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Register a new userSpin correlations and cobalt charge states: A new phase diagram of sodium cobaltates
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Using 23Na NMR measurements on sodium cobaltates at intermediate dopings (0.44<=x<=0.62), we establish the qualitative change of behavior of the local magnetic susceptibility at x*=0.63-0.65, from a low x Pauli-like regime to the high x Curie-Weiss regime. For 0.5<=x<=0.62, the presence of a maximum T* in the temperature dependence of the susceptibility shows the existence of an x-dependent energy scale. T_1 relaxation measurements establish the predominantly antiferromagnetic character of spin correlations for x<x*. This contradicts the commonly assumed uncorrelated Pauli behavior in this x range and is at odds with the observed ferromagnetic correlations for x>x*. It is suggested that at a given x the ferromagnetic correlations might dominate the antiferromagnetic ones above T*. From 59Co NMR data, it is shown that moving towards higher x away from x=0.5 results in the progressive appearance of nonmagnetic Co3+ sites, breaking the homogeneity of Co states encountered for x<=0.5. The main features of the NMR-detected 59Co quadrupolar effects, together with indications from the powder x-ray diffraction data, lead us to sketch a possible structural origin for the Co3+ sites. In light of this ensemble of new experimental observations, a new phase diagram is proposed, taking into account the systematic presence of correlations and their x-dependence.
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We present an explanation for the puzzling spectral and transport properties of layered cobaltates close to the band-insulator limit, which relies on the key effect of charge ordering. Blocking a significant fraction of the lattice sites deeply modifies the electronic structure in a way that is shown to be quantitatively consistent with photoemission experiments. It also makes the system highly sensitive to interactions (especially to intersite ones), hence accounting for the strong correlations effects observed in this regime, such as the high effective mass and quasiparticle scattering rate. These conclusions are supported by a theoretical study of an extended Hubbard model with a realistic band structure on an effective kagom`e lattice.
Metastable self-organized electronic states in quantum materials are of fundamental importance, displaying emergent dynamical properties that may be used in new generations of sensors and memory devices. Such states are typically formed through phase transitions under non-equilibrium conditions and the final state is reached through processes that span a large range of timescales. By using time-resolved optical techniques and femtosecond-pulse-excited scanning tunneling microscopy (STM), the evolution of the metastable states in the quasi-two-dimensional dichalcogenide 1T-TaS2 is mapped out on a temporal phase diagram using the photon density and temperature as control parameters on timescales ranging from 10^(-12) to 10^3 s. The introduction of a time-domain axis in the phase diagram enables us to follow the evolution of metastable emergent states created by different phase transition mechanisms on different timescales, thus enabling comparison with theoretical predictions of the phase diagram and opening the way to understanding of the complex ordering processes in metastable materials.
Recently the unusual metallic state with a substantially non-uniform distribution of a charge and mag-ne-tic density in CoO$_2$ planes was found experimentally in the Na$_x$CoO$_2$ compound with $x>0.6$. We have investigated an origin of such electron disproportionation in the lamellar sodium cobaltates by calculating the ion states as a function of a strength of the electron correlations in the $d$(Co)-shells within the GGA+U approximation for the system with a realistic crystal structure. It was found that the nonuniformity of spin and charge densities are induced by an ordering of the sodium cations and enhanced correlations. Two important magnetic states of cobalt lattice competing with each other at realistic values of the correlation parameter were found~---~low spin hexagons (LS) and higher spin kagome lattice (HS-KSL). In the heterogeneous metallic HS-KSL phase magnetic Co ions form a kagome structure. In LS phase the kagome pattern is decomposed into hexagons and Co ions possess minimal values of their spin. Coexistence of these states could explain the emergence of the disproportionation with the peculiar kagome structure experimentally revealed in previous studies of the cobaltates.
Several experimental and theoretical studies in cobaltates suggest the proximity of the system to charge ordering (CO). We show, qualitatively, in the frame of a $t-V$ model coupled to phonons that optical phonon modes at the $K$ and $M$ points of the Brillouin zone, which involves only $O$-ions displacement around a $Co$-ion, are good candidates to display anomalies due to the CO proximity. If by increasing of $H_2O$ content the system is pushed closer to CO, the mentioned phonon modes should show softening and broadening.
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.
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