Surface features on aged ²³⁸Pu-doped Eu-monazite

Several ²³⁸Pu-doped Eu monazite single crystals stored at ambient conditions are monitored for 15 years using Scanning and Transmission electron microscopy, spectroscopy, diffraction and optical microscopy. Despite preservation of high crystalline quality, mechanical cracking and formation of small flakes is observed. After several month of aging, a new phase appeared on surfaces of the crystals, which later formed a continuous shell of most crystallographic faces. Electron diffraction indicated that the shell consists of submicron Pu-containing rhabdophanes. Its formation likely occurs due to combined action of atmospheric moisture and recrystallisation of radiation damage in monazite domains adjacent to external and internal surfaces. Extent of the rhabdophane formation appears to be influenced by crystallography and Pu content of corresponding growth sectors of the parent monazite. Whereas macroscopic rhabdophanes and monazites are relatively stable against irradiation, formation of sub-microscopic particles is a point of concern for development of monazite-based ceramic forms for actinide immobilization.