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We report on a comprehensive optical, transport and thermodynamic study of the Zintl compound Yb$_{14}$MnSb$_{11}$, demonstrating that it is the first ferromagnetic Kondo lattice compound in the underscreened limit. We propose a scenerio whereby the combination of Kondo and Jahn-Teller effects provides a consistent explanation of both transport and optical data., Comment: 4 pages

We have measured the polarized Raman scattering spectra of Cd2Re2O7, the first superconducting pyrochlore, as a function of temperature. For temperatures below the cubic-to-tetragonal structural phase transition (SPT) at 200K, a peak with B1 symmetry develops at zero frequency with divergent intensity. We identify this peak as the first observation of the Goldstone phonon in a crystalline solid. The Goldstone phonon is a collective excitation that exists due to the breaking of the continuous symmetry with the SPT. Its emergence coincides with that of a Raman-active soft mode. The order parameter for both features derives from an unstable doubly-degenerate vibration (with Eu symmetry) of the O1 atoms which drives the SPT., Comment: 4+ pages, 4 figures. Updated figures and text. Accepted to PRL

We report a systematic angle-resolved photoemission study on Na$_x$CoO$_2$ for a wide range of Na concentrations ($0.3 \leq x \leq 0.72$). In all the metallic samples at different $x$, we observed (i) only a single hole-like Fermi surface centered around $\Gamma$ and (ii) its area changes with $x$ according to the Luttinger theorem. We also observed a surface state that exhibits a larger Fermi surface area. The $e_g^\prime$ band and the associated small Fermi surface pockets near the $K$ points predicted by band calculations are found to ``sink'' below the Fermi energy in a manner almost independent of the doping and temperature., Comment: 4 pages, 5 figures

We report specific heat measurements down to 0.4 K on the layered oxide Na$_x$CoO$_2\cdot\it{y}$H$_2$O/D$_2$O with 0 $\le$ $\it{x}$ $\le$ 0.74 and $\it{y}$ = 0 and 1.4. For the nonhydrated system ($\it{y}$ = 0), the electronic specific heat coefficient $\gamma_N$ and the Debye temperature $\Theta_D$ vary nonmonotonically with $\it{x}$, both displaying minima when $\it{x}$ is close to 0.5. This indicates a systematic change of the electronic and vibrational structures with Na content. For both hydrated and deuterated systems ($\it{x}$ = 0.35 and $\it{y}$ = 1.4), the specific heat reveals a sharp peak with $\Delta$C$_p \sim$ 45.5 mJ/mol-K at T$_c^{mid} \sim$ 4.7 K and an anomaly at T$_x \sim$ 0.8 K. While the origin of the later is unknown, the former corresponds to the superconducting transition. Interestingly, the electronic specific heat, after subtracting lattice and Schottky contributions, exhibits roughly T$^2$ behavior between 0.2T$_c$ and T$_c$. This can be explained by assuming an unconventional superconducting symmetry with line nodes. The results obtained under applied magnetic field further support this scenario., Comment: 4 page, 3 figures, 1 table

We present resonant ultrasound elastic constant measurements of the clathrate compounds Eu8Ga16Ge30 and Sr8Ga16Ge30. The elastic response of the Eu clathrate provides clear evidence for the existence of a new type of four-well tunneling states, described by two nearly degenerate four level systems (FLS). The FLS's are closely linked with the fourfold split positions of Eu known from neutron diffraction density profiles. Using a realistic potential we estimate the tunneling frequencies and show that the energy gap between the two FLS's is of the same order as the Einstein oscillator frequency. This explains why the observed harmonic oscillator type specific heat is not modified by tunneling states. In addition the quadrupolar interaction of FLS's with elastic strains explains the pronounced depression observed in elastic constant measurements. In the case of the Sr clathrate, we show that the shallow dip in the elastic constant c44 is explained using the same type of quadrupolar interaction with a soft Einstein mode instead of a FLS., Comment: 4 pages, 4 figures; accepted for publication in Physical Review Letters

