59Co NMR evidence for charge ordering below T_(CO) approximately 51 K in Na0.5CoO2

The CoO2 layers in NaxCoO2 may be viewed as a spin S=1/2 triangular-lattice doped with charge carriers. The underlying physics of the cobaltates is very similar to that of the high T_(c) cuprates. We will present unequivocal 59Co NMR evidence that below T_(CO) approximately 51 K, the insulating ground state of the itinerant antiferromagnet Na0.5CoO2 (T_(N) approximately 86 K) is induced by charge ordering.     

Charge ordering and magnetopolarons in Na0.82CoO2

Using spectral ellipsometry, we measured the dielectric function of a Na(0.82(2))CoO2 crystal that exhibits bulk antiferromagnetism with T(N)=19.8 K. We identify two prominent transitions as a function of temperature. The first one at 280 K involves marked changes of the electronic and lattice responses that are indicative of charge ordering in the CoO2 layers. The second transition occurs around T(N)=19.8 K and reveals sizable spin-charge coupling. The data are discussed in terms of charge ordering and formation of magnetopolarons due to a charge-induced spin-state transition of adjacent Co3+ ions.     

Infrared spectroscopy of the charge ordering transition of Na0.5CoO2

We report infrared reflectivity study of charge ordering in a Na0.5CoO2 single crystal. In comparison with x=0.7 and 0.85 compounds, we found that the effective carrier density increases systematically with decreasing Na contents. The charge ordering transition only affects the optical spectra below 1000 cm(-1). A hump near 800 cm(-1) develops below 100 K, which is accompanied by the appearance of new lattice modes as well as the strong antiresonance feature of phonon spectra. These observations signify a polaronic characteristic of charge carriers. Below T(co), an optical gap develops at the magnitude of 2Delta approximately 3.5k(B)T(co) (T相似文献   

Charge ordering in charge-compensated Na0.41CoO2 by oxonium ions

Charge ordering behavior is observed in the crystal prepared through the immersion of the Na_0.41CoO₂ crystal in distilled water. Discovery of the charge ordering in the crystal with Na content less than 0.5 indicates that the immersion in water brings about the reduction of the Na_0.41CoO₂. The formal valence of Co changes from +3.59 estimated from the Na content to +3.50, the same as that in Na_0.5CoO₂. The charge compensation is confirmed to arise from the intercalation of the oxonium ions as occurred in the superconducting sodium cobalt oxide bilayer-hydrate [K. Takada, et al. J. Mater. Chem. 14 (2004) 1448]. The charge ordering is the same as that observed in Na_0.5CoO₂. It suggests that the Co valence of +3.50 is necessary for the charge ordering.     

Low to high spin-state transition induced by charge ordering in antiferromagnetic YBaCo2O5

The oxygen-deficient double perovskite YBaCo2O5, containing corner-linked CoO5 square pyramids as principal building units, undergoes a paramagnetic to antiferromagnetic spin ordering at 330 K. This is accompanied by a tetragonal to orthorhombic distortion. Below 220 K orbital ordering and long-range Co(2+)/Co(3+) charge ordering occur as well as a change in the Co2+ spin state from low to high spin. This transition is shown to be very sensitive to the oxygen content of the sample. To our knowledge this is the first observation of a spin-state transition induced by long-range orbital and charge ordering.     

Charge and spin ordering in insulating Na0.5CoO2: effects of correlation and symmetry

Ab initio band theory including correlations due to intra-atomic repulsion is applied to study charge disproportionation and charge and spin ordering in insulating Na0.5CoO2. Various ordering patterns (zigzag and two striped) for four-Co supercells are analyzed before focusing on the observed "out-of-phase stripe" pattern of antiferromagnetic Co4+ spins along charge-ordered stripes. This pattern relieves frustration and shows distinct analogies with the cuprate layers: a bipartite lattice of antialigned spins, with axes at 90degrees angles. Substantial distinctions with cuprates are also discussed, including the tiny gap of a new variant of "charge-transfer" type within the Co 3d system.     

