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At least 37 records · Page 2

Phonon-Spin Scattering from Unpaired f-electrons in U atoms and It’s Influence on Thermal Transport in Uranium-doped Thorium Dioxide Single Crystals

In this work, impact of low level of uranium (U) atom substitution on thermal conductivity of thorium dioxide (ThO2) is investigated. ThO2 is an electronic insulator with a wide optical band-gap and no unpaired electrons whose thermal transport is governed by phonons. U-substitution introduces unpaired f-electrons resulting in paramagnetic behavior of U-ThO2 at room temperature, which significantly suppresses its thermal conductivity. A single crystal of U-ThO2 with graded composition of U is grown using a hydrothermal synthesis method, and thermal conductivity measurements are performed in regions with uniform composition of U at levels of 0%, 6%, 9% and 16%. Measured thermal conductivity profiles over 77–300 K temperature range are analyzed using an analytical expression for phonon-mediated thermal transport based on Klemens-Callaway model. Temperature dependent thermal conductivity is found to deviate significantly from the Rayleigh scattering trend expected for a simple substitutional point defect with a small perturbation to mass and interatomic forces. With the resonant scattering term, observed large suppression of thermal conductivity at low temperatures can be closely reproduced. Additionally, the extracted phonon-spin coupling constants imply a nonlinear relation of phonon-spin interaction intensity with respect to U doping percentage. Our study reveals how phonon-spin scattering contributed by unpaired f-electrons in U atoms influences thermal transport in the U-ThO2 system.

36 - MATERIALS SCIENCE

Thorium Bis‐Salophen Trimers as Anion Detectors and Binding Agents

Bis‐salophen ligands are the condensation product of a tetramine and a salicylaldehyde derivative. They feature two binding sites, both of which are tetradentate with mixed O/N donor atoms. Reaction with the ligand precursor and thorium nitrate tetrahydrate forms a 3:3 metal‐to‐ligand trimer with a ΔΔΔ‐chirality confirmed by X‐ray crystallography of a racemic single crystal. The structure has a pore in the center of the triangular structure measuring 6.22 Å at its narrowest point. This compound is air‐ and water‐stable as well as soluble in organic solvents. Here, this compound was screened with a series of tetrabutyl ammonium halide salts, and tetrabutylammonium (TBA) chloride showed the strongest binding to the complex. After the addition of 2 equivalents of TBACl, the complex and salt precipitate out of solution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Thermal conductivity suppression in uranium-doped thorium dioxide due to phonon-spin interactions

In this work, impact of low level of uranium (U) atom substitution on thermal conductivity of thorium dioxide (ThO 2 ) is investigated. ThO 2 is an electronic insulator with a wide optical band-gap and no unpaired electrons whose thermal transport is governed by phonons. U-substitution introduces unpaired f-electrons resulting in paramagnetic behavior of U-ThO 2 at room temperature, which significantly suppresses its thermal conductivity. A single crystal of U-ThO 2 with graded composition of U is grown using a hydrothermal synthesis method, and thermal conductivity measurements are performed in regions with uniform composition of U at levels of 0%, 6%, 9% and 16%. Measured thermal conductivity profiles over 77–300 K temperature range are analyzed using an analytical expression for phonon-mediated thermal transport based on Klemens-Callaway model. Temperature dependent thermal conductivity is found to deviate significantly from the Rayleigh scattering trend expected for a simple substitutional point defect with a small perturbation to mass and interatomic forces. With the resonant scattering term, observed large suppression of thermal conductivity at low temperatures can be closely reproduced. Additionally, the extracted phonon-spin coupling constants imply a nonlinear relation of phonon-spin interaction intensity with respect to U doping percentage. Our study reveals how phonon-spin scattering contributed by unpaired f-electrons in U atoms influences thermal transport in the U-ThO 2 system.

36 MATERIALS SCIENCE

Frequency reproducibility of solid-state thorium-229 nuclear clocks

Solid-state thorium-229 ( 229 Th) nuclear clocks are set to provide new opportunities for precision metrology and fundamental physics. Taking advantage of inherent low sensitivity of a nuclear transition to its environment, orders of magnitude more emitters can be hosted in a solid-state crystal compared with current optical lattice atomic clocks. Furthermore, solid-state systems needing only simple thermal control are key to the development of field-deployable compact clocks. Here we explore and characterize the frequency reproducibility of the 229 Th:CaF 2 nuclear clock transition, a key performance metric for all clocks. We measure the transition linewidth and centre frequency as a function of the doping concentration, temperature and time. We report the concentration-dependent inhomogeneous linewidth of the nuclear transition, limited by the intrinsic host crystal properties. We determine an optimal working temperature for the 229 Th:CaF 2 nuclear clock at 196(5) K, at which the first-order thermal sensitivity vanishes. This would enable in situ temperature co-sensing using different quadrupole-split lines, reducing the temperature-induced systematic shift below the 10 −18 fractional frequency uncertainty level. At 195 K, the reproducibility of the nuclear transition frequency is 220 Hz (fractionally 1.1 × 10 −13 ) for two differently doped 229 Th:CaF 2 crystals over 7 months. Furthermore, these results form the foundation for understanding, controlling and harnessing the coherent nuclear excitation of 229 Th in solid-state hosts and for their applications in constraining temporal variations of fundamental constants.

