No Arabic abstract
Measurements of the phonon density of states by inelastic neutron emph{time-of-flight} scattering and specific heat measurements along with first principles calculations, provide compelling evidence for the existence of an Einstein oscillator (emph{rattler}) at ${omega}_{E1} approx$ 5.0 meV in the filled skutterudite Yb$_{0.2}$Co$_{4}$Sb$_{12}$. Multiple dispersionless modes in the measured density of states of Yb$_{0.2}$Co$_{4}$Sb$_{12}$ at intermediate transfer energies (14 meV $leq$ emph{$omega$} $leq$ 20 meV) are exhibited in both the experimental and theoretical emph{density-of-states} of the Yb-filled specimen. A peak at 12.4 meV is shown to coincide with a second Einstein mode at emph{$omega_{E2} approx$} 12.8 meV obtained from heat capacity data. The local modes at intermediate transfer energies are attributed to altered properties of the host CoSb$_{3}$ cage as a result of Yb-filling. It is suggested that these modes are owed to a complementary mechanism for the scattering of heat-carrying phonons in addition to the mode observed at ${omega}_{E1} , approx$ 5.0 meV. Our observations offer a plausible explanation for the significantly-higher textit{dimensionless figures of merit} of filled skutterudites, compared to their parent compounds.
The phonon dynamics of filled skutterudite CeRu4Sb12 have been studied at room temperature by inelastic neutron scattering. Optical phonons associated with a large vibration of Ce atoms are observed at a relatively low energy of E = 6 meV, and show anticrossing behavior with acoustic phonons. We propose that the origin of the low lattice thermal conductivity in filled skutterudites can be attributed to intensive Umklapp scattering originating from low-lying optical phonons. By an analysis based on a Born-von Karman force model, the longitudinal force constants of the nearest Ce-Sb and Ce-Ru pairs are estimated to be 0.025 mdyn/A, while that of the nearest Ru-Sb pair is estimated to be 1.4 mdyn/A, indicating that the Ce atoms are bound very weakly to the surrounding rigid RuSb6-octahedron cages.
The filled skutterudite compound PrOsSb{} exhibits superconductivity below a critical temperature $T_mathrm{c} = 1.85$ K that develops out of a nonmagnetic heavy Fermi liquid with an effective mass $m^{*} approx 50 m_mathrm{e}$, where $m_mathrm{e}$ is the free electron mass. Analysis of magnetic susceptibility, specific heat, electrical resistivity and inelastic neutron scattering measurements within the context of a cubic crystalline electric field yields a Pr$^{3+}$ energy level scheme that consists of a $Gamma_{3}$ nonmagnetic doublet ground state that carries an electric quadrupole moment, a low lying $Gamma_{5}$ triplet excited state at $sim 10$ K, and $Gamma_{4}$ triplet and $Gamma_{1}$ singlet excited states at much higher temperatures. The superconducting state appears to be unconventional and to consist of two distinct superconducting phases. An ordered phase of magnetic or quadrupolar origin occurs at high fields and low temperatures, suggesting that the superconductivity may occur in the vicinity of a magnetic or electric quadrupolar quantum critical point.
Anomalous metal-insulator transition observed in filled skutterudite CeOs$_4$Sb$_{12}$ is investigated by constructing the effective tight-binding model with the Coulomb repulsion between f electrons. By using the mean field approximation, magnetic susceptibilities are calculated and the phase diagram is obtained. When the band structure has a semimetallic character with small electron and hole pockets at $Gamma$ and H points, a spin density wave transition with the ordering vector $mathbf{Q}=(1,0,0)$ occurs due to the nesting property of the Fermi surfaces. Magnetic field enhances this phase in accord with the experiments.
A filled skutterudite, La$_{0.5}$Rh$_4$Sb$_{12}$, with a lattice constant of 9.284(2) {AA} was synthesized using a high-pressure technique. The electrical resistivity showed semiconducting behavior and the energy gap was estimated to be more than 0.08 eV. Magnetic susceptibility measurements indicated temperature-independent diamagnetism, which originates from Larmor diamagnetism. The electrical properties of this compound are more similar to those of the La$_{0.5}$Rh$_4$As$_{12}$ semiconductor with an energy gap of 0.03 eV than to those of the La$_{0.6}$Rh$_4$P$_{12}$ superconductor.
We report a study of the superconducting and normal-state properties of the filled-skutterudite system PrPt$_{4}$Ge$_{12-x}$Sb$_x$. Polycrystalline samples with Sb concentrations up to $x =$ 5 were synthesized and investigated by means of x-ray diffraction, electrical resistivity, magnetic susceptibility, and specific heat measurements. We observed a suppression of superconductivity with increasing Sb substitution up to $x =$ 4, above which, no signature of superconductivity was observed down to 140 mK. The Sommerfeld coefficient, $gamma$, of superconducting specimens decreases with increasing $x$ up to $x =$ 3, suggesting that superconductivity may depend on the density of electronic states in this system. The specific heat for $x =$ 0.5 exhibits an exponential temperature dependence in the superconducting state, reminiscent of a nodeless superconducting energy gap. We observed evidence for a weak rattling mode associated with the Pr ions, characterized by an Einstein temperature $Theta_{mathrm{E}} sim$ 60 K for 0 $leq x leq$ 5; however, the rattling mode may not play any role in suppressing superconductivity.