Spin dynamics and charge order in beta-Na1/3V2O5

We present detailed electron-spin resonance investigations on single crystals of the one-dimensional vanadium-oxide bronze beta-Na(1/3)V2O5. From the angular dependence of the g value it can be concluded that the electrons are primarily located on the V1 zigzag chains. The anisotropy of the linewidth, which is determined by the intrachain symmetric anisotropic exchange interaction, favors statistic electron distribution in the metallic and blockwise charge-order in the insulating phase. The temperature dependence of the linewidth indicates the opening of a charge gap at the metal-to-insulator transition at T(MI)=132 K.     

Zener double exchange from local valence fluctuations in magnetite

Magnetite (Fe3O4) is a mixed valent system where electronic conductivity occurs on the B site (octahedral) iron sublattice of the spinel structure. Below T(V)=123 K, a metal-insulator transition occurs which is argued to arise from the charge ordering of 2+ and 3+ iron valences on the B sites (Verwey transition). Inelastic neutron scattering measurements show that optical spin waves propagating on the B site sublattice (approximately 80 meV) are shifted upwards in energy above T_{V} due to the occurrence of B-B ferromagnetic double exchange in the mixed valent phase. The double exchange interaction affects only spin waves of Delta(5) symmetry, not all modes, indicating that valence fluctuations are slow and the double exchange is constrained by short-range electron correlations above T(V).     

Negative volume thermal expansion via orbital and magnetic orders in Ca₂Ru₁-(x)Cr(x)O₄(0 < x < 0.13)

Ca?RuO? undergoes a metal-insulator transition at T(MI)=357 K, followed by a well-separated transition to antiferromagnetic order at T(N)=110 K. Dilute Cr doping for Ru reduces the temperature of the orthorhombic distortion at T(MI) and induces ferromagnetic behavior at T(C). The lattice volume V of Ca?Ru?-(x)Cr(x)O? (0 < x < 0.13) abruptly expands with cooling at both T(MI) and T(C), giving rise to a total volume expansion ΔV/V ≈ 1%, which sharply contrasts the smooth temperature dependence of the few known examples of negative volume thermal expansion driven by anharmonic phonon modes. In addition, the near absence of volume thermal expansion between T(C) and T(MI) represents an Invar effect. The two phase transitions, which surprisingly mimic the classic freezing transition of water, suggest an exotic ground state driven by an extraordinary coupling between spin, orbit, and lattice degrees of freedom.     

Nonlocal Coulomb correlations in metals close to a charge order insulator transition

The charge ordering transition induced by the nearest-neighbor Coulomb repulsion V in the 1/4-filled extended Hubbard model is investigated using cellular dynamical mean-field theory. We find a transition to a strongly renormalized charge ordered Fermi liquid at V(CO) and a metal-to-insulator transition at V(MI)>V(CO). Short range antiferromagnetism occurs concomitantly with the CO transition. Approaching the charge ordered insulator, V approximately 相似文献   

Evidence for multiband superconductivity in the heavy Fermion compound UNi2Al3

Epitaxial thin films of the heavy fermion superconductor UNi2Al3 with Tc(max)=0.98 K were investigated. The transition temperature Tc depends on the current direction which can be related to superconducting gaps opening at different temperatures. Also the influence of the magnetic ordering at TN approximately 5 K on R(T) is strongly anisotropic, indicating different coupling between the magnetic moments and itinerant charge carriers on the multisheeted Fermi surface. The upper critical field Hc2(T) suggests an unconventional spin-singlet superconducting state.     

Spin-singlet clusters in the ladder compound NaV2O5

The space group of alpha(')-NaV2O5 turns below T(c) = 34 K from Pmmn with all V sites equivalent, into Fmm2 with three independent vanadium sites per layer. This is incompatible with models of charge ordering into V4+ and V5+. Our structure determination indicates that the phase transition consists of a charge ordering with three distinct valence states, formally V4+, V4.5+, and V5+. The singlet formation is not associated with dimerization on the spin ladder, but with the formation of spin clusters. Finally, we ascribe the quadrupling of the c axis to the large polarizability of the V2O5 skeleton.     

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.     

Pressure-induced superconductivity in beta- Na (0.33) V(2)O(5) beyond charge ordering

We report the discovery of a new superconducting phase in highly correlated 3d electron systems. The compound is beta-vanadium bronze, beta- Na0.33V 2O5, in which the charge-ordered phase collapses under hydrostatic high pressure and a pressure-induced superconducting phase appears around T(S C)=8 K, P=8 GPa. This report presents the first observation not only of superconductivity in vanadium oxides but also of a phase transition from charge ordered to superconducting on a pressure-temperature (P- T) plane. The phase diagrams seem to have universal aspects across the classes of materials. This indicates a profound physics of superconductivity in highly correlated electron systems.     

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   

Nonlinear transport in {\sf \beta}-Na 0.33V 2O 5

Transport properties of the charge ordering compound β-Na_0.33V₂O₅ are studied in the temperature range from 30 K to 300 K using current driven DC conductivity experiments. It is found that below the metal-insulator transition temperature ( ) this material shows a nonlinear charge density modulation behavior. The observed conductivity is discussed in terms of a classical domain model for charge density modulation transport.     

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.     

