Spin and charge order in Mott insulators and d-wave superconductors

We argue that aspects of the anomalous, low temperature, spin and charge dynamics of the high temperature superconductors can be understood by studying the corresponding physics of undoped Mott insulators. Such insulators display a quantum transition from a magnetically ordered Néel state to a confining paramagnet with a spin gap; the latter state has bond-centered charge order, a low energy S=1 spin exciton, confinement of S=1/2 spinons, and a free S=1/2 moment near non-magnetic impurities. We discuss how these characteristics, and the quantum phase transitions, evolve upon doping the insulator into a d-wave superconductor. This theoretical framework was used to make a number of predictions for STM measurements and for the phase diagram of the doped Mott insulator in an applied magnetic field.     

Critical behavior near the paramagnetic to ferromagnetic phase transition temperature in La0.7Pb0.05Na0.25MnO3

Critical behavior in La_0.7Pb_0.05Na_0.25MnO₃ has been investigated by dc magnetization measurements. Magnetic data indicate that the compound exhibits a continuous (second-order) paramagnetic (PM) to ferromagnetic (FM) phase transition. Estimates of critical exponents yield δ=4.80±0.01, γ=1.296±0.002 and β=0.344±0.007 (consistent with both the predictions for the three-dimensional-Heisenberg model and with those reported for materials when the FM transition is ascribed to the double exchange (DE) mechanism as a major origin) with T_C=334.54±0.08. The critical exponent γ is slightly inferior than predicted from the 3D Heisenberg model. Such a difference may be due, within the context of the quenched disorder, to the presence of some alterations of short-range magnetic order of FM clusters in the PM phase. The temperature variation in the effective exponent (γ_eff) is similar to those for disordered ferromagnets.     

Coexistence of superconductivity and magnetism in the La0.87−xLnxSr0.13FeAsO (Ln=Sm, Gd, Dy) system

The interplay between the superconducting phase and spin density wave order phase was studied. We report the magnetic and superconducting properties of the hole-doped FeAs-based superconducting compound La_0.87−xLn_xSr_0.13FeAsO (Ln=Sm, Gd, Dy; 0≤x≤0.06). Both resistivity and magnetic susceptibility measurements show that the superconducting transition temperature decreases with increase in composition of magnetic ions. The hysteresis loop of the La_0.87−xLn_xSr_0.13FeAsO sample shows a superconducting hysteresis in addition to a paramagnetic background. The experiment demonstrates that the magnetism and superconductivity coexist in hole-doped FeAs-based superconducting compounds. Among these three magnetic rare-earth elements, the influence of Dy³⁺ doping on superconductivity is more evident than that of Gd³⁺ doping, while the influence of Sm³⁺ doping is the weakest. The trend is consistent with the variation of the lattice parameter along c-axis.     

Evolution of electronic structure in Eu1−xLaxFe2As2

We report an angle-resolved photoemission spectroscopy study of electronic structures of Eu_1−xLa_xFe₂As₂ single crystals, in which the spin density wave transition is suppressed with La doping. In the paramagnetic state, the Fermi surface maps are similar for all dopings, with chemical potential shifts corresponding to the extra electrons introduced by the La doping. In the spin density wave state, we identify electronic structure signatures that relate to the spin density wave transition. Bands around M show that the energy of the system is saved by the band shifts towards high energies, and the shifts decrease with increasing doping, in agreement with the weakened magnetic order.     

Magnetism on Mg1−xZnxCyNi3

The magnetic phase diagram for Mg_1−xZn_xC_yNi₃ has been tentatively constructed based on magnetization and muon spin relaxation (μSR) measurements. The superconducting phase was observed to fade as x (y) increases (decreases). The low y samples show early stages of long-range ferromagnetism, or complete long-range ferromagnetism. In the phase diagram, the ferromagnetic phase exists in addition to the superconducting phase, suggesting that there is some correlation between superconductivity and ferromagnetism, even though the coexistence of ferromagnetism and superconductivity is not observed from the μSR measurements down to 20 mK for the superconducting sample (T_c=2.5 K, (x, y)=(0, 0.9)).     

Structure and magnetic properties of perovskite Sr2CuNbO6−δ

Single phase perovskite Sr₂CuNbO_6−δ with a high proportion of Cu¹⁺ ions and oxygen vacancies was synthesized by solid-state reaction. The structure was determined by Rietveld method with space group Pm3m. Isotropic g value was evaluated from electron spin resonance (ESR) measurements. The ESR result is consistent with that of magnetic susceptibility.     

