An integrated experimental and computational investigation of defect and microstructural effects on thermal transport in thorium dioxide

Dennett, Cody A.; Deskins, W. Ryan; Khafizov, Marat; Hua, Zilong; Khanolkar, Amey; Bawane, Kaustubh; Fu, Lyuwen; Mann, J. Matthew; Marianetti, Chris A.; Hurley, David H.; El–Azab, Anter

doi:10.1016/j.actamat.2021.116934

Cited by 33 publications

(42 citation statements)

References 79 publications

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“…Owing to their impact on optical permittivity, these defects are referred to as color centers. Figure 15(a) shows representative spectra for proton irradiated ThO2 exhibiting absorption peaks at 1.8 and 2.0 eV [132]. The location of these peaks matches previous reports on irradiated ThO2 [219,354].…”

Section: Optical Spectroscopysupporting

confidence: 83%

“…MTR has also been applied on a variety of materials following ion irradiation including silicon [583], sapphire [584], fuel cladding alloys [585], and a variety of oxide nuclear fuels and surrogates including UO2 [586], CeO2 [315], and ThO2 [29]. Recent work has focused on measurements of defect-bearing oxides at cryogenic temperatures in order to discriminate between phonon scattering resulting from multiple types of defects [132].…”

Section: Experimental Measurement Of Thermal Conductivitymentioning

confidence: 99%

“…Further measurements of the thermal conductivity in defected single crystal ThO2 were conducted on a subset of the crystals irradiated at 600˚C over a temperature range of 77 to 300 K using MTR (see Figure 34) [132]. These data provide a low-temperature comparison for BTE calculations of defect-affected thermal transport (similar to the 300K and higher BTE calculation of transport in Udoped ThO2 shown in Figure 29).…”

Section: Mixed Impact Of Point Defects and Loops In Tho2mentioning

confidence: 99%

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Thermal Energy Transport in Oxide Nuclear Fuel

et al. 2021

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To efficiently capture the energy of the nuclear bond, advanced nuclear reactor concepts seek solid fuels that must withstand unprecedented temperature and radiation extremes. In these advanced fuels, thermal energy transport under irradiation is directly related to reactor performance as well as reactor safety. The science of thermal transport in nuclear fuel is a grand challenge due to both computational and experimental complexities. Here, we provide a comprehensive review of thermal transport research on two actinide oxides: one currently in use in commercial nuclear reactors, uranium dioxide (UO2), and one advanced fuel candidate material, thorium dioxide (ThO2). In both materials, 5Concluding Remarks .

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Section: Optical Spectroscopysupporting

confidence: 83%

Section: Experimental Measurement Of Thermal Conductivitymentioning

confidence: 99%

Section: Mixed Impact Of Point Defects and Loops In Tho2mentioning

confidence: 99%

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Thermal Energy Transport in Oxide Nuclear Fuel

et al. 2021

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“…Our training data were obtained from DFT calculations carried out via a projector augmented-wave (PAW) method [45,46], as implemented in the Vienna ab initio simulation package (VASP) [47,48]. The strongly constrained and appropriately normed (SCAN) [49] functional was used as the exchange correlation functional, as it provides phonon dispersion and thermal conductivity estimates that show good agreement with experiments conducted on ThO 2 [15,43,50]. SCAN calculations employ PAW potentials generated using the Perdew, Burke, Ernzerhof generalized gradient approximation (GGA) functional [51].…”

Section: Training and Validationmentioning

confidence: 99%

“…While EIPs determine the atomic interactions in MD, effective methods are needed for parametrization of EIPs in order to improve the accuracy of their predictions of transport properties. One particular application of interest to this study is understanding the impact of irradiation-induced defects on the thermal transport of nuclear fuels [12][13][14][15]. Another important aspect of EIPs is their utilization in estimating the defect formation and migration energies necessary for understanding the evolution of microstructures under bombardment by energetic particles [14][15][16][17].…”

Section: Introductionmentioning

confidence: 99%

Improving empirical interatomic potentials for predicting thermophysical properties by using an irreducible derivatives approach: The case of thorium dioxide

Zhou¹,

Jiang²,

Xiao³

et al. 2022

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The accuracy of physical property predictions using classical molecular dynamics simulations is determined by the quality of the empirical interatomic potentials (EIPs). We introduce a training approach for EIPs, based on direct comparisons of the second-and third-order interatomic force constants (IFCs) between EIP and density functional theory (DFT) calculations. This work's unique aspect is the utilization of irreducible derivatives (IDs) of the total energy, which leverage on the symmetry of the crystalline structure and provide a minimal representation of the IFCs. Our approach is tailored toward accurate predictions of thermal conductivity, thus requiring knowledge of both harmonic and anharmonic IFCs by matching second-and third-order displacement derivatives, whereas second-order strain derivatives are needed for determining the elastic constants. We demonstrate this approach as an efficient and robust manner in which to train EIPs for predicting phonons and related properties, by optimizing parameters of an embedded-atom method potential for ThO2, which is used as a model system for fluorite oxides. Our ID-trained EIP provides thermophysical properties in great agreement with DFT, and outperforms previously widely utilized EIP for ThO2 in phonon dispersion and thermal conductivity calculations. It also provides reasonable estimates of thermal expansion and the formation energies of simple defects.

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