This review provides a comprehensive evaluation of the state-of-knowledge of radiation effects in crystalline ceramics that may be used for the immobilization of high-level nuclear waste and plutonium. The current understanding of radiation damage processes, defect generation, microstructure development, theoretical methods, and experimental methods are reviewed. Fundamental scientific and technological issues that offer opportunities for research are identified. The most important issue is the need for an understanding of the radiation-induced structural changes at the atomic, microscopic, and macroscopic levels, and the effect of these changes on the release rates of radionuclides during corrosion.

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This paper is a comprehensive review of the state-of-knowledge in the field of radiation effects in glasses that are to be used for the immobilization of high-level nuclear waste and plutonium disposition. The current status and issues in the area of radiation damage processes, defect generation, microstructure development, theoretical methods and experimental methods are reviewed. Questions of fundamental and technological interest that offer opportunities for research are identified.

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Zirconate and titanate pyrochlores were subjected to 1 MeV of Kr+ irradiation. Pyrochlores in the Gd2(ZrxTi1-x)2O7 system (x = 0, 0.25, 0.5, 0.75, 1) showed a systematic change in the susceptibility to radiation-induced amorphization with increasing Zr content. Gd2Ti2O7 amorphized at relatively low dose (0.2 displacement per atom at room temperature), and the critical temperature for amorphization was 1100 K. With increasing zirconium content, the pyrochlores became increasingly radiation resistant, as demonstrated by the increasing dose and decreasing critical temperature for amorphization. Pyrochlores highly-enriched in Zr (Gd2Zr2O7, Gd2Zr1.8Mg0.2O6.8, Gd1.9Sr0.1Zr1.9Mg0.1O6.85, and Gd1.9Sr0.1Zr1.8Mg0.2O6.75) could not be amorphized, even at temperature as low as 25 K.

A comprehensive understanding of radiation effects in zircon, ZrSiO4, over a broad range of time scales (0.5 h to 570 million years) has been obtained by a study of natural zircon, Pu-doped zircon, and ion-beam irradiated zircon. Radiation damage in zircon results in the simultaneous accumulation of both point defects and amorphous regions. The amorphization process is consistent with models based on the multiple overlap of particle tracks, suggesting that amorphization occurs as a result of a critical defect concentration. The amorphization dose increases with temperature in two stages (below 300 K and above 473 K) and is nearly independent of the damage source (α-decay events or heavy-ion beams) at 300 K. Recrystallization of completely amorphous zircon occurs above 1300 K and is a two-step process that involves the initial formation of pseudo-cubic ZrO2.

The disposition of actinides, most recently 239 Pu from dismantled nuclear weapons, requires effective containment of waste generated by the nuclear fuel cycle. Because actinides (e.g., 239 Pu and 237 Np) are long-lived, they have a major impact on risk assessments of geologic repositories. Thus, demonstrable, long-term chemical and mechanical durability are essential properties of waste forms for the immobilization of actinides. Mineralogic and geologic studies provide excellent candidate phases for immobilization and a unique database that cannot be duplicated by a purely materials science approach. The ''mineralogic approach'' is illustrated by a discussion of zircon as a phase for the immobilization of excess weapons plutonium.

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