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Radiation damage from long-term alpha particle bombardment of silicates – a microfocus XRD and Fe K-edge XANES study

Published online by Cambridge University Press:  02 January 2018

W. R. Bower ,
C. I. Pearce ,
G. T. R. Droop ,
J. F. W. Mosselmans ,
K. Geraki  and
R. A. D. Pattrick
W. R. Bower*
Affiliation:
Research Centre for Radwaste Disposal and Williamson Research Centre, School of Earth, Atmospheric and Environmental Sciences, The University of Manchester M13 9PL, UK
C. I. Pearce
Affiliation:
Dalton Nuclear Institute & School of Chemistry, The University of Manchester M13 9PL, UK
G. T. R. Droop
Affiliation:
Research Centre for Radwaste Disposal and Williamson Research Centre, School of Earth, Atmospheric and Environmental Sciences, The University of Manchester M13 9PL, UK
J. F. W. Mosselmans
Affiliation:
Diamond Light Source, Harwell OX11 0QX, UK
K. Geraki
Affiliation:
Diamond Light Source, Harwell OX11 0QX, UK
R. A. D. Pattrick
Affiliation:
Research Centre for Radwaste Disposal and Williamson Research Centre, School of Earth, Atmospheric and Environmental Sciences, The University of Manchester M13 9PL, UK
*
*E-mail: william.bower@manchester.ac.uk
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Abstract

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A detailed understanding of the response of mineral phases to the radiation fields experienced in a geological disposal facility (GDF) is currently poorly constrained. Prolongued ion irradiation has the potential to affect both the physical integrity and oxidation state of materials and therefore may alter a structure's ability to react with radionuclides. Radiohalos (spheres of radiation damage in minerals surrounding radioactive (α-emitting) inclusions) provide useful analogues for studying long term α-particle damage accumulation. In this study, silicate minerals adjacent to Th- and U-rich monazite and zircon were probed for redox changes and long/short range disorder using microfocus X-ray absorption spectroscopy (XAS) and high resolution X-ray diffraction (XRD) at Beamline I18, Diamond Light Source. Fe3+ → Fe2+ reduction has been demonstrated in an amphibole sample containing structural OH– groups – a trend not observed in anhydrous phases such as garnet. Coincident with the findings of Pattrick et al. (2013), the radiolytic breakdown of OH– groups is postulated to liberate Fe3+ reducing electrons. Across all samples, high point defect densities and minor lattice aberrations are apparent adjacent to the radioactive inclusion, demonstrated by micro-XRD.

Keywords

radiation damagealpha particlesilicatesFe K-edgeXRDXANES
Type
Research Article
Information
Mineralogical Magazine , Volume 79 , Issue 6 , November 2015 , pp. 1455 - 1466
Creative Commons
Creative Common License - CCCreative Common License - BY
Copyright © The Mineralogical Society of Great Britain and Ireland 2015. This is an open access article, distributed under the terms of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2015

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