Charge-ordering signatures in the optical properties of beta-Na0.33V2O5

Temperature dependent optical spectra are reported for beta-Na0.33V2O5. The sodium ordering transition at T(Na)=240 K and, in particular, the charge ordering transition at T(MI)=136 K strongly influence the optical spectra. The metal-insulator transition at T(MI) leads to the opening of a pseudogap ( variant Planck's over 2pi omega=1700 cm(-1)) and to the appearance of a large number of optical phonons. These observations and the presence of a midinfrared band (typical for low dimensional metals) strongly suggest that the charge carriers in beta-Na0.33V2O5 are small polarons.     

Static magnetic order in metallic K0.49CoO2

By means of muon-spin spectroscopy, we have found that K0.49CoO2 crystals undergo successive magnetic transitions from a high-T paramagnetic state to a magnetic ordered state below 60 K and then to a second ordered state below 16 K, even though K0.49CoO2 is metallic at least down to 4 K. An isotropic magnetic behavior and wide internal-field distributions suggest the formation of a commensurate helical spin density wave (SDW) state below 16 K, while a linear SDW state is likely to exist above 16 K. It was also found that exhibits a further transition at 150 K presumably due to a change in the spin state of the Co ions. Since the dependence of the internal-field below 60 K was similar to that for Na0.5CoO2, this suggests that magnetic order is more strongly affected by the Co valence than by the interlayer distance or interaction and/or the charge ordering.     

Electronic texture of the thermoelectric oxide Na0.75CoO2

From 59Co and 23Na NMR, we demonstrate the impact of the Na+ vacancy ordering on the cobalt electronic states in Na0.75CoO2: at long time scales, there is neither a disproportionation into 75% Co3+ and 25% Co4+ states, nor a mixed-valence metal with a uniform Co3.25+ state. Instead, the system adopts an intermediate configuration in which 30% of the lattice sites form an ordered pattern of localized Co3+ states. Above 180 K, an anomalous mobility of specific Na+ sites is found to coexist with this electronic texture, suggesting that the formation of the latter may contribute to stabilizing the Na+ ordering. Control of the ion doping in these materials thus appears to be crucial for fine-tuning of their thermoelectric properties.     

Magnetism and superconductivity in Eu0.2Sr0.8(Fe0.86Co0.14)2As2 probed by 75As NMR

We report bulk superconductivity (SC) in Eu(0.2)Sr(0.8)(Fe(0.86)Co(0.14))(2)As(2) single crystals by means of electrical resistivity, magnetic susceptibility and specific heat measurements with T(c) is approximately equal to 20 K and an antiferromagnetic (AFM) ordering of Eu(2+) moments at T(N) is approximately equal to 2.0 K in zero field. (75)As NMR experiments have been performed in the two external field directions (H is parallel to ab) and (H is parallel to c). (75)As-NMR spectra are analysed in terms of first-order quadrupolar interaction. Spin-lattice relaxation rates (1/T(1)) follow a T(3) law in the temperature range 4.2-15 K. There is no signature of a Hebel-Slichter coherence peak just below the SC transition, indicating a non-s-wave or s(±) type of superconductivity. In the temperature range 160-18 K 1/T(1)T follows the C/(T+θ) law reflecting 2D AFM spin fluctuations.     

Disproportionation, metal-insulator transition, and critical interaction strength in Na(1/2)CoO2

Charge disproportionation (CD) and spin differentiation in Na(1/2)CoO2 are studied using the correlated band local-density approximation + Hubbard U (LDA+U) approach. The simultaneous CD and gap opening seen previously is followed in detail through a first-order charge disproportionation transition 2Co(3.5+)-->Co3++Co4+. Disproportionation in the Co a(g) orbital results in half of the ions (Co3+) becoming electronically and magnetically dead, transforming the quarter-filled a(g) system into a half-filled subsystem that subsequently undergoes the observed charge ordering or metal-insulator transition. Comparing with data in the x approximately 0.3 regime suggests the system has moved into the multiband regime where the effective Coulomb repulsion U-->U(eff)=U/sqrt[3] strongly lessens correlation effects.     

