Interplay of structure and magnetism in ruthenocuprates: a Raman scattering and dilatometry study

We present a Raman scattering and dilatometry study of polycrystalline samples of the magnetic superconducting ruthenocuprates RuSr₂Gd_2−xCe_xCu₂O_10+δ (RuGd₁₂₂₂) and RuSr₂GdCu₂O₈ (RuGd₁₂₁₂). In the Raman spectra a high-temperature diffusive-like laser-tail develops below the magnetic ordering temperature (T_M) into an underdamped peak which shifts up to 130 cm⁻¹. A line assigned to O(Ru) phonons hardens, narrows and strengthens strongly below T_M. Finally, a phonon peak appears below T_M at 590 cm⁻¹. These three magnetic-order-dependent features are observed for RuGd₁₂₁₂ and for RuGd₁₂₂₂ with x=1.0, but do not appear for x=0.5. Dilatometry measurements, on the other hand, evidence a change of the expansion coefficient at T_M. These results point to a structural effect accompanying the magnetic order, and suggest a complex interplay of spin and lattice degrees of freedom in these ruthenocuprates.     

Tuning the multiferroic properties of Pb(Fe1/2Nb1/2)O3 by cationic substitution

A series of substituted lead iron niobate compounds with the general formula Pb²⁺_(1−x)A^Z_x(Fe_{{(1−(2−Z)x)/2}}Nb_{{(1+(2−Z)x)/2}})O₃ (0<x<0.6 and A=La³⁺, K⁺ or Sr²⁺) were prepared by a modified solid-state synthesis. The relative concentrations of Fe³⁺ and Nb⁵⁺ were adjusted to compensate the charge imbalance due to the aliovalent substitution. The dielectric constant and magnetic susceptibilities were studied as a function of temperature. The temperature of the dielectric maximum, T_M, of the substituted compounds decreased linearly with increasing concentration of the substituent ions. The magnetic measurements showed an antiferromagnetic transition at temperatures T_N1 due to the superexchange interactions mediated by Fe–O–Fe and an additional antiferromagnetic-type transition at T_N2. T_N1 linearly increased with the increasing concentration of Fe³⁺ ion at the B-site of ABO₃-type substituted compounds. T_M is shown to be directly dependent on the concentration of the ferroactive Nb⁵⁺ ions at the B-site and Pb²⁺ ions at the A-site.     

Aspects of “low field” magnetotransport in epitaxial thin films of the ferromagnetic metallic oxide SrRuO3

Epitaxial thin films of the conductive ferromagnetic oxide SrRuO₃ were grown on an (0 0 1) SrTiO₃ (STO) substrate by using DC sputtering technique. The magnetic and magnetoresistive properties of the films were measured by applying the magnetic field both perpendicular (out-of-plane) and parallel (in-plane) to the film plane and ever maintaining the direction of the applied field perpendicular to that of the transport current. The films grown on an (0 0 1) STO substrate showed identical magnetization properties in two orthogonal crystallographic directions of the substrate, [1 0 0]_S and [0 0 1]_S (in-plane and out-of-plane geometry), which suggests the presence of a multi domain structure within the plane of the film. For such samples, no anisotropic field (hard axis) along de [0 0 1]s direction, i.e., perpendicular to the film-plane could be detected. Nevertheless, a distinguishable temperature dependent out-of-plane anisotropic magnetoresistance (MR) along with strong temperature dependent low field hysteretic MR(H) behavior was detected for the studied films. A negative MR ratio MR(T)=[ρ(μ₀H=9 T; T)−ρ( μ₀H=0 T; T)]/ρ( μ₀H=0 T; T) on the order of a few percent, with maximums of 6% and 4% (right at the Curie temperature, T_C 160 K) was calculated for an in-plane and out-of plane measuring geometry, respectively. In addition there is an equally strong MR effect at low temperatures, which might be related to the temperature dependence of the magnetocrystalline anisotropy together with a magnetization rotation. Both the MR(T) behavior and the achieved values (except for T<30 K) are similar to those obtained on SrRuO₃ films grown on 2° miscut (0 0 1) STO substrates with the current parallel to the field and parallel to the direction, which was identified as the easier axis for magnetization.     

