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Identifying and Quantifying Actinide Radiation Damage in Ceramics with Radiological Magic-Angle Spinning Nuclear Magnetic Resonance

Published online by Cambridge University Press:  26 February 2011

Ian Farnan ,
Herman Cho  and
William J. Weber
Ian Farnan
Affiliation:
ifarnan@esc.cam.ac.uk, University of Cambridge, Earth Sciences, Downing Street, Cambridge, CB3 9JA, United Kingdom, +44 1223 333431, +44 1223 333450
Herman Cho
Affiliation:
hm.cho@pnl.gov, Pacific Northwest National Laboratory, Richland, WA, 99352, United States
William J. Weber
Affiliation:
bill.weber@pnl.gov, Pacific Northwest National Laboratory, Richland, WA, 99352, United States
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Abstract

In the characterisation of amorphisation or local disordering due to actinide radiation damage, nuclear magnetic resonance (NMR) spectroscopy is attractive because it is element specific and equally sensitive to local structure in crystalline and amorphous materials. Here, we have applied high-resolution solid-state NMR spectroscopy (magic-angle spinning) to radiation damaged natural minerals containing 238U/232Th to determine the ‘number fraction’ of amorphous material (fa) through spin-counting techniques. In samples with a known alpha dose, the number of atoms displaced per alpha decay may be determined from an integration of the spectrum. A protocol for performing similar radiological magic-angle spinning experiments on plutonium containing ceramic samples with an activity of > 5 GBq isp described. Results obtained have allowed data from ancient, radiation damaged mineral samples of ZrSiO4 (238U/232Th) to be compared with modern 238/239Pu doped ceramic ZrSiO4 samples. The number of atomic displacements per alpha particle from 239Pu is similar to that for 238U/232Th (4980 ± 300/α). At lower ?-doses there are significant differences in the amorphous volume fraction (observed by density and x-ray diffraction) and the number fraction of displaced atoms (as measured by NMR) as a function of cumulative dose. These differences arise from local density considerations that manifest themselves in the local structure of the amorphous and crystalline phases. Using ab initio simulations of the damaged crystalline and amorphous regions, the magnetic response of these structures and hence the NMR shifts can be compared with experiment to reveal the nature of radiation induced changes occurring at the local scale.

Keywords

nuclear magnetic resonance (NMR)radiation effectsactinide
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 986: Symposium OO – Actinides 2006 – Basic Science, Applications and Technology , 2006 , 0986-OO10-04-MM10-04
Copyright
Copyright © Materials Research Society 2007

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