Atomic and molecular physics

Optical cycling on thorium monoxide for an improved test of fundamental symmetries

Optical cycling refers to repeated excitation and spontaneous emission on an electronic transition in an atom or molecule. Optical cycling in molecules can enable a wide range of quantum control and readout techniques, but unfortunately it has only been demonstrated on a small class of alkalilike or alkaline-earth-like molecules. Thorium monoxide (ThO), a molecule used in one of the most precise permanent electron electric dipole moment (eEDM) searches (ACME†) [Andreev et al., Nature (London) 562, 355 (2018)], does not fall into this category. In this work, we demonstrate the first optical cycling on this nonconventional class over a range of experimental parameter space, including laser intensity, polarization switching rate, and interaction time. We show that both the 𝐽 = 1 and 𝐽 = 2 rotational levels of ThO molecule are capable of cycling an average of 11(2) photons with a single laser, at scattering rates of 1.9⁢(6) × 10 6 and 2.3⁢(7) × 10 6 s −1 , respectively, before population is lost to other vibronic levels. We outline a scheme to apply this demonstrated optical cycling in an ACME-style eEDM measurement, improving the detection efficiency by over fourfold compared to noncycling fluorescence detection. This would lead to over a twofold enhancement in the statistical sensitivity of the eEDM search. This optical-cycling scheme can be further extended to scatter ∼100 photons, which would enable a wider range of quantum control and sensing using ThO molecules.

Atomic & molecular processes in external fields

The effect of yttrium and thorium on the oxidation behavior of Ni-Cr-Al alloys

The effect of quaternary additions of 0.5% Y, 0.5 and 1.0% Th to a base alloy of Ni-10CR-5Al on the oxidation behavior and mechanism was studied during oxidation in air over the range of 1000 to 1200 C. The presence of yttrium decreased the oxidation kinetics slightly, whereas, the addition of thorium caused a slight increase. Oxide scale adherence was markedly improved by the addition of the quaternary elements. Although a number of oxides formed on yttrium containing alloys, quantitative X-ray diffraction clearly showed that the rate-controlling step was the diffusion of aluminum through short circuit paths in a thin layer of alumina that formed parabolically with time. Although the scale adherence of the yttrium containing alloy was considerably better than the base alloys, spalling did occur that was attributed to the formation of the voluminous YAG particles which grew in a mushroom-like manner, lifting the protective scale off the subrate locally. The YAG particles formed primarily at grain boundaries in the substrate in which the yttrium originally existed as YNi9.

Kumar, A.

Tables for determining lead, uranium, and thorium isotope ages

Tables for determining lead, uranium, and thorium isotope ages are presented in the form of computer printouts. Decay constants, analytical expressions for the functions evaluated, and the precision of the calculations are briefly discussed.

Schonfeld, E.

The effect of yttrium and thorium on the oxidation behavior of Ni-Cr-Al alloys

The investigation reported included a determination of the optimum composition of a Ni-Cr-Al ternary alloy with respect to oxidation resistance and minimum film-spalling tendencies. Yttrium and thorium in small amounts were added to the ternary alloy and an investigation of the oxidation mechanism and the oxide scale adherence was conducted. It was found that the oxidation mechanism of Ni-Cr-Al ternary alloys depends upon the composition of the alloy as well as the time, oxygen pressure, and temperature of oxidation.

Kumar, A.

Thorium concentrations in the lunar surface. II - Deconvolution modeling and its application to the regions of Aristarchus and Mare Smythii

The broad angular response which characterized the Apollo gamma ray spectrometer resulted in a loss of spatial resolution and some of the contrast in determining surface concentrations within lunar regions small compared to the field of view. A deconvolution technique has been developed which removes much of this instrumental effect, thereby improving both spatial resolution and accuracy at the cost of a loss in precision. Geometric models of regional thorium distribution are convoluted through the response function of the instrument to yield a predicted distribution which is compared with the observed data field for quality of fit. Application to areas which include Aristarchus and Mare Smythii confirm some geological relationships and fail to support others.

Haines, E. L.

