The spin-ladder and spin-chain system (La,Y,Sr,Ca)14Cu24O41: Electronic phases,charge and spin dynamics

The quasi-one-dimensional cuprates (La,Y,Sr,Ca)₁₄Cu₂₄O₄₁, consisting of spin-chains and spin-ladders, have attracted much attention, mainly because they represent the first superconducting copper oxide with a non-square lattice. Theoretically, in isolated hole-doped two-leg ladders, superconductivity is tightly associated with the spin gap, although in competition with a charge-density wave (CDW). Indeed, both the gapped spin-liquid and CDW states have been established in the doped spin-ladders of _{Sr14-xCaxCu24O41}${\mathrm{Sr}}_{14-x}{\mathrm{Ca}}_x{\mathrm{Cu}}_{24}{\mathrm{O}}_{41}$, however the relevance of these objects to electronic properties and superconductivity is still subject of intensive discussion. In this treatise, an appreciable set of experimental data is reviewed, which has been acquired in recent years, indicating a variety of magnetic and charge arrangements found in the chains and ladders of underdoped (La,Y)_y(S,Ca)_14−yCu₂₄O₄₁ and fully doped _{Sr14-xCaxCu24O41}${\mathrm{Sr}}_{14-x}{\mathrm{Ca}}_x{\mathrm{Cu}}_{24}{\mathrm{O}}_{41}$. Based on these data, phase diagrams are constructed for the chains of underdoped systems (as a function of La, Y-substitution), as well as for the chains and ladders of the fully doped ones (as a function of Ca-substitution). We try to reconcile contradictory results concerning the charge dynamics in the ladders, like the hole redistribution between ladders and chains, collective modes and pseudogap, field-dependent transport and the temperature scales and doping levels at which the two-dimensional CDW develops in the ladder planes. The remaining open issues are clearly extracted. In the discussion the experimental results are contrasted with theoretical predictions, which allows us to conclude with two important remarks concerning the nature of the competing CDW and superconducting ground states. A density wave in ladders, characterized by a sinusoidal charge modulation, belongs to the class of broken symmetry patterns, which is theoretically predicted for strongly correlated low-dimensional electron systems; however its precise texture and nature is still an open issue. As for superconductivity, the presence of the spin gap in the normal state points towards d  -wave symmetry and magnetic origin of the attractive interaction. However, there is a finite density of mobile quasi-particles that appears for high Ca contents and increases with pressure, concomitantly with increased two-dimensionality and metallicity. For this reason the superconductivity in the doped ladders of _{Sr14-xCaxCu24O41}${\mathrm{Sr}}_{14-x}{\mathrm{Ca}}_x{\mathrm{Cu}}_{24}{\mathrm{O}}_{41}$ which occurs under high pressure cannot simply be a stabilization of the d-wave superconductivity expected for a pure single ladder system.     

Modification of the charge ordering transition in the quasi-one-dimensional conductor (TMTTF)2SbF6 under pressure

We have measured the temperature dependences of the conductance G and the dielectric permittivity ε′ of the (TMTTF)₂SbF₆ compound under a moderate pressure. The maximum of G(T) associated with the Mott-Hubbard localization disappears under pressure. With increasing pressure the peak in ε′(T), corresponding to the charge ordering (CO) phase transition, shifts to lower temperatures and broadens. At pressures above 0.24 GPa, ε′(T) becomes strongly frequency dependent. These modifications are explained in the frame of the extended Hubbard model and a slowing down behavior.     

Charge ordering in amorphous WOx films

We report on the observation of highly anisotropic viscous electronic conducting phase in amorphous WO_1.55 films that occurs below a current (I)- and frequency (f  )-dependent temperature T^∗(I,f)$T^{\ast }(I,f)$. At T<T^∗(I,f)$T<T^{\ast }(I,f)$ the rotational symmetry of randomly disordered electronic background is broken leading to the appearance of mutually perpendicular metallic- and insulating-like states. A rich dynamic behavior of the electronic matter occurring at T<T^∗(I,f)$T<T^{\ast }(I,f)$ provides evidence for an interplay between pinning effects and electron–electron interactions. The results suggest a dynamic crystallization of the disordered electronic matter, viz. formation of sliding Wigner crystal, as well as the occurrence of quantum liquid-like crystal or stripe phase at low drives.     

