Microstructure of 24-1928 Ma concordant monazites; implications for geochronology and nuclear waste deposits

The microstructure of monazite was studied using scanning electron microscopy (SEM), electron microprobe analysis (EMP), X-ray diffraction patterns (XRD), and transmission electron microscopy (TEM). Four well-characterized monazites were investigated, having very different concordant U-Pb ages (24 to 1928 Ma), and up to ∼15 wt.% ThO₂, and ∼0.94 wt. % UO₂. The SEM and EMP analyses of polished single crystal fragments reveal the absence of significant chemical zoning. XRD and TEM investigations show that the monazites are not metamict, despite their old ages, very high abundances of radionuclides, and hence, high time-integrated radiation doses. Except for the youngest one, the monazite crystals are composed of a mosaic of crystalline but slightly distorted domains. This structure is responsible for the presence of (1) mottled diffraction contrasts on the TEM, and (2) a second structural phase (B), with very broad reflections in the XRD patterns. Older monazites receive higher self-irradiation doses, and hence, they contain higher amounts of this B-phase. For the 1928 Ma monazite, XRD reveals only the broad reflections of phase B, implying that the whole monazite was affected by radiation damage that resulted in total distortion of the lattice. It is concluded that radiation damage in the form of amorphous domains does not accumulate in monazite because self-annealing heals the defects as they are produced by α-decay damage. The only memory of irradiation-induced defects is the presence of distorted domains. As the diffusion rate of Pb in an undisturbed monazite lattice is extremely low, Pb loss due to volume diffusion out of the monazite lattice is virtually impossible. This is considered as one reason why almost all monazites have concordant U-Th-Pb ages. Moreover, as long-term self-irradiation effects are limited in monazite, we consider this phase as a good candidate for the storage of high-level nuclear waste under the aspect of its high resistance to irradiation.