Flux creep and flux flow for thallium ceramics in a pulsed magnetic field

The resistive properties of Tl-ceramics with T_c|=0=114 K were investigated in a pulsed magnetic field (B) up to 30 T and in the temperature range of 4.2 K<T<140 K. It was shown that the character of the field dependence of the resistance differs qualitatively in high-and low-temperature regions. At low (T80K) temperatures the dynamic magnetoresistance arising in the sample is analogous to that observed earlier in LaSrCuO [1] and YBaCuO [2] ceramics. This magnetoresistance is defined by the magnetic field variation rate and leads to the appearance of a minimum at the maximum of the magnetic field pulse, i.e. at . In the region of high temperatures (80 K T<T_c) or magnetic fields (at T60K) the sample resistance rises monotonically with B increase, and dynamic resistance is not observed. In this temperature range the existence of a scaling relation is shown (here B^* and T^* meet the condition k=(B^*, T^*)/ _n(T^*)=const) for the ceramics resistance (B,T), which can be represented as . An estimate for the upper critical field B_c2(0)B_o=1030±40 T is obtained.     

Direct measurement of the magnetocaloric effect in La0.67Ca0.33MnO3

Polycrystalline perovskite La_0.67Ca_0.33MnO₃ was synthesized by a sol–gel method. Its adiabatic temperature change ΔT_ad induced by a magnetic field change was measured directly. At 268 K, near its Curie temperature T_C, ΔT_ad of La_0.67Ca_0.33MnO₃ induced by a magnetic field change of 2.02 T reaches 2.4 K. The latent heat Q and magnetic entropy change −ΔS_M induced by a magnetic field change were calculated from the temperature dependence of ΔT_ad and zero-field heat capacity C_p. The maximum values of Q and −ΔS_M in La_0.67Ca_0.33MnO₃ induced by a magnetic field change of 2.02 T are 1.85 J g⁻¹ and 6.9 J kg⁻¹ K⁻¹, respectively. The former is larger than the phase transition latent heat of heating or cooling, which is about 1.70 J g⁻¹.     

Metal/insulator manganite multilayers

We have studied the transport and magnetic properties of strongly textured metal/insulator La_1−xSr_xMnO₃ (x=0.4,0.1) bilayers and trilayers, grown by DC magnetron sputtering over MgO and SrTiO₃ substrates. The multilayers present transport properties similar to those of the La_0.6Sr_0.4MnO₃ films, being very sensitive to deposition conditions. Magnetic multilayers show a metal–insulator transition around T_c (250 K) and colossal magnetoresistance which is maximum around T_c. No extrinsic magnetoresistance associated with the multilayered structure was observed, probably due to the presence of ferromagnetic coupling between the metallic layers, as suggested by magnetization measurements.     

钙钛矿锰氧化物(La_(1-x)Eu_x)_(4/3)Sr_(5/3)Mn_2O_7(x=0,0.15)的磁性和电性研究

通过传统固相反应法制备了钙钛矿锰氧化物(La1-xEux)4/3Sr5/3Mn2O7(x=0,0.15)多晶样品,并且对其磁性和电性进行了研究.磁性测量表明:随着温度的降低,样品经历了一个复杂的转变过程,在温度为T*时经历二维短程铁磁有序转变,在温度为TC时进入三维长程铁磁态.随着Eu的掺杂,T*和TC减小,并且样品(La0.85Eu0.15)4/3Sr5/3Mn2O7在低温区表现出自旋玻璃行为.电性质测量表明:在母体La4/3Sr5/3Mn2O7中La位掺杂Eu后电阻率明显变大,金属绝缘转变温度TMI降低,磁电阻峰值增大.这些影响归因于较小的Eu3+离子替代La3+离子导致平均离子半径减小,晶格发生畸变.此外,较小的Eu3+离子优先占据层间岩盐层的R-site,使La3+,Sr3+,Eu3+离子在(La0.85Eu0.15)4/3Sr5/3Mn2O7中的分布更加有序,所以x=0.15的样品的ρ-T曲线只有一个峰.     

