High temperature singlet-based magnetism from Hund's rule correlations.

Uranium compounds can manifest a wide range of fascinating many-body phenomena, and are often thought to be poised at a crossover between localized and itinerant regimes for 5f electrons. The antiferromagnetic dipnictide USb2 has been of recent interest due to the discovery of rich proximate phase diagrams and unusual quantum coherence phenomena. Here, linear-dichroic X-ray absorption and elastic neutron scattering are used to characterize electronic symmetries on uranium in USb2 and isostructural UBi2. Of these two materials, only USb2 is found to enable strong Hund's rule alignment of local magnetic degrees of freedom, and to undergo distinctive changes in local atomic multiplet symmetry across the magnetic phase transition. Theoretical analysis reveals that these and other anomalous properties of the material may be understood by attributing it as the first known high temperature realization of a singlet ground state magnet, in which magnetism occurs through a process that resembles exciton condensation.

Phonon dispersion of Mo-stabilized γ-U measured using inelastic x-ray scattering.

We have measured the room-temperature phonon spectrum of Mo-stabilized γ-U. The dispersion curves show unusual softening near the H point, q = [1/2, 1/2, 1/2], which may derive from the metastability of the γ-U phase or from strong electron-phonon coupling. Near the zone center, the dispersion curves agree well with theory, though significant differences are observed away from the zone center. The experimental phonon density of states is shifted to higher energy compared to theory and high-temperature neutron scattering. The elastic constants of γ-UMo are similar to those of body-centered cubic elemental metals.

Pressure dependence of Ce valence in CeRhIn5.

We have studied the Ce valence as a function of pressure in CeRhIn5 at 300 K and at 22 K using x-ray absorption spectroscopy in partial fluorescent yield mode. At room temperature, we found no detectable change in Ce valence greater than 0.01 up to a pressure of 5.5 GPa. At 22 K, the valence remains robust against pressure below 6 GPa, in contrast to the predicted valence crossover at P = 2.35 GPa. This work yields an upper limit for the change in Ce-valence and suggests that the critical valence fluctuation scenario, in its current form, is unlikely.

A combined theoretical and experimental investigation of uranium dioxide under high static pressure.

We have investigated the behavior of uranium dioxide (UO2) under high static pressure using a combination of experimental and theoretical techniques. We have made Raman spectroscopic measurements up to 87 GPa, electrical transport measurements up to 50 GPa from 10 K to room temperature, and optical transmission measurements up to 28 GPa. We have also carried out theoretical calculations within the GGA + U framework. We find that Raman frequencies match to a large extent, theoretical predictions for the cotunnite (Pnma) structure above 30 GPa, but at higher pressures some behavior is not captured theoretically. The Raman measurements also imply that the low-pressure fluorite phase coexists with the cotunnite phase up to high pressures, consistent with earlier reports. Electrical transport measurements show that the resistivity decreases by more than six orders of magnitude with increasing pressure up to 50 GPa but that the material never adopts archetypal metallic behavior. Optical transmission spectra show that while UO2 becomes increasingly opaque with increasing pressure, a likely direct optical band gap of more than 1 eV exists up to at least 28 GPa. Together with the electrical transport measurements, we conclude that the high pressure electrical conductivity of UO2 is mediated by variable-range hopping.

Persistent non-metallic behavior in Sr2IrO4 and Sr3Ir2O7 at high pressures.

Iridium-based 5d transition-metal oxides are attractive candidates for the study of correlated electronic states due to the interplay of enhanced crystal-field, Coulomb and spin-orbit interaction energies. At ambient pressure, these conditions promote a novel Jeff = 1/2 Mott-insulating state, characterized by a gap of the order of ~0.1 eV. We present high-pressure electrical resistivity measurements of single crystals of Sr2IrO4 and Sr3Ir2O7. While no indications of a pressure-induced metallic state up to 55 GPa were found in Sr2IrO4, a strong decrease of the gap energy and of the resistance of Sr3Ir2O7 between ambient pressure and 104 GPa confirm that this compound is in the proximity of a metal-insulator transition.

Pressure-induced unconventional superconducting phase in the topological insulator Bi2Se3.

Simultaneous low-temperature electrical resistivity and Hall effect measurements were performed on single-crystalline Bi2Se3 under applied pressures up to 50 GPa. As a function of pressure, superconductivity is observed to onset above 11 GPa with a transition temperature Tc and upper critical field Hc2 that both increase with pressure up to 30 GPa, where they reach maximum values of 7 K and 4 T, respectively. Upon further pressure increase, Tc remains anomalously constant up to the highest achieved pressure. Conversely, the carrier concentration increases continuously with pressure, including a tenfold increase over the pressure range where Tc remains constant. Together with a quasilinear temperature dependence of Hc2 that exceeds the orbital and Pauli limits, the anomalously stagnant pressure dependence of Tc points to an unconventional pressure-induced pairing state in Bi2Se3 that is unique among the superconducting topological insulators.

High pressure transport properties of the topological insulator Bi2Se3.

We report x-ray diffraction, electrical resistivity, and magnetoresistance measurements on Bi2Se3 under high pressure and low temperature conditions. Pressure induces profound changes in both the room temperature value of the electrical resistivity as well as the temperature dependence of the resistivity. Initially, pressure drives Bi2Se3 toward increasingly insulating behavior and then, at higher pressures, the sample appears to enter a fully metallic state coincident with a change in the crystal structure. Within the low pressure phase, Bi2Se3 exhibits an unusual field dependence of the transverse magnetoresistance Δρ(xx) that is positive at low fields and becomes negative at higher fields. Our results demonstrate that pressures below 8 GPa provide a non-chemical means to controllably reduce the bulk conductivity of Bi2Se3.

Competing ordered phases in URu2Si2: hydrostatic pressure and rhenium substitution.

A persistent kink in the pressure dependence of the "hidden order" (HO) transition temperature of URu(2-x)RexSi2 is observed at a critical pressure P(c)=15 kbar for 0

Field-dependent ordered phases and Kondo phenomena in the filled skutterudite compound PrOs4As12.

Electrical resistivity, specific heat, and magnetization measurements to temperatures as low as 80 mK and magnetic fields up to 16 T were made on the filled skutterudite compound PrOs4As12. The measurements reveal the presence of two ordered phases at temperatures below approximately 2.3 K and in fields below approximately 3 T. Neutron-scattering experiments in zero field establish an antiferromagnetic ground state < 2.28 K. In the antiferromagnetically ordered state, the electronic-specific heat coefficient gamma approximately 1 J/mol x K2 below 1.6 K and 0 < or = H < or = 1.25 T. The temperature and magnetic-field dependence of the electrical resistivity and specific heat in the paramagnetic state are consistent with single-ion Kondo behavior with a low Kondo temperature on the order of 1 K. The electronic-specific heat in the paramagnetic state can be described by the resonance-level model with a large zero-temperature electronic-specific heat coefficient that decreases with increasing magnetic field from approximately 1 J/mol x K2 at 3 T to approximately 0.2 J/mol x K2 at 16 T.