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The atomic structures of nanocrystalline powders of ceria, CeO2, and ceria-zirconia solid solution, (Ce,Zr)O2, were studied by the pulsed neutron diffraction technique. Ceria is used as an oxygen storage component in automotive exhaust emission control systems, but the degradation of its oxygen storage capacity (OSC) after extended use at high temperatures has been a problem. Our results for the first time establish a direct correlation between the concentration of vacancy-interstitial oxygen defects and OSC. The surface area, on the other hand, exhibits much less correlation with OSC. The results also show that zirconia, which is known to retard the degradation when incorporated into ceria, reduces ceria and preserves oxygen defects. It is suggested that oxygen defects are the source of OSC in ceria-based catalyst supports, and the preservation of oxygen defects is critical for the stability of OSC against thermal aging.
The spin dynamics of the underdoped superconductor YBa 2 Cu 3 O 6.7 (T c ϳ 67 K) was revealed to have an incommensurate wave vector dependence with "pillars" in the dispersion relation at the positions ( 1 2 6 d, 1 2 , 0) and ( 1 2 , 1 2 6 d, 0). This is the same symmetry as that found in La 22x Sr x CuO 4 . The value of the incommensurability, d 0.11 6 0.01 r.l.u ϳ 1 8 , is very close to the value expected from the hole concentration. These results have demonstrated that the spin dynamics do not depend on the details of Fermi surface but have an analogous form to that for the proposed stripe domain structure.
Inelastic neutron scattering measurements on single crystals of superconducting BaFe1.84Co0.16As2 reveal a magnetic excitation located at wavevectors (1/2 1/2 L) in tetragonal notation. On cooling below TC, a clear resonance peak is observed at this wavevector with an energy of 8.6(0.5) meV, corresponding to 4.5(0.3) kBTC . This is in good agreement with the canonical value of 5 kBTC observed in the cuprates. The spectrum shows strong dispersion in the tetragonal plane but very weak dispersion along the c-axis, indicating that the magnetic fluctuations are two-dimensional in nature. This is in sharp contrast to the anisotropic three dimensional spin excitations seen in the undoped parent compounds.PACS numbers: 78.70.Nx, 74.20.Mn Understanding the physics of superconductivity in high-T c cuprates and other unconventional superconductors remains a central unresolved problem at the forefront of condensed matter physics. One widespread school of thought maintains that magnetic fluctuations are intimately involved in the pairing mechanism. This view is supported by a growing number of neutron scattering investigations showing the appearance of a magnetic excitation coincident with the onset of superconductivity [1,2,3,4,5,6,7,8]. The spectrum shows a resonance at a wavevector related to the antiferromagnetic order in the non-superconducting parent compounds. The apparent resonance energy scales with T C for different cuprate materials exhibiting a wide range of superconducting transition temperatures [9], providing tantalizing evidence for a common mechanism related to magnetic fluctuations.The discovery of a new family of Fe-based high temperature superconductors with T C as high as 55 K [10,11,12,13,14,15,16] presents an exciting opportunity to examine the relationship of spin excitations to the superconducting condensate in unconventional superconductors. The new materials are composed of Fe containing planes (FeAs or FeSe). Both theory and experiment indicate that simple electron-phonon coupling cannot describe superconductivity in these materials [17,18]. Furthermore, the superconducting state exists in close proximity to magnetism as the parent compounds exhibit spin-density wave order [19,20]. These observations have been put forth as evidence that the superconductivity in the Fe-based materials is unconventional. The presence of the Fe planes suggests quasi-two-dimensionality, as observed in the cuprates. However, neutron scattering investigations of the spin waves in the undoped parent compounds SrFe 2 As 2 [21], BaFe 2 As 2 [22], and CaFe 2 As 2 [23], indicate anisotropic exchange that cannot be classified as two dimensional. Band structure calculations [24,25] indicate that doping should enhance the twodimensionality of the Fermi surface, favoring superconductivity [25]. Directly probing the magnetic fluctuations in superconducting Fe-based systems is crucial for further progress.Recent measurements on a polycrystalline sample of Ba 0.6 K 0.4 Fe 2 As 2 found a spin excitation that appears at the onset...
We report inelastic x-ray scattering measurements of the temperature dependence of phonon dispersion in the prototypical charge-density-wave (CDW) compound 2H-NbSe2. Surprisingly, acoustic phonons soften to zero frequency and become overdamped over an extended region around the CDW wave vector. This extended phonon collapse is dramatically different from the sharp cusp in the phonon dispersion expected from Fermi surface nesting. Instead, our experiments, combined with ab initio calculations, show that it is the wave vector dependence of the electron-phonon coupling that drives the CDW formation in 2H-NbSe2 and determines its periodicity. This mechanism explains the so far enigmatic behavior of CDW in 2H-NbSe2 and may provide a new approach to other strongly correlated systems where electron-phonon coupling is important.
Hydrous ruthenium oxide (RuO2·xH2O or RuO x H y ) is a mixed proton−electron conductor which could be used in fuel cells and ultracapacitors. Its charge-storage (pseudocapacitance) and electrocatalytic properties vary with water content and are maximized near the composition RuO2·0.5 mol % H2O. We studied the atomic structure of RuO2·xH2O as a function of water content from x = 0.84 to 0.02 using X-ray diffraction and atomic pair density function (PDF). Even though the diffraction patterns of samples containing 0.84 to 0.35 mole of water are suggestive of “amorphous” structures, the PDF analysis clearly shows that up to 0.7 nm, the short-range atomic structure of all of these RuO2·xH2O samples resembles that of the anhydrous rutile RuO2 structure. We conclude that RuO2·xH2O is a composite of anhydrous rutile-like RuO2 nanocrystals dispersed by boundaries of structural water associated with Ru−O. Metallic conduction is supported by the rutile-like nanocrystals, while proton conduction is facilitated by the structural water along the grain boundaries. This structural picture explains the charge-storage and electrocatalytic properties of RuO2·xH2O in terms of competing percolation networks of metallic and protonic conduction pathways, that vary in volume as a function of the water content of the RuO2·xH2O. The control and optimization of electron and proton conducting volumes and pathways will lead to improved performance and guide the design of new materials.
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