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Register a new userThe Parent of Misfit-Layered Cobalt Oxides: [Sr2O2]qCoO2
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Misfit-layered (ML) cobalt oxides of the general formula of [MmA2Om+2]qCoO2 have been proven to be efficient thermoelectric materials as the structure is capable in accommodating the two seemingly contradictory characteristics of high electrical conductivity and large thermo-electric power. They are also potential hosts for other oxymoron-like functions. The known phases all contain one or two square-planar MO (M = Co, Bi, Pb, Tl, etc.) layers sandwiched together with AO (A = Ca, Sr, Ba, etc.) planes of square symmetry and CoO2 layers of hexagonal symmetry. Here we report realization of the simplest (m = 0) ML phase forming in the Sr-Co-O system with the cation ratio, Sr/Co = 1. Atomic-resolution TEM imaging confirms for the new phase the parent three-layer crystal structure, SrO-SrO-CoO2, which is compatible with the formula of [Sr2O2]qCoO2. Electron diffraction reveals that the phase is rather commensurate, i.e. the misfit parameter q is 0.5. Nevertheless, in terms of the transport-property characteristics the new ML parent is comparable to its earlier-established and more complex derivatives.
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We investigate both thermoelectric and thermodynamic properties of the misfit cobalt oxide [Bi$_{1.7}$Co$_{0.3}$Ca$_{2}$O$_{4}$]$^{RS}_{0.6}$CoO$_{2}$. A large negative magnetothermopower is found to scale with both magnetic field and temperature revealing a significant spin entropy contribution to thermoelectric properties giving rise to a constant S$_0approx$ 60 $mu$V K$^{-1}$ equal to the high temperature asymptotic value of the spin 1/2 entropy. Low temperature specific heat measurements allow us to determine an enhanced electronic part with $gammaapprox$ 50 mJ (mol K$^{2}$)$^{-1}$ attesting of strong correlations. Thereby, a critical comparison between [Bi$_{1.7}$Co$_{0.3}$Ca$_{2}$O$_{4}$]$^{RS}_{0.6}$CoO$_{2}$, other cobaltites as well as other materials reveals a universal behavior of the thermopower low temperature slope as a function of $gamma$ testifying thus a purely electronic origin. This potentially generic scaling behavior suggests here that the high room temperature value of the thermopower in misfit cobalt oxides results from the addition of a spin entropy contribution to an enlarged electronic one.
The results of DC magnetization measurements under hydrostatic (helium-gas) pressure are reported for an ambient pressure superconductor Na0.35CoO2.1.4D2O and its precursor compound, the gamma-phase Na0.75CoO2 that is known to combine a metallic conductivity with an unusual magnetic state below ~22K. The obtained data allowed us to present for the first time the pressure dependence of the magnetic transition in a metallic sodium cobaltate system. This dependence appears to be positive, with the magnetic transition rapidly shifting towards higher temperatures when an applied pressure increases. We ascribe the observed effect to the pressure-induced enhancement of the out-of-plane antiferromagnetic coupling mediated by localized spins interactions (of either superexchange or RKKY type), the scenario consistent with the A-type antiferromagnetic state suggested by recent neutron-scattering data. As for the pressure effect on the superconductivity in Na0.35CoO2.1.4D2O, our measurements established negative and linear for the entire pressure range from 1 bar to 8.3 kbar pressure dependence of Tc, the behavior quite different from the reported by previous workers strong non-linearity of the Tc (P) dependence. (Dated September 12, 2005) PACS numbers: 74.62.Fj, 74.70.-b, 75.20. En, 75.50 Ee, 75.30 Kz.
Relativistic massless Dirac fermions can be probed with high-energy physics experiments, but appear also as low-energy quasi-particle excitations in electronic band structures. In condensed matter systems, their massless nature can be protected by crystal symmetries. Classification of such symmetry-protected relativistic band degeneracies has been fruitful, although many of the predicted quasi-particles still await their experimental discovery. Here we reveal, using angle-resolved photoemission spectroscopy, the existence of two-dimensional type-II Dirac fermions in the high-temperature superconductor La$_{1.77}$Sr$_{0.23}$CuO$_4$. The Dirac point, constituting the crossing of $d_{x^2-y^2}$ and $d_{z^2}$ bands, is found approximately one electronvolt below the Fermi level ($E_mathrm{F}$) and is protected by mirror symmetry. If spin-orbit coupling is considered, the Dirac point degeneracy is lifted and the bands acquire a topologically non-trivial character. In certain nickelate systems, band structure calculations suggest that the same type-II Dirac fermions can be realised near $E_mathrm{F}$.
Intriguing properties of the misfit layered chalcogenide (LaS)$_{1.196}$VS$_2$ crystals were investigated by transport, optical measurements, angle-resolved photoemission (ARPES) and x-ray diffraction. Although no clear anomaly is found in transport properties as a function of temperature, a large spectral weight transfer, up to at least 1 eV, is observed by both optical and photoemission spectroscopies. ARPES reveals that a nearly filled band with negative curvature, close enough from the Fermi level at 300K to produce metallic-like behaviour as observed in optical conductivity spectra. At low temperature, the band structure is strongly modified, yielding to an insulating state with a optical gap of 120 meV. An accurate (3+1)D analysis of x-ray diffraction data shows that, although a phase transition does not occur, structural distortions increase as temperature is decreased, and vanadium clusterization is enhanced. We found that the changes of electronic properties and structure are intimately related. This indicates that structural distorsion play a major role in the insulating nature of (LaS)$_{1.196}$VS$_2$ and that electronic correlation may not be important, contrary to previous belief. These results shed a new light on the mechanism at the origin of non-linear electric properties observed in (LaS)$_{1.196}$VS$_2$.
The magnetic excitations in the cuprate superconductors might be essential for an understanding of high-temperature superconductivity. In these cuprate superconductors the magnetic excitation spectrum resembles an hour-glass and certain resonant magnetic excitations within are believed to be connected to the pairing mechanism which is corroborated by the observation of a universal linear scaling of superconducting gap and magnetic resonance energy. So far, charge stripes are widely believed to be involved in the physics of hour-glass spectra. Here we study an isostructural cobaltate that also exhibits an hour-glass magnetic spectrum. Instead of the expected charge stripe order we observe nano phase separation and unravel a microscopically split origin of hour-glass spectra on the nano scale pointing to a connection between the magnetic resonance peak and the spin gap originating in islands of the antiferromagnetic parent insulator. Our findings open new ways to theories of magnetic excitations and superconductivity in cuprate superconductors.
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