Comprehensive characterization of irradiation induced defects in ceria: Impact of point defects on vibrational and optical properties

Chauhan, Vinay S.; Ferrigno, Joshua; Adnan, Saqeeb; Pakarinen, Janne; He, Lingfeng; Hurley, David H.; Khafizov, Marat

doi:10.1063/5.0099189

Title: Comprehensive characterization of irradiation induced defects in ceria: Impact of point defects on vibrational and optical properties

Journal Article · 24 August 2022 · Journal of Applied Physics

DOI: https://doi.org/10.1063/5.0099189 · OSTI ID:1883646

Chauhan, Vinay S.;

;

; Pakarinen, Janne;

; Hurley, David H.;

Validation of multiscale microstructure evolution models can be improved when standard microstructure characterization tools are coupled with methods sensitive to individual point defects. We demonstrate how electronic and vibrational properties of defects revealed by optical absorption and Raman spectroscopies can be used to compliment transmission electron microscopy (TEM) and x-ray diffraction (XRD) in the characterization of microstructure evolution in ceria under non-equilibrium conditions. Experimental manifestation of non-equilibrium conditions was realized by exposing cerium dioxide (CeO2) to energetic protons at elevated temperature. Two sintered polycrystalline CeO2 samples were bombarded with protons accelerated to a few MeVs. These irradiation conditions produced a microstructure with resolvable extended defects and a significant concentration of point defects. A rate theory (RT) model was parametrized using the results of TEM, XRD, and thermal conductivity measurements to infer point defect concentrations. An abundance of cerium sublattice defects suggested by the RT model is supported by Raman spectroscopy measurements, which show peak shift and broadening of the intrinsic T2g peak and emergence of new defect peaks. Additionally, spectroscopic ellipsometry measurements performed in lieu of optical absorption reveals the presence of Ce3+ ions associated with oxygen vacancies. This work lays the foundation for a coupled approach that considers a multimodal characterization of microstructures to guide and validate complex defect evolution models.

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Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI ID:: 1883646

Journal Information:: Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 8 Vol. 132; ISSN 0021-8979

Publisher:: American Institute of PhysicsCopyright Statement

Country of Publication:: United States

Language:: English

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