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A transient liquid-like phase in the displacement cascades of zircon, hafnon and thorite

Nature volume 395, pages 56–58 (1998)Cite this article

Abstract

The study of radiation effects in solids is important for the development of ‘radiation-resistant’ materials for fission-reactor applications1. The effects of heavy-ion irradiation in the isostructural orthosilicates zircon (ZrSiO4), hafnon (HfSiO4) and thorite (ThSiO4) are particularly important because these minerals are under active investigation for use as a waste form for plutonium-239 resulting from the dismantling of nuclear weapons2,3,4. During ion irradiation, localized ‘cascades’ of displaced atoms can form as a result of ballistic collisions in the target material, and the temperature inside these regions may for a short time exceed the bulk melting temperature. Whether these cascades do indeed generate a localized liquid state5,6,7,8 has, however, remained unclear. Here we investigate the irradiation-induced decomposition of zircon and hafnon, and find evidence for formation of a liquid-like state in the displacement cascades. Our results explain the frequent occurrence of ZrO2 in natural amorphous zircon9,10,11,12. Moreover, we conclude that zircon-based nuclear waste forms should be maintained within strict temperature limits, to avoid potentially detrimental irradiation-induced amorphization or phase decomposition of the zircon.

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Figure 1: Critical amorphization dose as a function of temperature for zircon, hafnon and thorite.
Figure 2: Sequences of electron-diffraction patterns documenting the effects of ion irradiation at different temperatures.
Figure 3: High-resolution TEM image of zircon irradiated at 1,050 K (dose, 3 d.p.a.), showing randomly orientated ZrO2 nanocrystals (highlighted).

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Acknowledgements

This work was sponsored by the Division of Materials Sciences, Basic Energy Sciences, and the Environmental Management Sciences Program, US-DOE, with Lockheed Martin Energy Research Corporation.

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Authors and Affiliations

  1. Solid State Division, Oak Ridge National Laboratory, Oak Ridge, 37831-6057, Tennessee, USA

    A. Meldrum & L. A. Boatner

  2. Metals and Ceramics Division, Oak Ridge National Laboratory, Oak Ridge, 37831-6376, Tennessee, USA

    S. J. Zinkle

  3. Department of Nuclear Engineering and Radiological Sciences and the Department of Geological Sciences, The University of Michigan, Ann Arbor, 48109-2104, Michigan, USA

    R. C. Ewing

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  1. A. Meldrum
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Correspondence to A. Meldrum.

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Meldrum, A., Zinkle, S., Boatner, L. et al. A transient liquid-like phase in the displacement cascades of zircon, hafnon and thorite. Nature 395, 56–58 (1998). https://doi.org/10.1038/25698

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