Laser ablated bismuth cuprate thin films preparation and effect of oxygen nonstoichiometry upon superconductivity

Thin films of Bi₂Sr₂CaCu₂O₈ and (Bi, Pb)₂Sr₂Ca₂Cu₃O₁₀ have been prepared on monocrystalline (100) MgO substrates, using a laser ablation method with post annealing treatment. The influence of substrate temperature and oxygen pressure during deposition were investigated. SEM observations, EDS analysis, electric and magnetic measurements have been used to characterize the films. Superconducting “2212” films, with T_c(R = 0) at 80–83 K and J_c (50 K) up to 5 × 10⁵ A/cm², have been currently achieved, while Pb-doped “2223” films exhibit T_c as high as 110 K with J_c = 5 × 10⁴ A/cm² at 77 K. The effect of annealing at low temperature (350°C) in an argon flow has been studied for the 2212 phase, it shows the influence of the oxygen non-stoichiometry, i.e. of the hole carrier density upon T_c's which can be measured up to 89 K (zero resistance).     

Synthesis of YBa2Cu3O7−x superconducting thin films on LaAlO3 by means of PAMOCVD

High-T_c superconducting thin films have been deposited in situ by means of a plasma assisted metal-organic chemical vapour deposition (PAMOCVD) process on LaAlO₃. An EMCORE high-speed rotating disc reactor was used to deposit the films at a substrate temperature of 600°C to 800°C. The system is equipped with a (remote) 120 W microwave plasma generator. The oxidising plasma gas is N₂O and/or O₂ while Ar was used as the inert carrier gas for the different metal-organics. The influence of different process parameters (such as the temperatures of the metal-organics, substrate temperature, and plasma gas composition) on the superconductive properties and on the morphology of the films was investigated. Surface morphology and composition were studied by SEM/EDX or EPMA, and AC susceptibility measurements were used to investigate the superconductive properties (T_c and J_c). X-ray diffraction measurements indicated that single-phase YBa₂Cu₃O_7−x films were epitaxially grown with the 00l orientation perpendicular to the substrate surface. The critical temperature (T_c) of the films is about 90 K and the critical current density (J_c) is higher than 10⁶ A/cm² at 77 K and zero field.     

Temperature range for critical scaling behavior in YBCO thin films

The magnetic and transport properties of thin films and single crystals of YBa₂Cu₃O_7−δ are compared. For measurements on thin films, the apparent critical scaling behavior is observed to exist over a temperature range from 87 K down to the vortex-glass transition T_g = 84.2 K at 2.5 kOE and from 83 K to T_g = 70.4 K at 50 kOe. The inflection point (T_inf) in temperature dependent resistivity measurements R(T) coincides with the highest temperature at which current-voltage (I–V) characteristics are found to scale. The region between T_g and T_inf shows a behavior characteristics of thermally activated flux motion, while above T_inf I–V curves show ohmic behavior. No similar scaling region is observed in some single crystal results, supporting recent claims that the phase transition in some single crystals may not be critical in nature (of order greater than one).     

Over-doping of Tl2Ba2CuO6 due to charge transfer Tl-(Cu-O)

Superconductivity was observed in La substituted Tl₂Ba₂CuO₆. Both T_c and unit cell dimension, a, increase with increasing La concentration, indicating that an over-doping state in Tl₂Ba₂CuO₆, which was due to charge transfer Tl^3−t-(Cu-O)^p as supported from XPS measurements, was relieved by La substitution for Ba.     

Charge susceptibility and charge correlation function in the d---p model

The properties of the charge fluctuation are investigated in the d---p model with the repulsion U_pd between holes on the nearest-neighbor Cu and O sites and the infinite on-site repulsion U_d at the Cu site. We calculate the charge susceptibility χ^c(q, iω_n) and the charge correlation function S^c(q) = TΣ_ωn χ^c(q, iω_n). It is found that S^c(q) has a peak at the Γ point and a maximum in a ring around the Γ point. The former is due to Tχ^c(q, 0). Its intensity is proportional to temperature T and strongly enhanced by U_pd. The latter is due to TΣ_{ωn ≠ 0} χ^c(q, iω_n) and shows a weak T and U_pd dependence. The intensity of the diffuse X-ray scattering on taking the charge fluctuation into account is also calculated. The result is consistent with the experiments in La_2−δSr_δCuO₄.     

