Pressure effects on the transition temperature and the magnetic field penetration depth in the pyrochlore superconductor RbOs2O6

Magnetization measurements under hydrostatic pressure up to 8 kbar in the pyrochlore superconductor RbOs2O6 (T(c) approximately or equal 6.3 K at p=0) were carried out. A positive pressure effect on T(c) with dT(c)/dp=0.090(3) K/kbar was observed, whereas no pressure effect on the magnetic penetration depth lambda was detected. The pressure independent ratio 2 Delta(0)/k(B)T(c)=3.72(2) (Delta(0) is the superconducting gap at zero temperature) was found to be close to the BCS value 3.52. Magnetization and muon-spin rotation measurements of lambda(T) indicate that RbOs2O6 is an adiabatic s-wave BCS-type superconductor. The value of lambda extrapolated to zero temperature and ambient pressure was estimated to be 230(30) nm.     

NMR observation of rattling phonons in the pyrochlore superconductor KOs2O6

We report nuclear magnetic resonance studies on the beta-pyrochlore oxide superconductor KOs2O6. The nuclear relaxation at the K sites is entirely caused by fluctuations of the electric field gradient, which we ascribe to highly anharmonic low frequency oscillation (rattling) of K ions. A phenomenological analysis shows a crossover from overdamped to underdamped behavior of the rattling phonons with decreasing temperature and its sudden sharpening below the superconducting transition temperature T(c). Suppression of the Hebel-Slichter peak in the relaxation rate at the O sites below T(c) also indicates strong electron-phonon coupling.     

Thermal conductivity of the pyrochlore superconductor KOs2O6: strong electron correlations and fully gapped superconductivity

To elucidate the nature of the superconducting ground state of the geometrically frustrated pyrochlore KOs2O6 (Tc=9.6 K), the thermal conductivity was measured down to low temperatures (approximately Tc/100). We found that the quasiparticle mean free path is strikingly enhanced below a transition at Tp=7.8 K, indicating enormous electron inelastic scattering in the normal state. In magnetic fields, the conduction at T-->0 K is nearly constant up to approximately 0.4Hc2, in contrast with the rapid growth expected for superconductors with an anisotropic gap. This unambiguously indicates a fully gapped superconductivity, in contrast with previous studies. These results highlight that KOs2O6 is unique among superconductors with strong electron correlations.     

Structure and proton mobility in the defect pyrochlore (H2O)xH2Ta2O6

The structure of the defect pyrochlore (D₂O)_0.38D₂Ta₂O₆ has been determined by powder neutron diffraction. The deuteroxyl deuterons randomly occupy sites ∼ 1.04 Å from the framework oxygens. The water molecules are situated on sites at the centre of the defect pyrochlore cavity, 8b position of Fd3m, and the O_W-D_W bonds lengths are 0.97 Å. A pulsed solid state N.M.R. study of (H₂O)_0.42H₂Ta₂O₆ has shown that this material is a reasonable proton conductor with a room temperature diffusion co-efficient of ∼ 10^-9 cm² s^-1.     

Temperature dependence of the magnetic penetration depth in the vortex state of the pyrochlore superconductor,Cd2Re2O7

We report transverse-field and zero-field muon spin rotation and relaxation studies of the superconducting rhenium oxide pyrochlore, Cd2Re2O7. Transverse-field measurements (H=0.007 T) show line broadening below T(c), which is characteristic of a vortex state, demonstrating conclusively the type-II nature of this superconductor. The penetration depth is seen to level off below about 400 mK (T/T(c) approximately 0.4), with a rather large value of lambda(T=0) approximately 7500 A. The temperature independent behavior below approximately 400 mK is consistent with a nodeless superconducting energy gap. Zero-field measurements indicate no static magnetic fields developing below the transition temperature.     

Evidence for gapped spin-wave excitations in the frustrated Gd2Sn2O7 pyrochlore antiferromagnet from low-temperature specific heat measurements

We have measured the low-temperature specific heat of the geometrically frustrated pyrochlore Heisenberg antiferromagnet Gd2Sn2O7 in zero magnetic field. The specific heat is found to drop exponentially below approximately 350 mK. This provides evidence for a gapped spin-wave spectrum due to an anisotropy resulting from single-ion effects and long-range dipolar interactions. The data are well fitted by linear spin-wave theory, ruling out unconventional low-energy magnetic excitations in this system, and allowing a determination of the pertinent exchange interactions in this material.     

