Low-lying optical phonon modes in the filled skutterudite CeRu4Sb12

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.Comment: 4pages, 5 figures, J. Phys. Soc. Jpn. (2006) in pres

31P-NMR and muSR Studies of Filled Skutterudite Compound SmFe4P12: Evidence for Heavy Fermion Behavior with Ferromagnetic Ground State

The 31P-NMR (nuclear magnetic resonance) and muSR (muon spin relaxation) measurements on the filled skutterudite system SmFe4P12 have been carried out. The temperature T dependence of the 31P-NMR spectra indicates the existence of the crystalline electric field effect splitting of the Sm3+$ (J = 5/2) multiplet into a ground state and an excited state of about 70 K. The spin-lattice relaxation rate 1/T1 shows the typical behavior of the Kondo system, i.e., 1/T1 is nearly T independent above 30 K, and varies in proportion to T (the Korringa behavior, 1/T1 \propto T) between 7.5 K and 30 K. The T dependence deviated from the Korringa behavior below 7 K, which is independent of T in the applied magnetic field of 1 kOe, and suppressed strongly in higher fields. The behavior is explained as 1/T1is determined by ferromagnetic fluctuations of the uncovered Sm3+ magnetic moments by conduction electrons. The muSR measurements in zero field show the appearance of a static internal field associated with the ferromagnetic order below 1.6 K.Comment: 6 pages, 9 figures, to be published in J. Phys. Soc. Jpn. 75 (2006

Determination of the high-pressure crystal structure of BaWO4 and PbWO4

We report the results of both angle-dispersive x-ray diffraction and x-ray absorption near-edge structure studies in BaWO4 and PbWO4 at pressures of up to 56 GPa and 24 GPa, respectively. BaWO4 is found to undergo a pressure-driven phase transition at 7.1 GPa from the tetragonal scheelite structure (which is stable under normal conditions) to the monoclinic fergusonite structure whereas the same transition takes place in PbWO4 at 9 GPa. We observe a second transition to another monoclinic structure which we identify as that of the isostructural phases BaWO4-II and PbWO4-III (space group P21/n). We have also performed ab initio total energy calculations which support the stability of this structure at high pressures in both compounds. The theoretical calculations further find that upon increase of pressure the scheelite phases become locally unstable and transform displacively into the fergusonite structure. The fergusonite structure is however metastable and can only occur if the transition to the P21/n phases were kinetically inhibited. Our experiments in BaWO4 indicate that it becomes amorphous beyond 47 GPa.Comment: 46 pages, 11 figures, 3 table

Superconductivity in the YIr2Si2 and LaIr2Si2 Polymorphs

We report on existence of superconductivity in YIr2Si2 and LaIr2Si2 compounds in relation to crystal structure. The two compounds crystallize in two structural polymorphs, both tetragonal. The high temperature polymorph (HTP) adopts the CaBe2Ge2-structure type (space group P4/nmm) while the low temperature polymorph (LTP) is of the ThCr2Si2 type (I4/mmm). By studying polycrystals prepared by arc melting we have observed that the rapidly cooled samples retain the HTP even at room temperature (RT) and below. Annealing such samples at 900C followed by slow cooling to RT provides the LTP. Both, the HTP and LTP were subsequently studied with respect to magnetism and superconductivity by electrical resistivity, magnetization, AC susceptibility and specific heat measurements. The HTP and LTP of both compounds respectively, behave as Pauli paramagnets. Superconductivity has been found exclusively in the HTP of both compounds below Tsc (= 2.52 K in YIr2Si2 and 1.24 K in LaIr2Si2). The relations of magnetism and superconductivity with the electronic and crystal structure are discussed with comparing experimental data with the results of first principles electronic structure calculations

Novel features in the flux-flow resistivity of the heavy fermion superconductor PrOs4_{4}Sb12_{12}

