has shown irradiation of titanate-based ceramics to change the local cation environment significantly, particularly in the case of Ti which was shown to change from 6- to 5-fold coordination. Here, this work expands the Ti-based study to investigate the behavior in Fe-based materials, using LaFeO3 as an example material. Irradiation was simulated by heavy ion implantation of the bulk LaFeO3 ceramic, with the resulting amorphous layer characterized with grazing angle X-ray absorption spectroscopy (GA-XAS). Insights into the Fe speciation changes exhibited by the amorphized surface layer were provided through quantitative analysis, including pre-edge analysis, and modeling of the extended X-ray absorption fine structure (EXAFS), of the GA-XAS data.