Magnetic structure of geometrically frustrated compound Co2Cl(OH)3 determined by proton NMR

The magnetic structure of a geometrically frustrated system Co₂Cl(OH)₃ is determined by comparing the observed proton NMR spectrum with numerical calculations based on various magnetic models. The best fit is obtained with a model that the magnetic moments of Co²⁺ ions in the triangular plane are parallel to the principal axis of local crystal field and those of Co²⁺ ions in the kagome lattice plane are randomly disordered in the a-b plane, which nearly bisects the angle between the principal axis of the local field and a line pointing towards the body center of the tetrahedron. The coexistence of the ferromagnetic order in the triangular plane and the random disorder in the kagome plane is consistent with the results of measurements by Zheng et al. However, the magnetic moments of Co²⁺ ions are not directed towards the body center of the tetrahedron as characteristic in the “spin ice” magnetic structure. Furthermore, the Co²⁺ ions in the triangular plane have a smaller magnitude of magnetic moment than those in the kagome plane. Thus, our result suggests that the transition metal compound Co₂Cl(OH)₃ is different from the “spin ice” in magnetic structure, although it is similar to rare-earth pyrochlores in crystal structure.     

Charge and spin dynamics in antiferromagnetic metallic phase of iron-based superconductors

The electronic states, charge dynamics, and spin dynamics in the antiferromagnetic metallic phase of iron-arsenide superconductors are investigated by mean-field calculations for a five-band Hubbard model. Taking into account the difference of observed magnetic moments between LaFeAsO (1111 system) and BaFe₂As₂ (122 system), we investigate the effect of the magnitude of the moments on band dispersion, optical conductivity, and dynamical spin susceptibility. We clarify how the magnitude affects on these quantities and predict different behaviors between the 1111 and 122 systems in the antiferromagnetic metallic phase.     

Spin-dependent electron transport in a type II GaInAsSb/p-InAs heterojunction doped with Mn in quantized magnetic fields

We report a study of spin-related magnetotransport properties of a type II broken-gap heterostructure formed by InAs substrate bulky doped with Mn and δ-Mn-doped GaInAsSb epilayer. Planar and vertical quantum magnetotransport in a 2D-electron-hole system at the single type II broken-gap InAs/GaInAsSb heterointerface was investigated in high magnetic fields under the quantum Hall regime up to 15 T at low temperature (T=1.5 K). The I-V characteristics near the dielectric phase boundary show the step-like behavior that corresponds to the quantum conductance in a disordered 2D structure through the extended edge states of the nearest Landau level closest to the Fermi level. The value of these steps is determined by the orientation of the 2D-electron spin at the Landau level and the magnetic moment of Mn in the δ-layer.     

Magnetic disorder induced enhanced magneto-resistance in La0.5Sr0.5Co1−xRuxO3

We observe a sharp increase in negative magneto-resistance ratio up to 40% for x=0.1, in La_0.5Sr_0.5Co_1−xRu_xO₃ which is due to the magnetic disorder induced by an anti-ferromagnetic interaction between Co and Ru ions. We also observe a metal to insulator and a ferromagnetic to anti-ferromagnetic transition for 0≤x≤0.3. Ruthenium (IV) ion disrupts an intermediate spin state of cobalt (Co³⁺:t_2g⁵e_g¹), forcing a double exchange mediated ferromagnetic state to an anti-ferromagnetic spin state for x≥0.2.     

Mössbauer spectroscopic study of the thermal spin crossover in [Fe(II)(isoxazole)6](ClO4)2

The ⁵⁷Fe Mössbauer spectroscopy of mononuclear [Fe(II)(isoxazole)₆](ClO₄)₂ has been studied to reveal the thermal spin crossover of Fe(II) between low-spin (S=0) and high-spin (S=2) states. Temperature-dependent spin transition curves have been constructed with the least-square fitted data obtained from the Mössbauer spectra measured at various temperatures between 84 and 270 K during a cooling and heating cycle. This compound exhibits an unusual temperature-dependent spin transition behaviour with T_C(↓)=223 and T_C(↑)=213 K occurring in the reverse order in comparison to those observed in SQUID observation and many other spin transition compounds. The compound has three high-spin Fe(II) sites at the highest temperature of study of which two undergo spin transitions. The compound seems to undergo a structural phase transition around the spin transition temperature, which plays a significant role in the spin crossover behaviour as well as the magnetic properties of the compound at temperatures below T_C. The present study reveals an increase in high-spin fraction upon heating in the temperature range below T_C, and an explanation is provided.     