We have investigated the electrical resistivity of the heavy fermion superconductor PrOs$_{4}$Sb$_{12}$ in the mixed state. We found unusual double minima in the flux-flow resistivity as a function of magnetic field below the upper critical field for the first time, indicating double peaks in the pinning force density ($F_{\rm P}$). Estimated $F_{\rm P}$ at the peak exhibits apparent dependence on applied field direction; composed of two-fold and four-fold symmetries mimicking the reported angular dependence of thermal conductivity ($\kappa$). The result is discussed in correlation with the double step superconducting (SC) transition in the specific heat and the multiple SC-phases inferred from the angular dependence of $\kappa$.Comment: 5 pages, 7 figures, to appear in J. Phys. Soc. Jpn. Vol. 74, No. 6 or

XANES study of rare-earth valency in LRu4P12 (L = Ce and Pr)

Valency of Ce and Pr in LRu4P12 (L = Ce and Pr) was studied by L2,3-edge x-ray absorption near-edge structure (XANES) spectroscopy. The Ce-L3 XANES spectrum suggests that Ce is mainly trivalent, but the 4f state strongly hybridizes with ligand orbitals. The band gap of CeRu4P12 seems to be formed by strong hybridization of 4f electrons. Pr-L2 XANES spectra indicate that Pr exists in trivalent state over a wide range in temperature, 20 < T < 300 K. We find that the metal-insulator (MI) transition at TMI = 60 K in PrRu4P12 does not originate from Pr valence fluctuation.Comment: 4 page

Anomalous electric conductions in KSbO3-type metallic rhenium oxides

Single crystals of KSbO3-type rhenium oxides, La4Re6O$19, Pb6Re6O19, Sr2Re3O9 and Bi3Re3O11, were synthesized by a hydrothermal method. Their crystal structures can be regarded as a network of three-dimensional orthogonal-dimer lattice of edge-shared ReO6 octahedra. All of them exhibit small magnitude of Pauli paramagnetism, indicating metallic electronic states without strong electron correlations. The resistivity of these rhenates, except Bi3Re3O11, have a temperature dependence of$rho(T)=\rho_{0}+AT^{n}$$(n \approx 1.6)$ in a wide temperature range between 5 K and 300 K, which is extraordinary for three-dimensional metals without strong electron correlations. The resistivity of Bi3Re3O11 shows an anomaly around at 50 K, where the magnetic susceptibility also detects a deviation from ordinary Pauli paramagnetism.Comment: 13 pages, 7 figures. J. Phys. Soc. Japan, in pres

Optical Properties of MFe_4P_12 filled skutterudites

Infrared reflectance spectroscopy measurements were made on four members of the MFe_4P_12 family of filled skutterudites, with M=La, Th, Ce and U. In progressing from M=La to U the system undergoes a metal-insulator transition. It is shown that, although the filling atom induces such dramatic changes in the transport properties of the system, it has only a small effect on lattice dynamics. We discuss this property of the compounds in the context of their possible thermoelectric applications.Comment: Manuscript in ReVTeX format, 7 figures in PostScirpt forma

Unusual behaviors in the transport properties of REFe4_{4}P12_{12} (RE: La, Ce, Pr, and Nd)

We have investigated the resistivity ($\rho$), thermoelectric power (TEP) and Hall coefficient ($R_{H}$) on high quality single crystals of REFe$_{4}$P$_{12}$. TEP in CeFe$_{4}$P$_{12}$ is extremely large ($\sim$ 0.5mV/K at 290K) with a peak of $\sim$ 0.75mV/K at around 65K. The Hall mobility also shows a peak at $\sim$ 65K, suggesting carriers with heavy masses developed at lower temperatures related with the f-hybridized band. Both Pr- and Nd- systems exhibit an apparent increase of $\rho$ with decreasing temperature far above their magnetic transition temperatures. In the same temperature ranges, TEP exhibits unusually large absolute values of -50$\mu$V/K for PrFe$_{4}$P$_{12}$ and -15$\mu$V/K for NdFe$_{4}$P$_{12}$, respectively. For PrFe$_{4}$P$_{12}$, such anomalous transport properties suggest an unusual ground state, possibly related with the Quadrupolar Kondo effect.Comment: 5 pages, 8 figure