Engineering topics

Chappell, Greta L.

Publications and source records attributed to Chappell, Greta L..

5 records

DOE OSTI2025

Adaptation of Wallace's approach to the specific heat of elemental solids with significant intrinsic anharmonicity, particularly the light actinide metals

The quasiharmonic approximation is the most common method for modeling the specific heat of solids; however, it fails to capture the effects of intrinsic anharmonicity. In this study, we introduce the “elastic softening approximation,” an alternative approach to modeling intrinsic anharmonic effects on thermodynamic quantities, which is grounded in Wallace's thermodynamic framework that tracks entropy changes resulting from the continuous change (e.g., softening) of phonons as a function of temperature. A key finding of our study is a correlation between Poisson's ratio and the differential rate of phonon softening at finite frequencies, compared to lower frequencies relevant to elastic moduli measurements. We observe that elemental solids such as α -Be, diamond, Al, Cu, In, W, Au, and Pb, which span a wide range of Poisson's ratios and exhibit varying degrees of intrinsic anharmonicity, consistently follow this trend. When applied to α -U, α -Pu, and δ -Pu, our method reveals unusually large anharmonic phonon contributions at elevated temperatures across all three light actinide metals. These findings are attributed to the unique combination of enhanced covalency and softer elastic moduli inherent in the actinides, potentially influenced by their 5 f -electron bonding. Published by the American Physical Society 2025

36 MATERIALS SCIENCE↗

DOE OSTI2024

Indications of flat bands driving the δ to α volume collapse of plutonium

On cooling from the melt, plutonium (Pu) undergoes a series of structural transformations accompanied by a ≈ 28% reduction in volume from its δ phase to its α phase at low temperatures. While Pu’s partially filled 5 f -electron shells are known to be involved, their precise role in the transformations has remained unclear. By using calorimetry measurements on α -Pu and gallium-stabilized δ -Pu combined with resonant ultrasound and X-ray scattering data to account for the anomalously large softening of the lattice with temperature, we show here that the difference in electronic entropy between the α and δ phases dominates over the difference in phonon entropy. Rather than finding an electronic specific heat characteristic of broad f -electron bands in α -Pu, as might be expected to occur within a Kondo collapsed phase in analogy with cerium, we find it to be indicative of flatter subbands. An important role played by Pu’s 5 f electrons in the formation of its larger unit cell α phase comprising inequivalent lattice sites and varying bond lengths is therefore suggested.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Electronic Tuning in URu2Si2 Through Ru to Pt Chemical Substitution

Studies that control the unit cell volume and electronic composition have been useful in revealing what factors lead to hidden order and superconductivity in the strongly correlated electron system URu 2 Si 2 . For example, isoelectronic tuning that increases the hybridization between the f and conduction electron states (i.e., applied pressure and Ru → Fe/Os chemical substitution) 1) converts hidden order into antiferromagnetism and 2) destroys the superconductivity. The impact of nonisoelectronic chemical substitution has been less clear, but several unifying trends have recently emerged for chemical substitution vectors that qualitatively add electrons (e.g., Ru → Rh/Ir and Si → P). This includes 1) the rapid destruction of hidden order and superconductivity, 2) composition regions where the underlying Kondo lattice is preserved but does not harbor an ordered state, and 3) the emergence of complex magnetism at large substitutions. In order to assess the limits of this perspective, we have investigated the series U(Ru 1− x Pt x ) 2 Si 2 for x ≲ 0.19, where the Ru and Pt d -shells differ substantially from each other. Magnetic susceptibility, electrical resistivity, and heat capacity measurements unexpectedly reveal a phase diagram with notable similarities to those of other electron doping series. This result reinforces the viewpoint that there is a quasi-universal affect that results from electron doping in this material, and we anticipate that an understanding of these trends will be useful to isolate what factors are foundational for hidden order and superconductivity.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Influence of hydrostatic pressure on hidden order, the Kondo lattice, and magnetism in URu 2 Si 2-x P x

Within the chemical substitution series URu 2 Si 2-x P x , there is an evolution in the ground-state behavior from hidden ordered (HO) for x ≲ 0.03, to Kondo lattice behavior with no ordering (NO) for 0.03 ≲ x ≲ 0.26, to antiferromagnetism (AFM-2) for 0.26 ≲ x ≲ 0.5 [A. Gallagher et al., Nat. Commun. 7, 10712 (2016); A. Gallagher et al., J. Phys.: Condens. Matter 29, 024004 (2016)]. To better understand what factors control this behavior, temperature-dependent electrical resistivity measurements are performed for this series under applied pressures P up to 20.5 kbar. Specimens in the HO x region show similarities to the parent compound, where HO transforms into antiferromagnetism (AFM-1) at a critical pressure (P c ). P c decreases with increasing x and collapses towards P = 0 near x ≈ 0.03, suggesting that AFM-1 occurs at ambient pressure for this concentration. No pressure-induced phase transitions are observed in the NO x region and the AFM-2 state is only weakly suppressed by P. Measurements further reveal that AFM-1 and AFM-2 are distinct from each other. Calculations of the wave functions using the tight-binding Hartree-Fock approximation are performed and show (i) that the radial probability distributions for the phosphorus ions are more tightly bound than those for the silicon and (ii) that the energy difference between the orbitals decreases with increasing x. The cumulative effect of these two factors is that Si → P substitution decreases the hybridization strength, which correlates with the weakening of HO. At large x, additional effects such as electrical charge tuning also play an important role in determining the ground-state

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Charge density wave with anomalous temperature dependence in UPt 2 Si 2

Using single-crystal neutron and x-ray diffraction, we discovered a charge density wave (CDW) below 320 K, which accounts for the long-sought origin of the heat capacity and resistivity anomalies in UPt 2 Si 2 . The modulation wave vector, Q mod , is intriguingly similar to the incommensurate wave vector of URu 2 Si 2 . Q mod shows an unusual temperature dependence, shifting from commensurate to incommensurate position upon cooling and becoming locked at aproximately (0.42 0 0) near 180 K. Furthermore, bulk measurements indicate a crossover toward a correlated coherent state around the same temperature, suggesting an interplay between the CDW and Kondo-lattice-like coherence before coexisting antiferromagnetic order sets in at T N =35 Κ.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