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Interfacial Cation Mixing and Microstructural Changes in Bilayer GTO/GZO Thin Films After Irradiation

  • Properties and Evolution of Defects and Interfaces
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Abstract

In many applications involving functional oxides, composite structures consisting of multiple oxides and interfaces between the two are of particular interest, as they provide enhanced properties over the individual phases. Often, materials intended for radioisotope immobilization are composite structures, consisting of multiple chemistries and structures. In this work, two pyrochlore materials, Gd\(_2\)Zr\(_2\)O\(_7\) (GZO) and Gd\(_2\)Ti\(_2\)O\(_7\) (GTO) are interfaced in a bilayer structure and irradiated to test the composite’s capacity to accommodate lattice point defects and the potential for cation transport across the interface. Using x-ray energy dispersive spectroscopy after the pristine bilayer was irradiated to damage levels of 0.2–0.8 dpa using a 12 MeV Cu\(^{4+}\) ion beam, significant cation intermixing was observed by the highest dose. While, as might be expected, the bulk of the GTO layer easily amorphized, surprisingly, the GZO layer also amorphized with arelatively small dose. More interestingly, the structure maintained a crystalline layer at the original interface between the two pyrochlores, even though the interface moved significantly during the irradiation. These results are explained through a physical model for ballistic mixing in pyrochlore. These results highlight the complex structural response of oxide heterostructures under extreme conditions.

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Acknowledgements

Research presented in this article was primarily supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under grant number LANLE4BU. B.K.D. also acknowledges the Laboratory Directed Research and Development program of Los Alamos National Laboratory under Project Number(s) 20210760PRD1, which supported the chemical analysis at the interface. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Los Alamos National Laboratory, an affirmative action equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy’s NNSA, under contract 89233218CNA000001.

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Authors and Affiliations

  1. Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    B. K. Derby, Y. Sharma, D. J. Williams & A. Chen

  2. Materials Science and Technology - 8, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    J. A. Valdez, M. Chancey, Y. Q. Wang, M. M. Schneider & B. P. Uberuaga

  3. Materials Physics and Applications - 11, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    E. L. Brosha & C. R. Kreller

  4. Materials Science and Technology Division - 16, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    M. T. Janish

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Derby, B.K., Sharma, Y., Valdez, J.A. et al. Interfacial Cation Mixing and Microstructural Changes in Bilayer GTO/GZO Thin Films After Irradiation. JOM 74, 4015–4025 (2022). https://doi.org/10.1007/s11837-022-05402-0

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