The magnetic, thermal and transport properties of Na0.75CoO2 single crystals grown by the floating zone (FZ) method are reported. Magnetic susceptibility, resistivity, magnetoresistance, and heat capacity data from these crystals indicate a bulk phase transition at T1 = 22 K. These data are most consistent with the formation of an antiferromagnet spin-density-wave (SDW) at 22 K with the easy axis for magnetization nearly along the c axis. Weak and soft ferromagnetism is observed for applied magnetic fields less than 0.5 T, which suggests a slight canting of the SDW magnetization with respect to the c axis. The jump in the heat capacity at the SDW transition is 0.45 J/K-mole-Co or about 50% of the value expected from mean-field weak-coupling theory. The reduced jump and the decrease in the resistivity below T1 are consistent with a gap for only part of the Fermi surface. The magnetoresistance is small at the SDW transition but increases in both directions reaching a value of 100% at 2 K for applied fields of 8 Tesla. The magnetoresistance data imply that the mobility of the remaining carriers is large and increases below T1. The observation of a SDW transition in this material is found to be sensitive to the preparation conditions and the degree of order in the Na layers. No SDW transition is observed in our polycrystalline powder with the same nominal composition (Na0.75CoO2) and lattice constants. Differential scanning calorimetry data, however, show distinct differences between the powder and crystal, suggesting a higher degree of order in the Na layers within the crystal. The crystal exhibits a sharp phase transition at T2 = 340 K while for the powder this transition is smeared over the temperature range from 250 to 310 K., Comment: 18 pages, 11 figures, submitted to Phys. Rev. B

A class of materials known as ``ferroelectric metals'' was discussed theoretically by Anderson and Blount in 1965 [Phys. Rev. Lett. 14, 217 (1965)], but to date no examples of this class have been reported. Here we present measurements of the elastic moduli of Cd2Re2O7 through the 200 K cubic-to-tetragonal phase transition. A Landau analysis of the moduli reveals that the transition is consistent with Cd2Re2O7 being classified as a ``ferroelectric metal'' in the weaker sense described by Anderson and Blount (loss of a center of symmetry). First-principles calculations of the lattice instabilities indicate that the dominant lattice instability corresponds to a two-fold degenerate mode with Eu symmetry, and that motions of the O ions forming the O octahedra dominate the energetics of the transition., Comment: 4 pages, 2 figures

The electronic structure of single crystals Na$_{0.6}$CoO$_2$, which are closely related to the superconducting Na$_{0.3}$CoO$_2$.$y$H$_2$O ($T_c \sim 5K$), is studied by angle-resolved photoelectron spectroscopy. While the measured Fermi surface is found to be consistent with the prediction of a local density band theory, the energy dispersion is highly renormalized, with an anisotropy along the two principle axes ($\Gamma$-$K$, $\Gamma$-$M$). Our ARPES result also indicates that an extended flat band is formed slightly above $E_F$ along $\Gamma$-$K$. In addition, an unusual band splitting is observed in the vicinity of the Fermi surface along the $\Gamma$-$M$ direction, which differs from the predicted bilayer splitting., Comment: 4 figures

Poly- and single-crystalline Na$_x$CoO$_2$ has been successfully intercalated with H$_2$O and D$_2$O as confirmed by X-ray diffraction and thermogravimetric analysis. Resistivity, magnetic susceptibility, and specific heat measurements show bulk superconductivity with T$_c$ close to 5 K in both cases. The substitution of deuterium for hydrogen has an effect on T$_c$ of less than 0.2 K. Investigation of the resistivity anisotropy of Na$_x$CoO$_2\cdot$yH$_2$O single crystals shows: (a) almost zero resistivity below T$_c$, and (b) an abrupt upturn at $T^* \sim$ 52 K in both the $\it {ab}$ plane and the $\it {c}$ direction. The implications of our results on the possible superconducting mechanism will be discussed., Comment: 4 pages, 4 figures and 1 table

We report measurements of the two-magnon states in a dimerized antiferromagnetic chain material, copper nitrate (Cu(NO3)2*2.5D2O). Using inelastic neutron scattering we have measured the one and two magnon excitation spectra in a large single crystal. The data are in excellent agreement with a perturbative expansion of the alternating Heisenberg Hamiltonian from the strongly dimerized limit. The expansion predicts a two-magnon bound state for q ~ (2n+1)pi*d which is consistent with the neutron scattering data., Comment: 11 pages of revtex style with 6 figures included

We demonstrate that angle-resolved soft x-ray spectroscopy can resolve absorption by inequivalent oxygen sites and by different orbitals belonging to the same site in NaV2O5. By rotating the polarization direction, we see a dramatic change in the absorption spectra at the oxygen K edge. Our theory identifies the detailed composition of the spectra and predicts a correct energy-ordering of the orbitals of three inequivalent oxygen atoms. Because different orbitals dominate absorption spectra at different energies and angles, one can excite at a specific site and ``orbital''. In contrast, absorption at the vanadium L edge does not show large changes when varying the polarization direction. The reason for this is that different excitation channels (involving different initial states for the excited electron) overlap in energy and vary in compensating ways, obscuring each channel's sensitive polarization dependence., Comment: 12 pages, 6 figures, accepted to PRB