Zener polaron ordering variants induced by A-site ordering in half-doped manganites

We have studied the magnetism of the half-doped charge ordered manganite YBaMn2O6. A formation of ferromagnetic plaquettes of four Mn atoms in the charge ordered phase below T_{CO} approximately 480 K is inferred from high temperature magnetic susceptibility data and the magnetic structure, as determined by neutron powder diffraction at T=1.5 K. The results indicate that new fourfold Mn paramagnetic units form between T_{N}相似文献   

Mössbauer study of Na0.82Co0.99Fe0.01O2

We studied by Mössbauer spectroscopy the Na_0.82CoO₂ compound using 1% ⁵⁷Fe as a local probe which substitutes for the Co ions. Mössbauer spectra at T=300 K revealed two sites which correspond to Fe³⁺ and Fe⁴⁺. The existence of two distinct values of the quadrupole splitting instead of a continuous distribution should be related with the charge ordering of Co⁺³, Co⁺⁴ ions and ion ordering of Na(1) and Na(2). Below T=10 K part of the spectrum area, corresponding to Fe⁴⁺ and all of Fe³⁺, displays broad magnetically split spectra arising either from short-range magnetic correlations or from slow electronic spin relaxation.     

Relevance of the Heisenberg-Kitaev model for the honeycomb lattice iridates A2IrO3

Combining thermodynamic measurements with theoretical calculations we demonstrate that the iridates A2IrO3 (A=Na, Li) are magnetically ordered Mott insulators where the magnetism of the effective spin-orbital S=1/2 moments can be captured by a Heisenberg-Kitaev (HK) model with interactions beyond nearest-neighbor exchange. Experimentally, we observe an increase of the Curie-Weiss temperature from θ≈-125 K for Na2IrO3 to θ≈-33 K for Li2IrO3, while the ordering temperature remains roughly the same T(N)≈15 K. Using functional renormalization group calculations we show that this evolution of θ and T(N) as well as the low temperature zigzag magnetic order can be captured within this extended HK model. We estimate that Na2IrO3 is deep in a magnetically ordered regime, while Li2IrO3 appears to be close to a spin-liquid regime.     

Modeling hyperfine parameters observed from the charge-ordered to valence-mixed state of NdBaFe(2)O(5)

Orbital populations of the minority-spin Fe(2+) electron in NdBaFe(2)O(5) are extracted from electric and magnetic hyperfine parameters of (57)Fe M?ssbauer spectra across the temperature interval where charge ordering of the valence state 2.5?+ of iron occurs. The previously used approach that assigns the minority-spin population to a single lowest-energy d orbital is expanded to three orbitals by setting up a system of equations in terms of the Fe(2+)/Fe(3+) balance from isomer shift, a point-charge model for the valence and ligand contributions to the electric-field gradient, a point-dipole model for the dipolar contribution and an iterative scheme for small orbital contributions to the internal magnetic field. This allows us to model the hyperfine fields (electric and magnetic) in the intermediate temperature range of partial charge ordering between T(V )?≈?210?K and T(p)?≈?285?K, for which the one-orbital model was insufficient.     

Nd0.5Ca0.5Mn1-xAlxO3 (x=0,0.03)体系中电荷有序态的超声研究

系统研究了Nd0．5Ca0．5Mn1-xAlxO3(x=0,0．03)单相多晶样品在低温下的电磁性质和超声特性．电阻和磁化率测量表明,Nd0．5Ca0.5O3体系在TCO-257 K处发生了电荷有序相变．超声声速从室温开始随着温度的降低逐渐减小,并在TCO附近达到最小,之后,随着温度的进一步降低,声速急刷增加,同时伴随着一个尖锐的超声衰减峰出现.TCO附近的超声异常表明体系中存在着强烈的电-声子相互作用,该电-声子耦合来源于Mn3 的Jahn-Teller效应．在低温下,出现了另一个超声衰减峰,它的出现归结为反铁磁相与顺磁相之间的相分离现象.随着Al在Mn位的掺入,超声声速的最低点和衰减峰向低温移动,表明体系中的电荷有序态和反铁磁相均被部分抑制,     

Tunneling properties of hybrid magnetoelectric nanoscale devices

The adsorption of alkali atom K and Na on Co(0001) in p(2×2) and (\(\sqrt 3\) × \(\sqrt 3\))R30° phases were studied by periodic density functional theory calculations. It was shown that K and Na adsorption in hollow, bridge and top sites are practically degenerate for the two phases. Optimized geometries for p(2×2)-K and predicted decrease of the work function induced by K are in good agreement with experiments. And our calculations are consistent with the general adsorption picture in comparison with other systems. Detailed analysis of the electronic structures indicates that the decrease of work function upon the adsorption of K and Na can be attributed to the dipole moment associated with the positively polarized alkali atom, which is characterized by the charge depletion from alkali layer and charge accumulation in the interface region. The bonding of K and Na with Co(0001) surface is found to have a metallic bond of covalent character at both 0.25 and 0.33 ML.     

