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V Keppens

Publications and source records attributed to V Keppens.

7 recordsLinked to original sources

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.

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Four-well tunneling States and elastic response of clathrates.

We present resonant ultrasound elastic constant measurements of the Eu8Ga16Ge30 and Sr8Ga16Ge30 clathrates. 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 explains the observed harmonic oscillator type specific heat. 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 explain the elastic properties assuming the same type of interaction, but with Sr Einstein mode.

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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.

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Disparate atomic displacements in skutterudite-type LaFe3CoSb12, a model for thermoelectric behavior.

Mean-square atomic displacements in lanthanum triiron cobalt dodecaantimonide, determined as a function of temperature using single-crystal neutron diffraction, show that the La atom exhibits an anomalously large displacement at room temperature, U(eq) = 0.0196 (9) Å(2), because it is too small to fill the atomic cage formed by the corner-linked octahedral framework of M(4)Sb(12), M = Fe, Co. Site-occupancy refinements show 25% vacancies on the La site and an actual Fe:Co ratio of 2.17:1. Analysis of the temperature dependence of the atomic displacements identifies a significant temperature-independent component for the La atom ascribed to static disorder, which amounts to 19% of the room-temperature value. The large-amplitude rattling of the La atom can be effectively linked to the dramatic decrease of the lattice contribution to the thermal conductivity, which is a key factor for improving the thermoelectric behavior of these materials. This structure-property relationship offers a new paradigm for the exploration of thermoelectric materials.

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