Transient behavior of the thermal ion emission from KCl(0 0 1) upon polarity reversal of the electric extraction field

The technique of polarity reversal of the external electric extraction field (strength: 10² V/cm) was applied to study the relaxation of the thermal ion emission from the KCl(0 0 1) single crystal surface. Transient currents of the K⁺ and K₂Cl⁺ ions upon switching from the emission suppression to the ion extraction mode were recorded as a function of the evaporation time, the temperature, and the time of field reversal. The temperature dependence of the time constants of the K⁺ ions obtained from the exponential decreases of the emission currents to their steady-state emission resulted as logτ_h(s)=−(13.39±0.56)+(12.42±0.49)10³/T in a high temperature interval of 826–930 K after a prolonged heating period and as logτ_l(s)=−(20.65±1.04)+(16.77±0.81)10³/T in a low temperature interval of 750–801 K at the initial stage of evaporation, with corresponding activation energies of E_h(K⁺)=2.47±0.14 eV and E_l(K⁺)=3.32±0.16 eV, respectively. The transient currents can be interpreted by a partial adsorption of the suppressed ion currents at the kinks of the surface steps. The differences in the high- and low-temperature runs may be attributed to a strong coarsening of the surface at higher temperatures, which occurs as a bunching of monosteps to macrosteps and/or to an enrichment and segregation of divalent impurities at the surface. The transient behavior of the molecular K₂Cl⁺ ions seems to be strongly correlated with that of the K⁺ ions. This correlation is possibly caused by changes of the strength or the sign of the local electrical field connected with the excess charge at the kinks.     

Anomalous magnetotransport phenomena in θ-(BEDT-TTF)2I3

Anomalous magnetotransport phenomena have been observed in θ-(BEDT-TTF)₂I₃ crystals at temperatures below 15 K. The magnetoresistance M : (1) is a linear function of the magnetic field H, (2) is not affected by the angle between the electric current and the magnetic field, (3) but depends on the magnetic field orientation with respect to the crystal axis. Magnetoresistance is expressed as M = (aH²_a + bH²_b + cH²_c)₀^-3/2/H in terms of H = (H_a, H_b, H_c), the zero field resistivity ₀, and parameters a, b, and c which are independent of temperature and magnetic field. We have found that b a > c. Magnetoresistance up to 40 is observed for H = 7T along the b-axis at T = 1.5K.     

Morphological and electrical properties of SrTiO_3/TiO_2/SrTiO_3 sandwich structures prepared by plasma sputtering

SrTiO_3(STO) and TiO_2 are insulating materials with large dielectric constants and opposite signs of the quadratic coefficient of voltage(α). Insertion of a TiO_2 thin film between STO layers increases the linearity of the capacitance in response to an applied voltage, to meet the increasing demand of large-capacitance-density dynamic random access memory capacitors. Both STO and TiO_2 suffer from the problem of high leakage current owing to their almost equivalent and low bandgap energies. To overcome this, the thickness of the thin TiO_2 film sandwiched between the STO films was varied. A magnetron sputtering system equipped with radio frequency and direct current power supply was employed for depositing the thin films. Ti N was deposited as the top and bottom metal electrodes to form a metal–insulator metal(MIM) structure,which exhibited a very large linear capacitance density of 21 fF/um~2 that decreased by increasing the thickness of the TiO_2 film. The leakage current decreased with an increase in the thickness of TiO_2, and for a 27-nm-thick film, the measured leakage current was 2.0 × 10~(-10) A. X-ray diffraction and Raman spectroscopy revealed that Ti N, STO, and TiO_2 films are crystalline and TiO_2 has a dominant anatese phase structure.     

Low temperature magnetotransport properties of La0.55Ho0.15Sr0.3MnO3

Magnetotransport data measured in thin films of La_0.55Ho_0.15Sr_0.3MnO₃ down to very low temperatures (0.25 K) are reported. The samples presented colossal magnetoresistance with a T_C close to 200 K. A minimum in the resistance vs. T curve and a drop in the ZFC magnetization were also observed. It was also found a T-dependent relaxation effect after the magnetic field was either applied or removed. These results can be understood within the framework where electronic scattering occurs across magnetic domain walls in a reentrant spin-glassy-like phase.     