Synthesis and physical characterization of superconductivity-magnetism crossover compound RuSr2EuCeCu2O10−δ

We carefully studied the nonsuperconducting sample of the magneto-superconducting RuSr₂(Eu_1−xCe_x)Cu₂O_10−δ series with composition RuSr₂EuCeCu₂O_10−δ. This compound seems to exhibit a complex magnetic state as revealed by host of techniques like resistivity, thermopower, magnetic susceptibility, and MR measurements. The studied compound exhibited ferromagnetic like M(H) loops at 5, 20, and 50 K, and semiconductor like electrical conduction down to 5 K, with −MR^7 T of up to 4% at low temperatures. The −MR^7 T decreases fast above 150 K and monotonically becomes close to zero above say 230 K. Below, 150 K −MR^7 T decreases to around 3% monotonically down to 75 K, with further increase to 4% at around 30 K and lastly having a slight decrease below this temperature. The thermopower S(T) behavior closely followed the −MR^7 T steps in terms of d(S/T)/dT slopes. Further, both MR^7 T steps and d(S/T)/dT slopes are found in close vicinity to various magnetic ordering temperatures (T_mag) of this compound.     

Magnetic-Field-Induced Semimetal-Insulator-like Transition in Highly Oriented Pyrolitic Graphite

We report the extraordinarily large positive magnetoresistances （MR, 69400% at 4.5K under a magnetic field of 8.15 T）, de Hass-van Alphen oscillations effect at 10 K and the semimetal-Jnsulator-like transition in a wide range of temperature in highly oriented pyrolitic graphite （HOPG）. Besides a dominating ordinary MR （OMR） mechanism in the free-electron mode, it is realized from qualitative analysis that the Coulomb interacting quasiparticles within graphite layers play some roles. However it is difficult to associate the transition with the simple OMR theory. In order to investigate the possible origins of the transition, further analysis is carried out. It is revealed that the magnetic-field-induced behaviour is responsible for the semimetal-insulator-like transitions in HOPG.     

Improvement of Atomic-Layer-Deposited Al2O3/GaAs Interface Property by Sulfuration and NH3 Thermal Nitridation

Fermi level pinning at the interface between high-h gate dielectric and GaAs induced by unstable native oxides is a major obstacle for high performance GaAs-based metal-oxide-semiconductor （MOS） devices. We demonstrate the improved Al2O3/GaAs interracial characteristics by （NH4）2S immersion and NH3 thermal pretreatment prior to A1203 deposition. X-ray photoelectron spectroscopy （XPS） analysis confirms that sulfuration of GaAs surface by （NH4 ）2S solution can effectively reduce As-O bonds while Ga-O bonds and elemental As still exist at Al2O3 /GaAs interface. However, it is found that N incorporation during the further thermal nitridation on sulfurated GaAs can effectively suppress the native oxides and elemental As in the sequent deposition of Al2O3. Atomic force microscopy （AFM） shows that the further thermal nitridation on sulfurated GaAs surface can also improve the surface roughness.     

Structural and electrical transport properties of ZnxFe3−xO4 thin film deposited on Si (1 1 1) by pulsed-laser deposition

Polycrystalline thin films of Fe_3−xZn_xO₄ (x = 0.0, 0.01 and 0.02) were prepared by pulsed-laser deposition technique on Si (1 1 1) substrate. X-ray diffraction studies of parent as well as Zn doped magnetite show the spinel cubic structure of film with (1 1 1) orientation. The order–disorder transition temperature for Fe₃O₄ thin film with thickness of 150 nm are at 123 K (Si). Zn doping leads to enhancement of resistivity by Zn²⁺ substitution originates from a decrease of the carrier concentration, which do not show the Verwey transition. The Raman spectra for parent Fe₃O₄ on Si (1 1 1) substrate shows all Raman active modes for thin films at energies of T_2g¹, T_2g³, T_2g², and A_1g at 193, 304, 531 and 668 cm⁻¹. It is noticed that the frequency positions of the strongest A_1g mode are at 668.3 cm⁻¹, for all parent Fe₃O₄ thin film shifted at lower wave number as 663.7 for Fe_2.98Zn_0.02O₄ thin film on Si (1 1 1) substrate. The integral intensity at 668 cm⁻¹ increased significantly with decreasing doping concentration and highest for the parent sample, which is due to residual stress stored in the surface.     