Thorium concentrations in the lunar surface. V - Deconvolution of the central highlands region

The distribution of thorium in the lunar central highlands measured from orbit by the Apollo 16 gamma-ray spectrometer is subjected to a deconvolution analysis to yield improved spatial resolution and contrast. Use of two overlapping data fields for complete coverage also provides a demonstration of the technique's ability to model concentrations several degrees beyond the data track. Deconvolution reveals an association between Th concentration and the Kant Plateau, Descartes Mountain and Cayley plains surface formations. The Kant Plateau and Descartes Mountains model with Th less than 1 part per million, which is typical of farside highlands but is infrequently seen over any other nearside highland portions of the Apollo 15 and 16 ground tracks. It is noted that, if the Cayley plains are the result of basin-forming impact ejecta, the distribution of Th concentration with longitude supports an origin from the Imbrium basin rather than the Nectaris or Orientale basins. Nectaris basin materials are found to have a Th concentration similar to that of the Descartes Mountains, evidence that the latter may have been emplaced as Nectaris basin impact deposits.

Metzger, A. E.

Helium on Venus - Implications for uranium and thorium

Helium is removed at an average rate of 10 to the 6th atoms per square centimeter per second from Venus's atmosphere by the solar wind following ionization above the plasmapause. The surface source of helium-4 on Venus is similar to that on earth, suggesting comparable abundances of crustal uranium and thorium.

Prather, M. J.

Mapping the Concentration of Iron, Titanium, and Thorium in Mare Basalts in the Western Procellarum Region of the Moon

Mare basalt flows in the Western Procellarum region (WPR) are extensive and include some of the youngest geologic features on the Moon. Compositional remote sensing by the Lunar Prospector gammaray spectrometer (LPGRS) indicates elevated Th concentrations in many of these flows relative to basalts sampled by the Apollo and Luna missions [1,2,3,4]. The primary goals of this investigation are to determine whether the Th enrichment in this region contributed to the extensive and prolonged volcanism in the WPR, and to determine whether the Th is inherent to the basalts themselves or a result of contamination from nonvolcanic material. Thorium enrichment indigenous to the basalts of the Western Procellarum Region would provide evidence that the general concentration of Th in the Procellarum region extends below the crust and possibly as deep as the sources for the basalts themselves.

Flor, E. L.

Revised Thorium Abundances for Lunar Red Spots

Lunar red spots are features on the nearside of the Moon that are characterized by high albedo and by a strong absorption in the ultraviolet. These red spots include the Gruithuisen domes, the Mairan domes, Hansteen Alpha, the southern portion of Montes Riphaeus, Darney Chi and Tau, Helmet, and an area near the Lassell crater. It has been suggested that many of the red spots are extrusive, nonmare, volcanic features that could be composed of an evolved lithlogy enriched in thorium. In fact, Hawke et al. used morphological characteristics to show that Hansteen Alpha is a nonmare volcanic construct. However, because the apparent Th abundances (6 - 7 ppm) were lower than that expected for evolved rock types, Hawke et al. concluded that Hansteen Alpha was composed of an unknown rock type. Subsequent studies by Lawrence et al. used improved knowledge of the Th spatial distribution for small area features on the lunar surface to revisit the interpretation of Th abundances at the Hansteen Alpha red spot. As part of their study, Lawrence et al. used a forward modeling technique to show that the Th abundance at Hansteen Alpha is not 6 ppm, but is more likely closer to 25 ppm, a value consistent with evolved lithologies. This positive correlation between the morphology and composition of Hansteen Alpha provides support for the presence of evolved lithologies on the lunar surface. It is possible, however, that Hansteen Alpha represents an isolated occurrence of non-mare volcanism. That is why we have chosen to use the forward modeling technique of Lawrence et al. to investigate the Th abundances at other lunar red spots, starting with the Gruithuisen domes. Additional information is included in the original extended abstract.

Hagerty, J. J.

High Efficiency Nuclear Power Plants using Liquid Fluoride Thorium Reactor Technology

An overall system analysis approach is used to propose potential conceptual designs of advanced terrestrial nuclear power plants based on Oak Ridge National Laboratory (ORNL) Molten Salt Reactor (MSR) experience and utilizing Closed Cycle Gas Turbine (CCGT) thermal-to-electric energy conversion technology. In particular conceptual designs for an advanced 1 GWe power plant with turbine reheat and compressor intercooling at a 950 K turbine inlet temperature (TIT), as well as near term 100 MWe demonstration plants with TITS of 950 K and 1200 K are presented. Power plant performance data were obtained for TITS ranging from 650 to 1300 K by use of a Closed Brayton Cycle (CBC) systems code which considered the interaction between major sub-systems, including the Liquid Fluoride Thorium Reactor (LFTR), heat source and heat sink heat exchangers, turbo -generator machinery, and an electric power generation and transmission system. Optional off-shore submarine installation of the power plant is a major consideration.

Juhasz, Albert J.