Radiation-induced paramagnetic defects in natural kaolinites: Alpha dosimetry with ion beam irradiation

Abstract

Three types of paramagnetic radiation-induced defects (RID), namely A, A′ (Si-O−-centers) and B (Al-O−-Al center), had been identified in natural kaolinites by means of electron paramagnetic resonance spectroscopy. The A-center, stable at the scale of geological periods, was thought to be of particular relevance to quantify past transits of radionuclides in the geosphere. Alpha radiation being likely the main source of RID in kaolinite, the objective of this paper is to define the role of α-particles on the creation of RID and to test the use of A-centers for an α-dosimetry. Three kaolinites with different crystalline order and containing other clays as impurities were irradiated with He+ ion beams. The radiation dose range (0–750 MGy) was consistent with natural radioactivity in environments from the Earth's surface. Irradiation drastically enhanced the original signals due to RID. An important increase of concentration of the unstable B-center, partly due to unrealistic dose rate provided by accelerator ion beam, was observed from the lower doses. The most stable defects remained of the Atype all along experimental irradiations. The contribution of ancillary phyllosilicates to EPR spectra was negligible. The concentration of the three types of RID was related to radiation doses up to 30 MGy. Dosimetry growth curves for the A-centers exhibited variable efficiencies and saturation levels that were related to the structural order and the chemical purity of the kaolinites: the more ordered and purer the kaolinite, the higher the efficiency and the lower the saturation plateau. Moreover, these results are of geochemical significance: dosimetry based on A-centers could be directly used to quantify past migrations of radioelements in the geosphere, by determination of the naturally-cumulated doses (paleodose) of kaolinites.