Anomalous critical behavior of NaV2O5

The temperature dependences and critical behavior of the dielectric constant were studied in NaV₂O₅ along the c axis in a frequency range of 1 MHz-1GHz and a temperature range of 4.2–300 K. An analysis of the data obtained, along with literature data on the heat capacity, magnetic losses, and the ultrasound velocity, indicates that the various physical quantities demonstrate similar temperature dependences in the vicinity of the transition, which corroborates the conclusion on the universality of the critical behavior in NaV₂O₅. Deviations from the predictions of the standard theory of second-order phase transitions were found, such as the asymmetry of the critical behavior above and below the transition and the presence of an anomalous base line.     

Evidence for dynamic behavior of O2 in oxyheme model compounds

We have performed Mössbauer studies on several oxy-heme model compounds, and for two of them we also have derived the threedimensional structure from X-ray studies; I: [Fe(O₂) (SC₆HF₄) TP_pivP] [Na?18C6] and II: [Fe(O₂) (SC₆HF₄)TP_pivP] [K?222]. Compound I shows a pronounced temperature-dependence of ΔE_Q, i. e. 2.17 mms^?1 at 4.2 K and 1.55 mms^?1 at 295 K, while ΔE_Q of compound II is practically temperature-independent, i.e. ca. 2.05 mms^?1. The X-ray structure analysis of these model compounds provides us with the fact that O₂ occupies three different sites in I and only two sites in II. From the experimentally known occupancies of these sites at specific temperatures we were able to apply relaxation calculations for the electric field gradient tensors in I and II, and we found for both compounds that our calculated ΔE_Q(T)-data are in agreement with our experimental results. These findings imply that the dynamic jump behavior of O₂ among the different sites in oxy-heme model compounds is responsible for the temperature-dependence (like in HbO₂) or temperature-independence of ΔE_Q (like in cytochrome P450).     

Nearly free electrons in the layered oxide superconductor Ag5Pb2O6

We present first measurements of quantum oscillations in the layered oxide superconductor Ag5Pb2O6. From a detailed angular and temperature dependent study of the de Haas-van Alphen effect we determine the electronic structure and demonstrate that the electron masses are very light, m* approximately 1.2me. The Fermi surface we observe is essentially that expected of nearly free electrons--establishing Ag5Pb2O6 as the first known example of a monovalent, nearly free electron superconductor at ambient pressure.     

Vortex redistribution below the first-order transition temperature in the beta-pyrochlore superconductor KOs2O6

A miniature Hall-sensor array was used to detect magnetic induction locally in the vortex states of the beta-pyrochlore superconductor KOs2O6. Below the first-order transition at T{p} approximately 8 K, which is associated with a change in the rattling motion of K ions, the lower critical field and the remanent magnetization both show a distinct decrease, suggesting that the electron-phonon coupling is weakened below the transition. At high magnetic fields, the local induction shows an unexpectedly large jump at T{p} whose sign changes with position inside the sample. Our results demonstrate a novel redistribution of vortices whose energy is reduced abruptly below the first-order transition at T{p}.     

Goldstone-mode phonon dynamics in the pyrochlore Cd2Re2O7

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 200 K, 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.     

Metallic "ferroelectricity" in the pyrochlore Cd2Re2O7

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 of materials 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 twofold degenerate mode with E(u) symmetry and that motions of the O ions forming the O octahedra dominate the energetics of the transition.     

Superconducting properties of the pyrochlore oxide Cd2Re2O7

We report the superconducting properties of the pyrochlore oxide Cd₂Re₂O₇. The bulk superconducting transition temperature T_c is about 1.0 K, and the upper critical field H_c2 determined by the measurement of specific heat under magnetic fields is 0.29 T. The superconducting coherence length is estimated to be 34 nm. Specific heat data measured on single crystals suggest that the superconducting gap of Cd₂Re₂O₇ is nodeless.