Experimental investigation of the resistivity $\rho$, susceptibility $\chi$, specific heat C$_p$, and Hall coefficient R$_H$ of the pyrochlore Cd$_2$Re$_2$O$_7$ reveals the presence of a continuous phase transition of uncertain origin with critical temperature T* = 200 K. Electron and X-ray diffraction measurements indicate that a commensurate structural transformation accompanies the changes in the electronic properties, implying that lattice as well as electronic degrees of freedom are involved in the transition. Remarkable scaling relationships between $\rho$, $\chi$, and C$_p$ are observed, indicating that fluctuations are crucial in the transition regime. Scenarios involving both spin and ionic density fluctuations are considered in the evaluation of the data. Although the observed structural transition suggests that ionic density fluctuations are likely to be important, a scaling relationship between $\rho$ and $\chi$ over a wide temperature range suggests that spin fluctuations may be playing a role as well., Comment: 4 pages, 4 figures

The growth mechanisms of MgB2 films obtained by different methods on various substrates are compared via a detailed cross-sectional scanning electron microscopy (SEM) study. The analyzed films include (a) samples obtained by an ex-situ post-anneal at 900 degree of e-beam evaporated boron in the presence of an Mg vapor (exhibiting bulk-like Tc0 about 38.8 K), (b) samples obtained by the same ex-situ 900 degree anneal of pulsed laser deposition (PLD)-grown Mg+B precursors (exhibiting Tc0 ~ 25 K), and (c) films obtained by a low-temperature (600 - 630 degree) in-situ anneal of PLD-grown Mg+B precursors (with Tc0 about 24 K). A significant oxygen contamination was also present in films obtained from a PLD-grown precursors. On the other hand, it is clearly observed that the films obtained by the high-temperature reaction of e-beam evaporated B with Mg vapor are formed by the nucleation of independent MgB2 grains at the film surface, indicating that this approach may not be suitable to obtain smooth and (possibly) epitaxial films., Comment: 1 table, 4 figures, 17 references, 16 pages PDF file

Superconducting magnesium diboride films with Tc0 ~ 24 K and sharp transition \~ 1 K were successfully prepared on silicon substrates by pulsed laser deposition from a stoichiometric MgB2 target. Contrary to previous reports, anneals at 630 degree and a background of 2x10^(-4) torr Ar/4%H2 were performed without the requirement of Mg vapor or an Mg cap layer. This integration of superconducting MgB2 films on silicon may thus prove enabling in superconductor-semiconductor device applications. Images of surface morphology and cross-section profiles by scanning electron microscopy (SEM) show that the films have a uniform surface morphology and thickness. Energy dispersive spectroscopy (EDS) reveals these films were contaminated with oxygen, originating either from the growth environment or from sample exposure to air. The oxygen contamination may account for the low Tc for those in-situ annealed films, while the use of Si as the substrate does not result in a decrease in Tc as compared to other substrates., Comment: 5 pages, 4 figures, 15 references; due to file size limit, images were blured

Thin superconducting films of magnesium diboride (MgB2) with Tc \approx 24K were prepared on various oxide substrates by pulsed laser deposition (PLD) followed by an in-situ anneal. A systematic study of the influence of various in-situ annealing parameters shows an optimum temperature of about 600C in a background of 0.7 atm. of Ar/4%H2 for layers consisting of a mixture of magnesium and boron. Contrary to ex-situ approaches (e.g. reacting boron films with magnesium vapor at 900C), these films are processed below the decomposition temperature of MgB2. This may prove enabling in the formation of multilayers, junctions, and epitaxial films in future work. Issues related to the improvement of these films and to the possible in-situ growth of MgB2 at elevated temperature are discussed., Comment: 5 pages, 4 figures

Cd2Os2O7 crystallizes in the pyrochlore structure and undergoes a metal-insulator transition (MIT) near 226 K. We have characterized the MIT in Cd2Os2O7 using X-ray diffraction, resistivity at ambient and high pressure, specific heat, magnetization, thermopower, Hall coefficient, and thermal conductivity. Both single crystals and polycrystalline material were examined. The MIT is accompanied by no change in crystal symmetry and a change in unit cell volume of less than 0.05%. The resistivity shows little temperature dependence above 226 K, but increases by 3 orders of magnitude as the sample is cooled to 4 K. The specific heat anomaly resembles a mean-field transition and shows no hysteresis or latent heat. Cd2Os2O7 orders magnetically at the MIT. The magnetization data is consistent with antiferromagnetic order, with a small parasitic ferromagnetic component. The Hall and Seebeck coefficients are consistent with a semiconducting gap opening at the Fermi energy at the MIT. We have also performed electronic structure calculations on Cd2Os2O7. These calculations indicate that Cd2Os2O7 is metallic, with a sharp peak in the density of states at the Fermi energy. We intepret the data in terms of a Slater transition. In this scenario, the MIT is produced by a doubling of the unit cell due to the establishment of antiferromagnetic order. A Slater transition-unlike a Mott transition-is predicted to be continuous, with a semiconducting energy gap opening much like a BCS gap as the material is cooled below $T_{MIT}$., Comment: 13 pages, 18 eps figures