Superconductivity in CoSr2(Y1−xCax)Cu2O7+δ

The roles of aliovalent Ca^II-for-Y^III substitution and high-pressure-oxygen annealing in the process of ‘superconducterizing’ the Co-based layered copper oxide, CoSr₂(Y_1−xCa_x)Cu₂O_7+δ (Co-1212), were investigated. The as-air-synthesized samples up to x=0.4 were found essentially oxygen stoichiometric (−0.03≤δ≤0.00). These samples, however, were not superconducting, suggesting that the holes created by the divalent-for-trivalent cation substitution are trapped on Co in the charge reservoir. Ultra-high-pressure heat treatment carried out at 5 GPa and 500 °C for 30 min in the presence of Ag₂O₂ as an excess oxygen source induced bulk superconductivity in these samples. The highest T_c was obtained for the high-oxygen-pressure treated x=0.3 sample at ∼40 K.     

Improved Resistive Switching Characteristics of Ag-Doped ZrO2 Films Fabricated by Sol-Gel Process

Ag-doped and pure ZrO₂ thin films are prepared on Pt/Ti/SiO₂/Si substrates by sol-gel process for resistive random access memory application. The highly reproducible resistive switching is achieved in the 10% Ag-doped ZrO₂ devices. The improved resistive switching behaviour in the Ag doped ZrO₂ devices could be attributed to Ag doping effect on the formation of the stablefilamentary conducting paths. In addition, dual-step reset processes corresponding to three stable resistance states are observed in the 10% Ag doped ZrO₂ devices, which may be implemented for the application of multi-bit storage.     

Revival of metastable behavior in phase separated La0.5Ca0.5MnO3+δ

The La_xCa_1−xMnO_3+δ compositions close to charge ordering (x∼0.5) show a gradual relaxation from a metallic/ferromagnetic state to an insulating/antiferromagnetic state with thermal cycling. Here, we report on the magnetic relaxation in the metastable state and also the revival of the metastable state (in a relaxed sample) due to high temperature thermal treatment. We also show the changes in the magnetization and the thermoelectric power as the revived metastable state is cycled. We find that the changes in the thermoelectric power extend well into the region above the charge ordering temperatures. This suggests that the micro-structural changes accompanying the thermal cycling leave their imprint in the paramagnetic insulating state as well.     

Spontaneous symmetry breaking approach to La2CuO4 properties: Hints for matching the Mott and Slater pictures

Special solutions of the Hartree-Fock (HF) problem for Coulomb interacting electrons described by a simple model of the Cu-O planes in La₂CuO₄ are presented. One of the mean field states obtained, is able to predict some of the most interesting properties of this material, such as its insulator character and the antiferromagnetic order. The natural appearance of pseudogaps in some states of this material is also indicated by another of the HF states obtained. These surprising results follow after eliminating spin and crystal symmetry restrictions usually imposed on the single particle HF orbitals, by employing the rotational invariant formulation of the HF scheme originally introduced by Dirac. Therefore, it is exemplified here, how up to know considered strong correlation effects, can be described by improving the HF solution of the considered system. In other words, it has been argued, that defining correlation effects as the ones shown by the system and not predicted by the HF best (lowest energy) solution, allows to explain important, up to know considered as strong correlation properties, as simple mean field ones. The discussion also helps to clarify the role of the antiferromagnetism and pseudogaps in the physical properties of the HTSC materials and indicates a promising way to start conciliating the Mott and Slater pictures in the physics of the transition metal oxides and other strongly correlated electron systems.     

Low-temperature thermal conductivity in a d-wave superconductor with coexisting charge order: Effect of self-consistent disorder and vertex corrections

Given the experimental evidence of charge order in the underdoped cuprate superconductors, we consider the effect of coexisting charge order on low-temperature thermal transport in a d  -wave superconductor. Using a phenomenological Hamiltonian that describes a two-dimensional system in the presence of a Q=(π,0)$\mathbf{Q}=(\pi \text{,}0)$ charge density wave and d-wave superconducting order, and including the effects of weak impurity scattering, we compute the self-energy of the quasiparticles within the self-consistent Born approximation, and calculate the zero-temperature thermal conductivity using linear response formalism. We find that vertex corrections within the ladder approximation do not significantly modify the bare-bubble result that was previously calculated. However, self-consistent treatment of the disorder does modify the charge-order-dependence of the thermal conductivity tensor, in that the magnitude of charge order required for the system to become effectively gapped is renormalized, generally to a smaller value.     