Experimental evidence of coupling interaction between charge ordering and spin ordering

In order to experimentally probe into the complicated interaction between charge ordering and spin ordering in manganites,two sets of samples Nd0.5Sr0.5Mn1-xGaxO3(NSMGO) and Nd 0.5Sr0.5Mn1-y CryO3(NSMCO)(0.0 x,y 0.075),have been studied by means of electrical transport,magnetization,electron spin resonance and transmission electron microscopy analysis.By comparing the influence of Cr-doping and Ga-doping in the Nd0.5Sr0.5MnO3(NSMO) system,large difference between the evolution of charge ordering temperature T co in the Cr-doping and the Ga-doping cases is found.In the NSMCO system,the CE-type antiferromagnetic(AFM)/charge ordering(CO) phase disappears with only 2.5 percent Cr doping;but in the NSMGO system,the CE-type AFM/CO phase always exists.This phenomenon indicates that the charge ordering formation is dominated by the spin ordering.As a result,it is experimentally proved that there is strong coupling interaction between charge ordering and spin ordering in NSMO system.     

Magnetic structure of the ferromagnetic new ternary silicide Nd5CoSi2

Nd(5)CoSi(2) was obtained from the elements by arc-melting followed by annealing at 883 K. Its investigation by single-crystal x-ray and neutron powder diffraction shows that this ternary silicide crystallizes as Nd(5)Si(3) in a tetragonal structure deriving from the Cr(5)B(3)-type (I4/mcm space group; a = 7.7472(2) and c = 13.5981(5) ? as unit cell parameters). The structural refinements confirm the mixed occupancy on the 8h site between Si and Co atoms, as already observed for Gd(5)CoSi(2). Magnetization and specific heat measurements reveal a ferromagnetic behavior below T(C) = 55 K for Nd(5)CoSi(2). This magnetic ordering is further evidenced by neutron powder diffraction investigation revealing between 1.8 K and T(C) a canted ferromagnetic structure in the direction of the c-axis described by a propagation vector k = (0 0 0). At 1.8 K, the two Nd(3+) ions carry ordered magnetic moments equal respectively to 1.67(7) and 2.37(7) μ(B) for Nd1 and Nd2; these two moments exhibit a canting angle of θ = 4.3(6)°. This magnetic structure presents some similarities with that reported for Nd(5)Si(3).     

Doping dependent evolution of magnetism and superconductivity in Eu(1-x)K(x)Fe2As2 (x = 0-1) and temperature dependence of the lower critical field H(c1)

We have synthesized polycrystalline samples of Eu(1-x)K(x)Fe2As2 (x = 0-1) and carried out systematic characterization using x-ray diffraction, ac and dc magnetic susceptibility, and electrical resistivity measurements. A clear signature of the coexistence of a superconducting transition (T(c) = 5.5 K) with spin density wave (SDW) ordering is observed in our underdoped sample with x = 0.15. The SDW transition disappears completely for the x = 0.3 sample and superconductivity arises below 20 K. The superconducting transition temperature Tc increases with increase in the K content and a maximum Tc = 33 K is reached for x = 0.5, beyond which it decreases again. The doping dependent Tx phase diagram is extracted from the magnetic and electrical transport data. It is found that magnetic ordering of Eu moments coexists with the superconductivity up to x = 0.6. The isothermal magnetization data taken at 2 K for the doped samples suggest the 2+ valence state of the Eu ions. We also present the temperature dependence of the lower critical field H(c1) of the superconducting polycrystalline samples. The values of H(c1)(0) obtained for x = 0.3, 0.5, and 0.7 after taking the demagnetization factor into account are 202, 330, and 212 Oe, respectively. The London penetration depth λ(T) calculated from the lower critical field does not show exponential dependence at low temperature, as would be expected for a fully gapped clean s-wave superconductor. In contrast, it shows a T2 power law feature up to T = 0.3Tc, as observed in Ba(1-x)K(x)Fe2As2 and BaFe(2-x)Co(x)As2.