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Heavy ion implantation combined with grazing incidence X-ray absorption spectroscopy (GIXAS): A new methodology for the characterisation of radiation damage in nuclear ceramics

Published online by Cambridge University Press:  15 February 2011

Martin C. Stennett
Affiliation:
Immobilization Science Laboratory, Department of Engineering Materials, University of Sheffield, Sheffield, South Yorkshire, UK
Neil C. Hyatt
Affiliation:
Immobilization Science Laboratory, Department of Engineering Materials, University of Sheffield, Sheffield, South Yorkshire, UK
Daniel P. Reid
Affiliation:
Immobilization Science Laboratory, Department of Engineering Materials, University of Sheffield, Sheffield, South Yorkshire, UK
Ewan R. Maddrell
Affiliation:
National Nuclear Laboratory, Sellafield, Cumbria, UK
Nianhua Peng
Affiliation:
Ion Beam Centre, University of Surrey, Guildford, Surrey, UK
Chris Jeynes
Affiliation:
Ion Beam Centre, University of Surrey, Guildford, Surrey, UK
Karen J. Kirkby
Affiliation:
Ion Beam Centre, University of Surrey, Guildford, Surrey, UK
Joseph C. Woicik
Affiliation:
National Synchrotron Light Source (NSLS), Brookhaven National Laboratory, New York, USA
Bruce Ravel
Affiliation:
National Synchrotron Light Source (NSLS), Brookhaven National Laboratory, New York, USA
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Abstract

An understanding of the effect of cumulative radiation damage on the integrity of ceramic wasteforms for plutonium and minor actinide disposition is key to the scientific case for safe disposal. Alpha recoil due to the decay of actinide species leads to the amorphisation of the initially crystalline host matrix, with potentially deleterious consequences such as macroscopic volume swelling and reduced resistance to aqueous dissolution. For the purpose of laboratory studies the effect of radiation damage can be simulated by various accelerated methodologies. The incorporation of short-lived actinide isotopes accurately reproduces damage arising from both alpha-particle and the heavy recoil nucleus, but requires access to specialist facilities. In contrast, fast ion implantation of inactive model ceramics effectively simulates the heavy recoil nucleus, leading to amorphisation of the host crystal lattice over very short time-scales. Although the resulting materials are easily handled, quantitative analysis of the resulting damaged surface layer has proved challenging.

In this investigation, we have developed an experimental methodology for characterisation of radiation damaged structures in candidate ceramics for actinide disposition. Our approach involves implantation of bulk ceramic samples with 2 MeV Kr+ ions, to simulate heavy atom recoil; combined with grazing incidence X-ray absorption spectroscopy (GI-XAS) to characterise only the damaged surface layer. Here we present experimental GI-XAS data acquired at the Ti and Zr K-edges of ion implanted zirconolite, as a function of grazing angle, demonstrating that this technique can be successfully applied to characterise only the amorphised surface layer. Comparison of our findings with data from metamict natural analogues provide evidence that heavy ion implantation reproduces the amorphous structure arising from naturally accumulated radiation damage.

Type
Research Article
Copyright
Copyright © Materials Research Society 2009

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Heavy ion implantation combined with grazing incidence X-ray absorption spectroscopy (GIXAS): A new methodology for the characterisation of radiation damage in nuclear ceramics
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Heavy ion implantation combined with grazing incidence X-ray absorption spectroscopy (GIXAS): A new methodology for the characterisation of radiation damage in nuclear ceramics
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