( Sr / Ca ) 14 Cu 24 O 41 spin ladders studied by NMR under pressure

⁶³Cu-NMR measurements have been performed on two-leg hole-doped spin ladders Sr_14-xCa_xCu₂₄O₄₁ single crystals 0 ? x ? 12 at several pressures up to the pressure domain where the stabilization of a superconducting ground state can be achieved. The data reveal a marked decrease of the spin gap derived from Knight shift measurements upon Ca substitution and also under pressure and confirm the onset of low lying spin excitations around P _c as previously reported. The spin gap in Sr ₂ Ca ₁₂ Cu ₂₄ O ₄₁ is strongly reduced above 20 kbar. However, the data of an experiment performed at P = 36 kbar where superconductivity has been detected at 6.7 K by an inductive technique have shown that a significant amount of spin excitations remains gapped at 80 K when superconductivity sets in. The standard relaxation model with two and three-magnon modes explains fairly well the activated relaxation data in the intermediate temperature regime corresponding to gapped spin excitations using the spin gap data derived from Knight shift experiments. The data of Gaussian relaxation rates of heavily doped samples support the limitation of the coherence length at low temperature by the average distance between doped holes. We discuss the interplay between superconductivity and the spin gap and suggest that these new results support the exciting prospect of superconductivity induced by the interladder tunneling of preformed pairs as long as the pressure remains lower than the pressure corresponding to the maximum of the superconducting critical temperature. Received 8 March 2001 and Received in final form 27 July 2001     

Metal to insulator transition in Mn substituted underdoped NdBa2Cu3O7−y: Evidence of strong charge localization

We have synthesized underdoped NdBa₂Cu₃O_7−y (NBCO) and NdBa₂Cu_3−xMn_xO_7−y (x = 0.1, 0.2, and 0.3) samples. The analysis of the lattice parameters has been done by using the X-ray diffraction (XRD) method. Using the Scanning Electron Microscope (SEM) the granular nature as well as the intergranular networks has been studied. The Energy Dispersive X-ray (EDX) and Rutherford Backscattering Spectroscopy (RBS) studies confirm the substitution of Mn in the Cu-sites. The transport measurements in several undoped and Mn-substituted NBCO samples have been carried out. We have observed an indication of the metal to insulator transition as a result of the strong charge localization induced by Mn substitution. The applicability of various conductivity equations has been verified for comparison. Estimations of the activation energy and localization length have been carried out and discussed.     

High-throughput characterization of local conductivity of Nd0.9Ca0.1Ba2Cu3O7−δ thin film by the low-temperature scanning microwave microscope

We developed a scanning microwave microscope (SμM) designed for high-throughput electric-property screening as well as for rapid construction of electronic phase diagrams at low temperatures. As a sensor probe, we used a high-Qλ/4 coaxial cavity resonator to which a thin needle with ball-tip end was attached. The sensor module was mounted on the low-temperature XYZ stage, which allowed us to map out the change of resonance frequency and quality factor due to the local tip-sample interaction at low temperatures. From the measurements of combinatorial thin films, such as Ti_1−xCo_xO_2−δ and Nd_0.9Ca_0.1Ba₂Cu₃O_7−δ (NCBCO), it was demonstrated that this SμM system has enough performance for the high-throughput characterization of sample conductance under variable temperature conditions.     

Calcium and oxygen doping in Y Ba2Cu3Oy

Both oxygen and calcium play important roles in inducing superconductivity in Y Ba₂Cu₃O_y (YBCO), which is an antiferromagnetic insulator at low O and Ca content. O induces superconductivity in Ca-free YBCO, while Ca does similarly in oxygen-deficient YBCO. For doping oxygen HgO was used as it decomposes at 476 ^°C into Hg, which escapes from the matrix leaving the crystal unaltered, and O, which provide a way to dope O in YBCO. Considering these facts, polycrystalline samples of Y _1−xCa_xBa₂Cu₃O_y with x=0, 0.1 and 0.2 with and without HgO addition were prepared through a solid-state reaction method. The samples were sintered at 950 ^°C in open atmosphere. These synthesized samples were characterized through using the X-ray diffraction technique (XRD) for phase evaluation, scanning electron microscopy (SEM) for grain morphology, energy dispersive X-ray analysis (EDX) for compositional analysis and the four-contact measurement technique for determining the superconducting transition temperature.     

