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Register a new userUnusual electron correlations in NaxCoO2 due to the spin-state quasidegeneracy of cobalt ions
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Ji\\v{r}\\'i Chaloupka
Publication date
2008
fields
Physics
and research's language is
English
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Recent studies exposed many remarkable properties of layered cobaltates NaxCoO2. Surprisingly, many-body effects have been found to increase at sodium-rich compositions of NaxCoO2 where one expects a simple, nearly free motion of the dilute S=1/2 holes doped into a band insulator NaCoO2. Here we discuss the origin of enigmatic correlations that turn a doped NaCoO2 into a strongly correlated electronic system. A minimal model including orbital degeneracy is proposed and its predictions are discussed. The model is based on a key property of cobalt oxides - the spin-state quasidegeneracy of CoO6 octahedral complex - which has been known, e.g., in the context of an unusual physics of LaCoO3 compound. Another important ingredient of the model is the 90-degree Co-O-Co bonding in NaxCoO2 which allows nearest-neighbor $t_{2g}-e_g$ hopping. This hopping introduces a dynamical mixture of electronic configurations $t_{2g}^6, S=0$ and $t_{2g}^5e_g^1, S=1$ of neighboring cobalt ions. We show that scattering of charge carriers on spin-state fluctuations suppresses their coherent motion and leads to the spin-polaron physics at $xsim 1$. At larger doping when coherent fermionic bands are formed, the model predicts singlet superconductivity of extended s-wave symmetry. The presence of low-lying spin states of Co$^{3+}$ is essential for the pairing mechanism. Implications of the model for magnetic orderings are also discussed.
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The sodium reordering in NaxCoO2 in the vicinity of room temperature is rationalized at high x in terms of phase transitions between square and striped phases. A striking hexagon-of-hexagons diffraction pattern observed for x=0.78 can be reproduced using coexisting square and striped phases that are related by simple shear deformations. All compositions exhibit a partial melting transition to a disordered stripe phase just below room temperature, which alters the topology of the electrical conduction pathways.
Here we present results of accurate wet-chemical redox analyses, revealing that the oxidation number of cobalt in the newly discovered CoO2-layer superconductor, NaxCoO2 yH2O (x ~ 0.36, y ~ 1.3) is ~ 3.46. This value is significantly lower than the one (~ 3.64) expected on the basis of the value determined for the Na to Co stoichiometry ratio, x. The lower-than-expected value for the Co oxidation state may be alternatively explained by presence of oxygen vacancies or excess protons. Moreover, the result implies that rather than an electron-doped Co(IV) lattice the phase should be considered as a hole-doped Co(III) lattice.
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.
We investigate the normal state of the 11 iron-based superconductor FeSe0.42Te0.58 by angle resolved photoemission. Our data reveal a highly renormalized quasiparticle dispersion characteristic of a strongly correlated metal. We find sheet dependent effective carrier masses between ~ 3 - 16 m_e corresponding to a mass enhancement over band structure values of m*/m_band ~ 6 - 20. This is nearly an order of magnitude higher than the renormalization reported previously for iron-arsenide superconductors of the 1111 and 122 families but fully consistent with the bulk specific heat.
Magnetic susceptibility, transport and heat capacity measurements of single crystal NaxCoO2 (x=0.71) are reported. A transition to a spin density wave (SDW) state at Tmag = 22 K is observable in all measurements, except chi(ac) data in which a cusp is observed at 4 K and attributed to a low temperature glassy phase. M(H) loops are hysteretic below 15 K. Both the SDW transition and low temperature hysteresis are only visible along the c-axis. The system also exhibits a substantial (~40%) positive magnetoresistance below this temperature. Calculations of the electronic heat capacity gamma above and below Tmag and the size of the jump in C indicate that the onset of the SDW brings about the opening of gap and the removal of part of the Fermi surface. Reduced in-plane electron-electron scattering counteracts the loss of carriers below the transition and as a result we see a net reduction in resistivity below Tmag. Sodium ordering transitions at higher temperatures are observable as peaks in the heat capacity with a corresponding increase in resistivity.
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