Exfoliation and diffusion following helium ion implantation in fluorapatite: implications for radiochronology and radioactive waste disposal

The properties of fluorapatite, both a useful radiochronometer and a potential storage matrix specific for minor actinides produced by the reprocessing of spent nuclear fuel, have been investigated with emphasis to its response to alpha decay. Exfoliation, which occurs after implantation of high doses of 1.6-MeV He-ions (> 1.4 x 10(17) ions cm(-2), corresponding to 5% atomic proportion), could set an upper limit to the concentration of imbedded actinides (about 2 atoms % corresponding to 20 wt. %) or storage age unless significant diffusion of radiogenic He intervenes. This process has been studied by combining He implantation, thermal treatments in the temperature range 124-250 degrees C and measurement of the resulting He profile by an ion beam technique (ERDA) using 8.5-MeV C ions. The diffusion coefficient follows an Arrhenius' law with an activation energy of 120 (+/-2) KJ/mole and a frequency factor of 14.5 (+/-7) x 10(-3) cm(2) sec(-1) in agreement with literature data. The inferred closure temperature which validates the U,Th-He radiochronological method also fits previous values: 97 (+/-10)degrees C for grain size 165 mu m. With respect to radwaste disposal. He volume diffusion is too small to exclude the occurrence of exfoliation unless diffusion at grain boundary is much higher and a fine-grain matrix is deliberately chosen. (C) 1998 Elsevier Science Ltd. All rights reserved.