Luminescence and Energy Transfer of Eu^2＋, Mn^2＋ in SrZnP2O7

The SrZnP2OT：Eu^2＋, Mn^2＋ phosphor is synthesized by high temperature solid state reaction. The luminescence properties and the energy transfer between Eu^2＋ and Mn^2＋ are investigated. The emission bands of this phosphor peaked at 42Ohm and 67Ohm are originated from the 5d → 4f transition of Eu^2＋ and from the 4T1 （4G） --〉 6A1 （6S） transit/on of Mn^2＋, respectively. With the increasing Mn^2＋ concentration, the intensity of fixed concentra- tion Eu^2＋ decreases and the intensity of Mn^2＋ also increases. It is suggested that there is an energy transfer from Eu^2＋ to Mn^2＋ in SrZnP2O7 host. According to Dexter＇s energy transfer formula of multipolar interaction, the energy transfer between Eu^2＋ and Mn^2＋ is due to the electric dipole-quadrupole interaction of the resonance transfer.     

Excellent Passivation of p-Type Si Surface by Sol-Gel Al2O3 Films

Al2O3 films with a thickness of about lOOnm synthesized by spin coating and thermally treated are applied for field-induced surface passivation of p-type crystalline silicon. The level of surface passivation is determined by techniques based on photoconductance. An effective surface recombination velocity below lOOcm/s is obtained on 10Ωcm p-type c-Si wafers （Cz Si）. A high density of negative fixed charges in the order of 10^12 cm^-2 is detected in the Al2O3 films and its impact on the level of surface passivation is demonstrated experimentally. Furthermore, a comparison between the surface passivation achieved for thermal SiO2 and plasma enhanced chemical vapor deposition SiNx ：H films on the same c-Si is presented. The high negative fixed charge density explains the excellent passivation of p-type c-S/by Al2O3.     

Electron localization induced by grain boundary disorder in the normal state of high-Tc superconductors

We have studied the effects of superconducting grain boundary disorder on the normal state transport properties of cuprate films. Dip-coated granular YBa₂Cu₃O_7−y (YBaCuO) thick films on polycrystalline MgO substrates were synthesized and networked grains were systematically made less disordered in order to probe the crossover from strong to weak inter-grain disorder. Grain boundary passivation was achieved by metallic inclusions of different forms. We have shown that the normal state of samples exhibit a semiconducting behavior and changes to ‘metallic’ with sharper transitions to the superconducting state as we reduce grain-interfaces disorder, i.e. increase metallic inclusion content. On the basis of electron localization mechanisms, the normal state conductivity is thus shown to undergo a dimensional crossover from 3D to 2D in the frame of the variable-range hopping (VRH) regime. The transition threshold was found to depend on the form of metallic inclusions.     

Frequency dependence of the resistive switching effect in Bi2Sr2CaCu2O8+y/Ag film heterocontacts

In this work we have performed the relaxation studies “in situ” of the electron instability effect (EIE) in the heterostructures based on BSCCO single crystals. The new effect of suppression of EIE or colossal electroresistance via application of an alternating low frequency electric field to the heterojunctions in the BSCCO-based single crystals has been found. It has been shown that the top possible frequencies for observation of the effect are of the order of 10³ Hz. This fact is interpreted as accumulation of the oxygen ions driven by the electric field to the interface. On the other hand, it has been shown that the switching events are limited by two time processes: t≈1 ms and about ten seconds. The first ones are caused by rearrangement of a charge net in the degraded surface at the electric field switching. The latter are caused by oxygen diffusion to vacancies under electric field above some threshold value. The considered experimental data confirm the correlation character of the HTSC properties as Mott systems, which appears in extreme sensitivity to the doping level, in the tendency to phase separation under external actions, in the hysteresis character of the metal-insulator transition.