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Register a new userLow-lying optical phonon modes in the filled skutterudite CeRu4Sb12
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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.
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The caged compound LaRu2Zn20 exhibits a structural transition at TS =150 K, whose driving mechanism remains elusive. We have investigated atomic dynamics by the measurements of specific heat C and inelastic X-ray scattering (IXS). The lattice part of the specific heat Clat divided by T3, Clat/T3, shows a broad peak at around 15 K, which is reproduced by two Einstein modes with characteristic temperatures of 35 K and 82 K, respectively. IXS measurements along the [111] and [110] directions reveal optical phonon modes at 3 meV (35 K) and 7 meV (80 K), respectively, whose values agree with the values of Einstein temperatures. The first principles calculation has assigned the phonon modes at 3 meV as the optical modes of Zn atoms located at the middle of two La atoms. The low-energy vibration of the Zn atom perpendicular to the there-fold axis is thought to lead the structural instability of LaRu2Zn20.
We report experimental results of nuclear magnetic resonance (NMR) at the La site and nuclear quadrupole resonance (NQR) at the Sb site in the filled skutterudite LaOs$_4$Sb$_{12}$. We found that the nuclear spin-lattice relaxation rate divided by temperature $1/T_1T$ at the La site exhibits a different temperature dependence from that at the Sb site. Although $1/T_1T$ at the Sb site is explained by the Korringa mechanism, $1/T_1T$ at the La site exhibits a broad maximum around 50 K, showing the presence of an additional contribution at the La site. The additional low-lying excitations observed at the La site can be understood with the relaxation from anharmonic phonons due to the rattling motion of the La atoms.
Specific heat and magnetization measurements have been performed on high-quality single crystals of filled-skutterudite PrFe_4P_{12} in order to study the high-field heavy-fermion state (HFS) and low-field ordered state (ODS). From a broad hump observed in C/T vs T in HFS for magnetic fields applied along the <100> direction, the Kondo temperature of ~ 9 K and the existence of ferromagnetic Pr-Pr interactions are deduced. The {141}-Pr nuclear Schottky contribution, which works as a highly-sensitive on-site probe for the Pr magnetic moment, sets an upper bound for the ordered moment as ~ 0.03 mu_B/Pr-ion. This fact strongly indicates that the primary order parameter in the ODS is nonmagnetic and most probably of quadrupolar origin, combined with other experimental facts. Significantly suppressed heavy-fermion behavior in the ODS suggests a possibility that the quadrupolar degrees of freedom is essential for the heavy quasiparticle band formation in the HFS. Possible crystalline-electric-field level schemes estimated from the anisotropy in the magnetization are consistent with this conjecture.
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.
Magnetization, specific heat, and electrical resistivity measurements were made on single crystals of the filled skutterudite compound PrOs$_{4}$As$_{12}$. Specific heat measurements indicate an electronic specific heat coefficient $gamma$ $sim 50-200$ mJ/mol K$^{2}$ at temperatures 10 K $leq T leq 18$ K, and $sim 1$ J/mol K$^{2}$ for $T leq 1.6$ K. Magnetization, specific heat, and electrical resistivity measurements reveal the presence of two, or possibly three, ordered phases at temperatures below $sim 2.3$ K and in fields below $sim 3$ T. The low temperature phase displays antiferromagnetic characteristics, while the nature of the ordering in the other phase(s) has yet to be determined.
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