Novel orbital ordering induced by anisotropic stress in a manganite thin film

A novel structure of orbital ordering is found in a Nd0.5Sr0.5MnO3 thin film, which exhibits a clear first-order transition, by synchrotron x-ray diffraction measurements. Lattice parameters vary drastically at the metal-insulator transition at 170 K (= T(MI)), and superlattice reflections appear below 140 K (= T(CO)). The electronic structure between T(MI) and T(CO) is identified as A-type antiferromagnetic with a d(x2-y2) ferro-orbital ordering. The new type of antiferro-orbital ordering characterized by the wave vector (1/4 1/4 1/2) in cubic notation emerges below T(CO). The accommodation of the large lattice distortion at the first-order phase transition and the appearance of the novel orbital ordering are brought about by the anisotropy in the substrate, a new parameter for the phase control.     

Valence transition of YbInCu4 observed in hard X-ray photoemission spectra

Yb 3d and valence-band photoemission spectra of the first-order valence-transition compound YbInCu4 have been measured with hard x ray at an excitation energy of 5.95 keV. Abrupt changes are clearly observed in both spectra around the transition temperature T(V)=42 K, in comparison with ultraviolet and soft x-ray photoemission (VUV-PES and SX-PES) spectra. From the Yb 3d spectra, the Yb valence has been estimated to be approximately 2.90 from 220 down to 50 K and approximately 2.74 at 30-10 K. We propose that Yb 3d hard x-ray photoemission spectroscopy is a very powerful method to estimate the valence of Yb with high accuracy. On the other hand, the Yb2+ 4f-derived peaks in the valence-band spectra exhibit a remarkable enhancement below T(V). The shape of the valence-band spectra is different from those of the VUV-PES and SX-PES spectra above T(V), reflecting the In 5s and 5p contributions.     

One-dimensional instability in BaVS3

The 3d(1) system BaVS3 undergoes a series of remarkable electronic phase transitions. We show that the metal-insulator transition at T(MI)=70 K is associated with a structural transition announced by a huge regime of one-dimensional (1D) lattice fluctuations, detected up to 170 K. These 1D fluctuations correspond to a 2k(F)=c(*)/2 charge-density wave (CDW) instability of the d(z(2)) electron gas. We discuss the formation below T(MI) of an unconventional CDW state involving the condensation of the other V4+ 3d(1) electrons of the quasidegenerate e(t(2g)) orbitals. This study stresses the role of the orbital degrees of freedom in the physics of BaVS3 and reveals the inadequacy of current first principle band calculations to describe its electronic ground state.     

Possible electron-phonon interaction-driven microscopic origin of the phase transitions in β-Na 0.33 V 2 O 5 and analogues

The microscopic origin of the various phase transitions which have been observed in g-Na 0.33 V 2 O 5 and its analogues can be explored experimentally by investigating the oxygen isotope effect on the phase transition temperatures. An absent oxygen isotope effect on the sodium-ordering transition would point to an antiferroelectrically driven instability, while a large isotope effect on the charge ordering and spin ordering transition temperatures would suggest the formation of a charge-density wave instability and phonon mediated long-range magnetic ordering. All instabilities can be attributed to strong electron-phonon interaction effects, which dominate the ground-state properties.     

Probing spin correlations with phonons in the strongly frustrated magnet ZnCr2O4

The spin-lattice coupling plays an important role in strongly frustrated magnets. In ZnCr2O4, an excellent realization of the Heisenberg antiferromagnet on the pyrochlore network, a lattice distortion relieves the geometrical frustration through a spin-Peierls-like phase transition at T(c)=12.5 K. Conversely, spin correlations strongly influence the elastic properties of a frustrated magnet. By using infrared spectroscopy and published data on magnetic specific heat, we demonstrate that the frequency of an optical phonon triplet in ZnCr2O4 tracks the nearest-neighbor spin correlations above T(c). The splitting of the phonon triplet below T(c) provides a way to measure the spin-Peierls order parameter.     

X-Ray anomalous scattering study of a charge-ordered state in NaV2O5

Charge ordering of V4+ and V5+ in NaV2O5 has been studied by an x-ray diffraction technique using anomalous scattering near a vanadium K-absorption edge to critically enhance a contrast between the two ions. A dramatic energy dependence of the superlattice intensities is observed below T(C) = 35 K. The charge ordering pattern is the fully charged zigzag-type ladder with the unit cell 2ax2bx4c, but not the chain-type originally proposed for the spin-Peierls state. Charge disproportionation suggested in our model as the average valence V(4.5+/-delta(c)/2) is observed below T(C), showing continuous variation of delta(c) as a function of temperature.     

Two dimensional ordering and fluctuations in alpha(')-NaV2O5

X-ray diffraction measurements of Bragg and diffuse scattering associated with charge ordering in the inorganic compound alpha(')- NaV2O5 show a continuous phase transition at a temperature of about 33.1 K. Many of this material's properties suggest a spin-Peierls transition, as established in CuGeO3 and MEM(TCNQ)(2). We compare the order parameter as well as fluctuations in the order parameter in these materials, and conclude that alpha(')- NaV2O5 is dissimilar, and that the transition is two dimensional in nature, due to charge ordering associated with the fractional average valence at the vanadium site within the orthorhombic a- b plane.     

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.     

Coherent magnetic oscillation in the spin ladder system alpha(')- NaV2O5

We report the first observation of coherent magnetic excitations in a spin ladder system NaV2O5 by using femtosecond time-domain spectroscopy. A pronounced coherent oscillation is observed at 127 cm(-1) (nearly twice the spin gap energy) and assigned to a two-magnon bound state, based on the temperature dependence of the intensity below the charge ordering phase transition at T(C) = 34 K. This mode can be observable only when circularly polarized light is used as a pump or a probe beam, suggesting that it corresponds to a spin-flip excitation from the singlet ground state. A phonon mode strongly coupled to the spin state is also found at 303 cm(-1).