Infrared-active phonon modes in single-crystal thorium dioxide and uranium dioxideShow others and affiliations
2020 (English)In: Journal of Applied Physics, ISSN 0021-8979, E-ISSN 1089-7550, Vol. 127, no 12, article id 125103Article in journal (Refereed) Published
Abstract [en]
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 pairs 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 pairs 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. Published under license by AIP Publishing.
Place, publisher, year, edition, pages
AMER INST PHYSICS , 2020. Vol. 127, no 12, article id 125103
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:liu:diva-165050DOI: 10.1063/1.5143724ISI: 000521989000001OAI: oai:DiVA.org:liu-165050DiVA, id: diva2:1423120
Note
Funding Agencies|National Science Foundation (NSF)National Science Foundation (NSF) [DMR 1420645, DMR 1808715]; Air Force Office of Scientific Research (AFOSR)United States Department of DefenseAir Force Office of Scientific Research (AFOSR) [FA9550-18-1-0360]; Defense Threat Reduction AgencyUnited States Department of DefenseDefense Threat Reduction Agency [HDTRA1-14-1-0041]; Domestic Nuclear Detection Office of the Department of Homeland SecurityUnited States Department of Homeland Security (DHS) [HSHQDC14X00089]; Center for Thermal Energy Transport under Irradiation, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy SciencesUnited States Department of Energy (DOE); J. A. Woollam Foundation; Nebraska Research Initiative
2020-04-142020-04-142020-04-14