Trapping of helium in nano-bubbles in euxenite: Positive identification and implications

Abstract

The (Y,REE,U,Th)–(Nb,Ta,Ti) oxides, like euxenite, fergusonite, pyrochlore, zirconolite, are known to contain nanometric spherical cavities or bubbles, interpreted to contain radiogenic helium. In-situ analyses by Scanning Transmission Electron Microscopy (STEM) coupled with Electron Energy Loss Spectroscopy (EELS) inside nano-bubbles from an euxenite crystal, sampled in its host c. 920 Ma old pegmatite in Norway, deliver, for the first time, a positive identification of helium and an estimation of helium pressure in such bubbles. The chemically unaltered euxenite crystal proves amorphous and homogeneously speckled with bubbles ranging from 5 to 68 nm in diameter, around a log-normal distribution centered at 19 nm. The euxenite contains 9.87 wt% UO2 and 3.15 wt% ThO2. It accumulated a theoretical alpha-decay dose of 3.46×1020 α/g (i.e. 170 He/nm3), at a dose rate of 11926 α/g/s. This corresponds to production of 0.23 wt% He. The density of helium inside the bubbles, estimated from EELS data, ranges from 2 to 45 He/nm3, leading to a pressure of 8 to 500 MPa. The proportion of produced helium trapped in bubbles is about 10%. Helium bubbles clearly influence helium diffusion. They may contribute to the swelling of euxenite during amorphization and to the fracturing of the host rock. Our results suggest that dose, dose rate and structural state seem to be important parameters for the nucleation, growth and coalescence of helium bubbles but also demonstrate the crucial need of experimental studies to be able to develop a predictive model of the long term behavior of materials in response to helium irradiation. Furthermore, chemical alteration of euxenite, here materialized by fluid driven dissolution–precipitation towards silica bearing euxenite, removes the bubbles and mobilizes helium into the rock via cracks and grain boundaries. It is then suggested that helium-rich fluid released from such U–Th rich sources may percolate into surrounding rock units, inducing perturbation of the (U–Th)/He systematics of apatite and zircon in these units.