Document Type

Article

Publication Date

3-2020

Abstract

The infrared-active phonon modes, in single-crystal samples of thorium dioxide (ThO2) and uranium dioxide (UO2), were investigated using spectroscopic ellipsometry and compared with density functional theory. Both ThO2 and UO2 are found to have one infrared-active phonon mode pair [consisting of one transverse optic (TO) and one associated longitudinal optic (LO) mode], which is responsible for the dominant features in the ellipsometric data. At room temperature, our results for the mode pair’s resonant frequencies and broadening parameters are comparable with previous reflectance spectroscopy characterizations and density functional theory predictions. For ThO2, our ellipsometry and density function theory results both show that the LO mode broadening parameter is larger than the TO mode broadening. This signifies mode anharmonicity, which can be attributed to the intrinsic phonon–phonon interaction. In addition to the main mode pair, a broad low-amplitude impurity-like vibrational mode pair is detected within the reststrahlen band for both ThO2 and UO2. Elevated temperature measurements were performed for ThO2 in order to study the mechanisms by which the phonon parameters evolve with increased heat. The observed change in the TO resonant frequency is in excellent agreement with previous density functional calculations, which only consider volume expansion of the crystal lattice. This suggests that the temperature-dependent change in the TO frequency is primarily due to volume expansion. The change in the main mode pair’s broadening parameters is nearly linear within the temperature range of this study, which indicates the intrinsic anharmonic scattering (via cubic anharmonicities) as the main decay mechanism.

Comments

© 2020 Author(s).
This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in volume 127 of Journal of Applied Physics as cited below, and may be found at https://doi.org/10.1063/1.5143724.

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DOI

10.1063/1.5143724

Source Publication

Journal of Applied Physics

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