Charge-orbital ordering and Verwey transition in magnetite measured by resonant soft X-ray scattering

We report experimental evidence for the charge-orbital ordering in magnetite below the Verwey transition temperature T(V). Measurements of O K-edge resonant x-ray scattering on magnetite reveal that the O 2p states in the vicinity of the Fermi level exhibit a charge-orbital ordering along the c axis with a spatial periodicity of the doubled lattice parameter of the undistorted cubic phase. Such a charge-orbital ordering vanishes abruptly above T(V) and exhibits a thermal hysteresis, correlating closely with the Verwey transition in magnetite.     

New phase transition in the Pr1-xCaxMnO3 system: evidence for electrical polarization in charge ordered manganites

In this Letter a detailed study of the electric field gradient (EFG) across the Pr(1-x)Ca(x)MnO(3) phase diagram and its temperature dependence is given. Clearly, distinct EFG behavior for samples outside or inside the charge order (CO) region are observed. The EFG temperature dependence evidences a new phase transition occurring over the broad CO region of the phase diagram. This transition is discontinuous and occurs at temperatures between the charge ordering and the Néel temperatures. The prominent features observed in the EFG are associated with polar atomic vibrations which eventually lead to a spontaneous local electric polarization below CO transition.     

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.     

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.     

Cooperative Jahn-Teller phase transition in LaMnO3 studied by X-ray absorption spectroscopy

The local structure of LaMnO3 across the Jahn-Teller (JT) transition at T(JT)=750 K was studied by means of x-ray absorption near edge structure and extended x-ray absorption fine structure at the Mn K-edge. Our results indicate a similar electronic local structure for Mn atoms above and below T(JT) and a dynamical tetragonal JT distortion of MnO6 octahedra above T(JT). The structural transition is originated by the ordering of tetragonally distorted octahedra. The entropy content of the transition is analyzed within the framework of the three-state Potts model with nearest neighbor antiferrodistortive coupling.     

Charge ordering due to magnetic symmetry breaking

It is argued that both transitions observed in 50% doped manganites, at the Néel temperature (T(N)) and the so-called charge ordering temperature (T(CO)), are magnetic. T(N) corresponds to the order-disorder transition, which takes place between ferromagnetic zigzag chains, while the coherent motion of spins within the chains is destroyed only around T(CO). The magnetic structure below T(CO) is highly anisotropic. It is dressed by the lattice distortion and leads to the huge anisotropy of the electronic structure, which explains stability of this state as well as the form of the charge-orbital pattern above T(N). The type of phase transition at T=T(N) is determined by lattice interactions.     

Two-dimensional superconducting fluctuations in stripe-ordered La1.875Ba0.125CuO4

Recent spectroscopic observations of a d-wave-like gap in stripe-ordered La(2-x)Ba(x)CuO(4) with x=1/8 have led us to critically analyze the anisotropic transport and magnetization properties of this material. The data suggest that concomitant with the spin ordering is an electronic decoupling of the CuO(2) planes. We observe a transition (or crossover) to a state of two-dimensional (2D) fluctuating superconductivity, which eventually reaches a 2D superconducting state below a Berezinskii-Kosterlitz-Thouless transition. Thus, it appears that the stripe order in La(2-x)Ba(x)CuO(4) frustrates three-dimensional superconducting phase order, but is fully compatible with 2D superconductivity and an enhanced T(c).     

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   

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).     

Antiferromagnetic spin fluctuations above the dome-shaped and full-gap superconducting states of LaFeAsO1-xFx revealed by (75)As-nuclear quadrupole resonance

We report a systematic study by (75)As nuclear-quadrupole resonance in LaFeAsO(1-x)F(x). The antiferromagnetic spin fluctuation found above the magnetic ordering temperature T(N) = 58 K for x = 0.03 persists in the regime 0.04 ≤ x ≤ 0.08, where superconductivity sets in. A dome-shaped x dependence of the superconducting transition temperature T(c) is found, with the highest T(c) = 27 K at x = 0.06, which is realized under significant antiferromagnetic spin fluctuation. With increasing x further, the antiferromagnetic spin fluctuation decreases, and so does T(c). These features resemble closely the cuprates La(2-x)Sr(x)CuO(4). In x = 0.06, the spin-lattice relaxation rate (1/T(1)) below T(c) decreases exponentially down to 0.13T(c), which unambiguously indicates that the energy gaps are fully opened. The temperature variation of 1/T(1) below T(c) is rendered nonexponential for other x by impurity scattering.     

