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Thermal conductivity suppression in uranium-doped thorium dioxide due to phonon resonant scattering

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arxiv 2303.01659 v1 pith:GQYOOGTX submitted 2023-03-03 cond-mat.mtrl-sci cond-mat.str-el

classification cond-mat.mtrl-scicond-mat.str-el
keywords thermalconductivitydopingscatteringlevelsphononresonantthoria
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abstract

In this work, the thermal transport properties of thorium dioxide (ThO$_2$, thoria) with low levels of substitutional uranium (U) doping are explored. We observe strong indications of resonant phonon scattering, an interaction between phonons and electronic degrees of freedom, induced by this doping in addition to common ``impurity'' scattering due to mass and interatomic force constant differences. Uranium doping levels of 6\%, 9\%, and 16\% were studied in a single hydrothermally synthesized U-doped thoria crystal with spatially-varying U doping levels. Within this crystal, isoconcentration regions with relatively uniform doping were located for local thermal conductivity measurements using a thermoreflectance technique. The measured thermal conductivity profiles in the temperature range of 77--300~K are compared to predictions of an analytical Klemens-Callaway thermal conductivity model to identify impacts from different phonon scattering mechanisms. Highly suppressed thermal conductivity at cryogenic temperatures at these doping levels suggests that phonon resonant scattering plays an important role in thermal conductivity reduction in U-doped thoria.

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  1. Experimental Confirmation of First-Principles Thermal Conductivity in Zirconium-Doped ThO$_2$

    cond-mat.mtrl-sci 2024-12 conditional novelty 5.0 of 10

    Measurement of Zr-doped ThO2 thermal conductivity from 77 to 300 K confirms a first-principles Green's function prediction between 100 and 300 K.

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