Magnetization and neutron diffraction measurements indicate long-range antiferromagnetic ordering below TN=4 K in the 2D, S=1/2 Heisenberg antiferromagnet K2V3O8. The ordered state exhibits ``weak ferromagnetism'' and novel, field-induced spin reorientations. These experimental observations are well described by a classical, two-spin Heisenberg model incorporating Dzyaloshinskii-Moriya interactions and an additional c-axis anisotropy. This additional anisotropy can be accounted for by inclusion of the symmetric anisotropy term recently described by Kaplan, Shekhtman, Entin-Wohlman, and Aharony. This suggests that K2V3O8 may be a very unique system where the qualitative behavior relies on the presence of this symmetric anisotropy., Comment: 5 pages, 4 ps figures, REVTEX, submitted to PRL

We report measurements of the two-magnon states in a dimerized antiferromagnetic chain material, copper nitrate (\QTR{group}{Cu(NO$_{3}$)$_{2}\cdot 2.5$D$_{2}$O}). Using inelastic neutron scattering, we have studied the one- and two-magnon excitation spectra in a large single crystal of this material. We compare this new data with perturbative expansions of the alternating Heisenberg chain and find good agreement with these calculations. The data may also show evidence for the recently proposed S=1 two-magnon bound state (Phys. Rev. B54, R9624 (1996))., Comment: 10 pages, 4 figures, fig(3) in color

Single crystals of the spin-gap system $\rm (VO)_2P_2O_7$ have been investigated by means of Raman scattering. At temperatures below T=75 K~$\approx 2\Delta_{01}({\bf k}=0)$, with $\Delta_{01}$ the singlet-triplet gap, a shoulder appears at 47 cm$^{-1}$. An analysis of the polarization selection rules and the temperature dependence of the scattering intensity leads to its identification as a singlet bound state with very small binding energy. Therefore in contrast to recent theoretical models the importance of frustration for this compound must be rejected. The observation of a strong anharmonicity of three phonons with energies close to $\Delta_{01}$ at the zone boundary and additional quasielastic light scattering, however, both point to a strong spin-phonon coupling in this system. We propose this coupling to be the origin of the second bound triplet state observed in recent neutron scattering experiments., Comment: 6 pages, 9 figures

The great reduction in thermal conductivity of skutterudites upon filling the ``void'' sites with Rare Earth (RE) ions is key to their favorable thermoelectric properties but remains to be understood. Using lattice dynamic models based on first principles calculations, we address the most popular microscopic mechanism, reduction via rattling ions. The model withstands inelastic neutron scattering and specific heat measurements, and refutes hypotheses of an anharmonic RE potential and of two distinct localized RE vibrations of disparate frequencies. It does indicate a strong hybridization between bare La vibrations and certain Sb-like phonon branches, suggesting anharmonic scattering by harmonic RE motions as an important mechanism for suppression of heat conductivity., Comment: modified version resubmitted to PRB. Results unchanged, text changed substantially

Magnetic excitations in an array of (VO)_2P_2O_7 single crystals have been measured using inelastic neutron scattering. Until now, (VO)_2P_2O_7 has been thought of as a two-leg antiferromagnetic Heisenberg spin ladder with chains running in the a-direction. The present results show unequivocally that (VO)_2P_2O_7 is best described as an alternating spin-chain directed along the crystallographic b-direction. In addition to the expected magnon with magnetic zone-center energy gap \Delta = 3.1 meV, a second excitation is observed at an energy just below 2\Delta. The higher mode may be a triplet two-magnon bound state., Comment: 4 pages, postscript figures

In this letter we report results from inelastic neutron scattering experiments on powder samples of vanadyl pyrophosphate, (VO)2P2O7. We see evidence for three magnetic excitations, at 3.5 meV, 6.0 meV and 14 meV. The intensity of the 3.5 meV mode is strong near Q=0.8 A-1, consistent with the one-magnon gap mode reported previously and predicted by the spin-ladder model. The magnetic scattering at 14 meV may be due to the top of the one-magnon band or the two-magnon continuum predicted in the ladder model. The 6.0 meV mode also peaks in intensity at Q=0.8 A-1. This mode has not been reported previously and was not anticipated by existing theoretical treatments of the spin ladder., Comment: 14 pages, 4 figures, REVTEX using epsfig. Postscript file available at http://csep2.phy.ornl.gov/theory_group/people/barnes/cm/cm.html as vopo.ps