Influence of Compositional Complexity on Amorphization Resistance of Swift Heavy Ion Irradiated Titanate Pyrochlores
Compositionally complex oxides have garnered attention recently for their potential technological applications in harsh environments such as thermal barrier coatings and nuclear waste forms. Therefore, their response to extreme conditions, including high temperature and intense irradiation fields, must be thoroughly investigated. Here, the structural evolution of two pyrochlore oxides with comparable cation size ratio, <i>r</i><sub>A</sub>/<i>r</i><sub>B</sub>, (Yb<sub>0.2</sub>Er<sub>0.2</sub>Dy<sub>0.2</sub>Tb<sub>0.2</sub>Gd<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> and Ho<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>, was evaluated after irradiation with 946 MeV Au ions up to a fluence of 8 × 10<sup>12</sup> ions/cm<sup>2</sup> using synchrotron X-ray diffraction, transmission electron microscopy, and Raman spectroscopy. The overall radiation response is comparable for both titanate oxides and is dominated by a loss of crystallinity. When compared to a series of conventional titanate pyrochlore compositions, the amorphous track diameter of (Yb<sub>0.2</sub>Er<sub>0.2</sub>Dy<sub>0.2</sub>Tb<sub>0.2</sub>Gd<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> is slightly larger than that of Ho<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub> and more in line with the diameter of the endmember with the maximum A-site cation size (Gd<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>). Density functional theory calculations suggest that this behavior may be linked to local lattice distortions and the associated energetics of cation antisite formation. TEM and Raman analyses show that a disordered, crystalline shell surrounds the amorphous ion tracks in (Yb<sub>0.2</sub>Er<sub>0.2</sub>Dy<sub>0.2</sub>Tb<sub>0.2</sub>Gd<sub>0.2</sub>)<sub>2</sub>Ti<sub>2</sub>O<sub>7</sub>, and the corresponding short-range structure resembles a weberite-type atomic arrangement.
Authors
- Veerle Keppens (ORCID: https://orcid.org/0000-0002-2624-034X)
- Maik Lang (ORCID: https://orcid.org/0000-0002-3422-2459)
- George W. Adamson
- Katharine Lynn Page (ORCID: https://orcid.org/0000-0002-9071-3383)
- John Hirtz (ORCID: https://orcid.org/0000-0003-0025-6957)
- Cale Overstreet (ORCID: https://orcid.org/0000-0001-6595-3767)
- Changyong Park (ORCID: https://orcid.org/0000-0002-3363-5788)
- Haixuan Xu (ORCID: https://orcid.org/0000-0001-6460-6149)
- Eric C. O’Quinn (ORCID: https://orcid.org/0000-0001-7386-852X)
- Candice Kinsler-Fedon (ORCID: https://orcid.org/0000-0002-8592-7520)
- P. Simon (ORCID: https://orcid.org/0000-0003-2575-3730)
- Xing Wang (ORCID: https://orcid.org/0000-0001-7190-3889)
- Tao Liang (ORCID: https://orcid.org/0000-0002-7479-4531)
Institutions
- Argonne National Laboratory (US)
- Oak Ridge National Laboratory (US)
- Pennsylvania State University (US)
- GSI Helmholtz Centre for Heavy Ion Research (DE)
- X-ray Instrumentation Associates (United States) (US)
- University of Tennessee at Knoxville (US)
Publication Details
- Journal
- Inorganic Chemistry
- Published
- 2025-12-18
- DOI
- https://doi.org/10.1021/acs.inorgchem.5c04254
- Primary Topic
- Nuclear materials and radiation effects
- Type
- article
- Field-Weighted Citation Impact
- 0.00