Competing phases in the cuprates: Charge vs spin order

We have investigated magnetic and charge instabilities of the cuprates within the Gutzwiller approximation RPA (GA+RPA). Interestingly, in GA the dressed Hubbard U is not a single parameter, but has different forms in the spin and charge responses, with distinct doping dependencies. While there are a number of competing magnetic instabilities for hole-doped cuprates, we fail to find any purely electronic charge density waves. The dominant magnetic instabilities are associated with ‘double nesting’, and the phase diagrams are material dependent, with LSCO differing from other cuprates.     

Cluster spin glass ordering in diluted spinel Zn0.5Co0.5FeCrO4

The disordered spinel system, Zn_0.5Co_0.5FeCrO₄ has been investigated using the low field magnetization and ac susceptibility measurements. From the present results it appears that this system orders into a cluster spin glass state with the magnetic moments of the ferrimagnetic clusters randomly frozen. Compared to the Ni and Co zinc ferrites with the same magnetic dilution, introduction of Cr into the B sites appears to increase the frustration and disorder dramatically. The predicted phase diagrams for the ordering in diluted magnetic spinels do not describe the magnetic behaviour of this system, presumably due to the disorder in the B sublattice in addition to the dilution in the A sublattice.     

Spin gap of a pressure-induced superconductor Sr2Ca12Cu24O41 at an optimum pressure of 3.8 GPa

Nuclear magnetic resonance (NMR) on ⁶³Cu nuclei was performed in a pressure-induced superconductor Sr₂Ca₁₂Cu₂₄O₄₁ at an optimum pressure of 3.8 GPa. A pressure of 3.8 GPa was achieved by improving a piston-cylinder-type pressure cell and developing a NMR probe with a steady-load control system. We found that the spin gap still exists even at the optimum pressure. The spin gap was almost the same at pressures below 3.5 GPa on the pressure-temperature phase diagram, whereas it decreased rather drastically above 3.5 GPa.     

Antiferromagnetic phase transition in garnet-type AgCa2Co2V3O12 and AgCa2Ni2V3O12

Antiferromagnetic phase transition in two vanadium garnets AgCa₂Co₂V₃O₁₂ and AgCa₂Ni₂V₃O₁₂ has been found and investigated extensively. The heat capacity exhibits sharp peak due to the antiferromagnetic order with the Néel temperature T_N=6.39 K for AgCa₂Co₂V₃O₁₂ and 7.21 K for AgCa₂Ni₂V₃O₁₂, respectively. The magnetic susceptibilities exhibit broad maximum, and these T_N correspond to the inflection points of the magnetic susceptibility χ a little lower than T(χ_max). The magnetic entropy changes from zero to 20 K per mol Co²⁺ and Ni²⁺ ions are 5.31 J K⁻¹ mol-Co²⁺-ion⁻¹ and 6.85 J K⁻¹ mol-Ni²⁺-ion⁻¹, indicating S=1/2 for Co²⁺ ion and S=1 for Ni²⁺ ion. The magnetic susceptibility of AgCa₂Ni₂V₃O₁₂ shows the Curie-Weiss behavior between 20 and 350 K with the effective magnetic moment μ_eff=3.23 μ_B Ni²⁺-ion⁻¹ and the Weiss constant θ=−16.4 K (antiferromagnetic sign). Nevertheless, the simple Curie-Weiss law cannot be applicable for AgCa₂Co₂V₃O₁₂. The complex temperature dependence of magnetic susceptibility has been interpreted within the framework of Tanabe-Sugano energy diagram, which is analyzed on the basis of crystalline electric field. The ground state is the spin doublet state ²E(t₂⁶e) and the first excited state is spin quartet state ⁴T₁(t₂⁵e²) which locates extremely close to the ground state. The low spin state S=1/2 for Co²⁺ ion is verified experimentally at least below 20 K which is in agreement with the result of the heat capacity.     