A new interpretation of the CO state in half-doped manganites: new results from neutron diffraction and synchrotron radiation experiments

In the R_1−xD_xMnO₃ (x0.5) manganites, the structural phase transition at T_CO is commonly interpreted as a concomitant charge and orbital ordering (CO/OO) process driven by a co-operative Jahn–Teller effect and Coulomb repulsion forces. The low-temperature phase is supposed to contain well-separated and ordered Mn³⁺ and Mn⁴⁺ ionic species in an NaCl-like pattern. Structure refinement, from a neutron diffraction experiment below T_CO on a Pr_0.6Ca_0.4MnO₃ single crystal, gives us a model for the displacement of atoms with respect to the high-temperature phase that invalidates the standard model based in the CO/OO picture. Our result is a non-centrosymmetric crystal structure with two non-equivalent MnO₆ octahedra, both being slightly elongated but displaying very similar average Mn–O distances (1.96 and 1.95 Å, respectively) and having off-centered Mn atoms. We argue that this is a proof of the absence of charge ordering in half-doped manganites in the sense of formation of separated Mn³⁺ and Mn⁴⁺ ionic species. A new qualitative interpretation of the CE-type spin ordering (SO) is proposed. The so-called CO transition is, in fact, a structural transition induced by the change in the mean free path of electrons that continue to be thermally activated below T_CO by forming ferromagnetic Mn–Mn pairs stabilized by a local double-exchange process. The CE SO pattern results from the ordering of these pairs formed at T_CO. High-resolution synchrotron powder diffraction shows a complex anisotropic/asymmetric strains appearing at the transition that can be phenomenologically fitted by additional phases. Complementary electron diffraction and microscopy have shown no trace of macroscopic phase separation.     

Magnetic scattering of spin polarized carriers in (In, Mn)Sb dilute magnetic semiconductor

Magnetoresistance measurements on the magnetic semiconductor (In, Mn)Sb suggest that magnetic scattering in this material is dominated by isolated Mn2+ ions located outside the ferromagnetically ordered regions when the system is below T(c). A model is proposed, based on the p-d exchange between spin-polarized charge carriers and localized Mn2+ ions, which accounts for the observed behavior both below and above the ferromagnetic phase transition. The suggested picture is further verified by high-pressure experiments, in which the degree of magnetic interaction can be varied in a controlled way.     

Magnetite, a model system for mixed-valence oxides, does not show charge ordering

We have investigated the charge ordering (CO) in magnetite below the Verwey transition. A new set of half-integer and mixed-integer superlattice reflections of the low-temperature phase have been studied by x-ray resonant scattering. None of these reflections show features characteristic of CO. We demonstrate the absence of CO along the c axis with the periodicity of either the cubic lattice q=(001) or the doubled cubic lattice q=(001/2). This result suggests that the Verwey transition is caused by strong electron-phonon interaction instead of an electronic ordering on the octahedral Fe atoms.     

(1)H and (87)Rb nuclear magnetic resonance study of the order-disorder phase transition of RbHSeO(4) single crystals

The ferroelectric phase transition at T(C2) (=370K) in RbHSeO(4) has been studied by (1)H and (87)Rb solid-state NMR. Although not large, the spin-lattice relaxation time, T(1), and the spin-spin relaxation time, T(2), of rubidium and of the alpha- and beta-type protons show distinct change near the phase transition. The intensity of the signal due to the alpha-type protons decreases with increasing temperature, and the intensity of alpha-type protons is quite weak above 330K: at a temperature which is about 40K lower than the phase transition temperature, the ordering of the alpha-type protons occurs. The alpha-type protons in the ferroelectric phase lead to a noticeable change in the proton magnetic resonance spectra. Our study of the (1)H spectra shows that the ferroelectric phase transition in RbHSeO(4) is of order-disorder type and is due to the ordering of protons in hydrogen bonds.     