Heat capacities of the electron acceptor 7,7,8,8-tetracyano- quinodimethane (TCNQ) and its radical-ion salt NH4(TCNQ) showing spin-Peierls transition

Heat capacities of the electron acceptor 7,7,8,8-tetracyanoquinodimethane (TCNQ) and its radical-ion salt NH₄-TCNQ have been measured at temperatures in the 12-350 K range by adiabatic calorimetry. A λ-type heat capacity anomaly arising from a spin-Peierls (SP) transition was found at 301.3 K in NH₄-TCNQ. The enthalpy and entropy of transition are Δ_trsH=(667±7) J mol⁻¹ and Δ_trsS=(2.19±0.02) J K⁻¹ mol⁻¹, respectively. The SP transition is characterized by a cooperative coupling between the spin and the phonon systems. By assuming a uniform one-dimensional antiferromagnetic (AF) Heisenberg chains consisting of quantum spin (S=1/2) in the high-temperature phase and an alternating AF nonuniform chains in the low-temperature phase, we estimated the magnetic contribution to the entropy as Δ_trsS_mag=0.61 J K⁻¹ mol⁻¹ and the lattice contribution as Δ_trsS_lat=1.58 J K⁻¹ mol⁻¹. Although the total magnetic entropy expected for the present compound is R ln 2 (=5.76 J K⁻¹ mol⁻¹), a majority of the magnetic entropy (∼4.6 J K⁻¹ mol⁻¹) persists in the high-temperature phase as a short-range-order effect. The present thermodynamic investigation quantitatively revealed the roles played by the spin and the phonon at the SP transition. Standard thermodynamic functions of both compounds have also been determined.     

Study on the competition between density waves, singlet, and triplet pairing superconductivity in organic conductors (TMTSF)2X

We study the effect of dimerization of TMTSF molecules and the effect of magnetic field (Zeeman splitting) on the phase competition in quasi one-dimensional organic superconductors (TMTSF)₂X by applying the random phase approximation method. As for the dimerization effect, we conclude that due to the decrease of the dimerization, which corresponds to applying the pressure and cooling, spin and charge density wave states are suppressed and give way to a superconducting state. As for the magnetic field effect, we find generally that spin-triplet pairing mediated by a coexistence of 2k_F spin and 2k_F charge fluctuations can be strongly enhanced by applying magnetic field rather than triplet pairing due to a ferromagnetic spin fluctuations. Applying the above idea to (TMTSF)₂X compounds, a magnetic field induced singlet-triplet transition is consistent with above mechanism in (TMTSF)₂ClO₄.     

57Fe Mössbauer spectroscopy on FePt invar alloys

From ⁵⁷Fe Mössbauer effect investigations on disordered FePt-Invar alloys we determine the concentration dependence of both the mean isomer shift and the mean magnetic hyperfine field. Evaluating these changes in terms of charge and spin densities at the nuclei and combining the results with X-ray investigations we find the electronic state of the iron atoms being 3d⁷4s¹ in these alloys. We present a “magnetic” phase diagram and discuss the influence of the martensitic transformation.     

Modeling of magnetic susceptibility of an antiferromagnetic system with disorder-driven quantum critical behavior

A simple model has been proposed for an antiferromagnetic system in which the quantum critical regime is induced by disorder. The proposed model makes it possible to find the magnetic susceptibility for an arbitrary ratio of the temperature T to the characteristic magnitude of the exchange integral J in a disordered magnet. The model analytically describes the crossover from the power dependence χ ～ 1/T ^ξ, which is characteristic of the ground state (the Griffiths phase, T ? J), to a dependence of the Curie-Weiss type (T ≥ J) with the effective parameters dependent on the characteristics of the distribution function of the exchange integrals. The characteristic size of spin clusters forming the Griffiths phase has been estimated. It has been demonstrated using iron-doped germanium cuprate as an example that, within the proposed approach, the experimental data can be adequately described over a wide temperature range in which the temperature changes by more than two orders of magnitude and the magnetic properties of the Griffiths phase are determined by spin clusters of nanometer size.     

NMR studies of magnetic superconductor RuSr2RECu2O8 (RE=Gd, Eu and Y)

We have carried out ^99/101Ru and ^63/65Cu nuclear magnetic resonance experiments in order to investigate magnetic and electronic properties of the magnetic superconductor RuSr₂RECu₂O₈ (RE=Gd, Eu and Y). The two kinds of ^99/101Ru signals were observed in the magnetically ordered state for each system, suggesting a charge segregation of Ru⁵⁺ (S=3/2) and Ru⁴⁺ (S=1) ions in the RuO₂ layers. The internal field at the Cu sites is revealed to be of the order of kilo Oe, indicating weak magnetic interactions between the CuO₂ and RuO₂ planes. The temperature dependence of nuclear spin-lattice relaxation time T₁ of ⁶³Cu in RE=Y shows a ‘spin gap’ like behavior, suggesting the system is under-doped.