NMR evidence for a "Generalized spin-peierls Transition" in the high-magnetic-field phase of the spin ladder Cu2(C5H12N2)2Cl4

The magnetic-field-induced 3D ordered phase of the two-leg spin ladder Cu2(C5H12N2)2Cl4 has been probed through measurements of 1H NMR spectra and 1/T1 in the temperature range 70 mK-1.2 K. The second order transition line T(c)(H) has been determined between H(c1) = 7.52 T and H(c2) = 13.5 T and varies as (H-H(c1))(2/3) close to H(c1). From the observation of anomalous shifts and a crossover in 1/T1 above T(c), the mechanism of the 3D transition is argued to be magnetoelastic as in spin-Peierls chains, here involving a displacement of the protons along the longitudinal exchange ( J( parallel)) path.     

Unveiling the nature of three-dimensional orbital ordering transitions: the case of e(g) and t(2g) models on the cubic lattice

We perform large scale finite-temperature Monte Carlo simulations of the classical e(g) and t(2g) orbital models on the simple cubic lattice in three dimensions. The e(g) model displays a continuous phase transition to an orbitally ordered phase. While the correlation length exponent ν ≈ 0.66(1) is close to the 3D XY value, the exponent η ≈ 0.15(1) differs substantially from O(N) values. At T(c) a U(1) symmetry emerges, which persists for T < T(c) below a crossover length scaling as Λ ～ ξ(a), with an unusually small a ≈ 1.3. Finally, for the t(2g) model we find a first order transition into a low-temperature lattice-nematic phase without orbital order.     

Two-dimensional charge order in layered 2-1-4 perovskite oxides

Monte Carlo simulations are performed on the three-dimensional (3D) Ising model with the 2-1-4 layered perovskite structure as a minimal model for checkerboard charge ordering phenomena in layered perovskite oxides. Because of the interlayer frustration, only 2D long-range order emerges with a finite correlation length along the c axis. Critical exponents of the transition change continuously as a function of the interlayer coupling constant. The interlayer long-range Coulomb interaction decays exponentially and is negligible even between the second-neighbor layers. Instead, monoclinic distortion of a tetragonal unit cell lifts the macroscopic degeneracy to induce a 3D charge ordering. The dimensionality of the charge order in La0.5Sr1.5MnO4 is discussed from this viewpoint.     

Jahn-Teller phonon anomaly and dynamic phase fluctuations in La0.7Ca0.3MnO3

Inelastic neutron scattering was used to study the temperature (T) dependence of the lattice excitations in La 0.7Ca 0.3MnO (3). An optical Jahn-Teller phonon exhibits continuous but anomalous damping with increasing temperature in the ferromagnetic-metallic phase and collapses above the Curie temperature T(C) (240 K). We attribute this anomaly to the growing dynamic phase segregation as T-->T(C), thus providing evidence of local fluctuations associated with the short-range polaron or charge/orbital ordering in the ferromagnetic-metallic state.     

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.     

Raman scattering study of anomalous spin, charge, and lattice dynamics in the charge-ordered phase of Bi1-xCaxMnO3 (x > 0.5)

We report an inelastic light scattering study of the effects of charge ordering on the spin, charge, and lattice dynamics of Bi1-xCaxMnO3 (x>0.5). We find that charge ordering results in anomalous phonon behavior, such as the appearance of "activated" modes. More significantly, however, the transition to the charge-ordered phase results in the appearance of a quasielastic scattering response with the symmetry of the spin-chirality operator ( T(1g)); this scattering response is thus indicative of magnetic or chiral spin fluctuations in the antiferromagnetic charge-ordered phase.