Field-induced parameters of re-entrant magnets and concentrated spin glasses

We have used electron spin resonance measurements to derive the temperature and frequency dependences of the field-induced magnetization [M(T, f)] and anisotropy field [H_an (T)] in a number of amorphous alloys belonging to the series (Fe_pNi_1−p)₇₅P₁₆B₆Al₃. In re-entrant (p > p_c, the critical concentration for ferromagnetism) alloys at hi gh frequencies (f = 35 GHz, field ≈ 12 kOe) M reduces as T^3/2 at high T and as T below ≈ 40 K, the deviation from T^3/2 becoming more marked as p → p⁺_c. For p close to p_c, lowering the frequency first causes the T term to increase and ultimately ( ≈ 4 GHz) changes the variation of M with T to that discovered previously for concentrated spin glasses, namely M is constant at low T and drops linearly at high temperatures. For the re-entrants, the results are interpreted on the basis of a model which invokes an energy gap in the spin-wave spectrum, introduces a non-zero density of states of the gap energy and takes into consideration a low-q cut-off in the spin-wave integral in thelow-T (T) regime.In the concentrated spin glasses [M (0) - M (T)]/ M (0) is well represented by the function [exp (Δ / T) - 1]^-1, where Δ has values close to the corresponding Curie-Weiss temperatures θ_p but much larger than the respective spin glass transition temperatures T_SG. The temperature dependence of H_an is largely given by the function (1 - T/T^*), where T^* is equal to the zero-field freezing temperature for the re-entrants and T_SG for the spin glasses, respectively.     

Effective activation energy Ue(T,J,H) in textured Bi1.84Pb0.4Sr2Ca2Cu3Oy silver-clamped thick films

We have measured the resistivity of textured Bi_1.84Pb_0.4Sr₂Ca₂Cu₃O_y silver-clamped thick films as a function of temperature, current density ranging from 10 to 1×10³ A/cm² and magnetic field up to 0.3 T. We find that the effective activation energy U_e follows U_e(T,J,H)=U₀(1−T/T_p)^mln(J_c0/J)H⁻ with m=1.75 for Hab-plane and 2.5 for Hc-axis and =0.76 for Hab and 0.97 for Hc, for the current density regime above 100 A/cm², where T_p is a function of applied magnetic field and current density. This result suggests the effective activation energy U_e be correlated with the temperature, current density and magnetic field. The possible dissipative mechanisms responsible for the temperature, current density and magnetic field dependence of the effective activation energy are discussed.     

MgB2超导膜的厚度与其Jc(5K,0T)的关系

通过混合物理化学气相沉积法 (hybrid physical-chemical vapor deposition, HPCVD), 在(000l) SiC 衬底上制得一系列从10 nm到8 μm的MgB₂超导膜样品, 并对它们的形貌、超导转变温度T_c 和临界电流密度J_c与膜厚度的关系进行了研究. 观察到T_c随膜厚度增加上升到最大值后, 尽管膜继续增厚, 但T_c值保持近乎平稳, 而J_c则先随膜厚度增加上升到最高值后, 继而则随膜的厚度的增加而下降. MgB₂膜的T_c(0)和T_c(onset)值与膜厚的关系基本一致, T_c(0)在膜厚为230 nm处达到最大值T_c(0)=41.4 K, 而J_c(5K,0T)在膜厚为100 nm时达到最大值, J_c (5 K, 0 T)=2.3×10⁸A·cm^-2, 这也说明了我们能用HPCVD方法制备出高质量干净MgB₂超导膜. 本文研究的超导膜厚度变化跨度非常大, 从10 nm级的超薄膜到100 nm级的薄膜, 再到几微米的厚膜, 如此T_c和J_c对膜厚度变化的依赖就有了较完整、成体系的研究. 并且本文的工作对MgB₂超导薄膜制备的厚度选取具有实际应用意义. 关键词： 2超导膜')" href="#">MgB₂超导膜 混合物理化学气相沉积法 厚度 临界电流密度     

Emerging weak antilocalization effect in Ta0.7Nb0.3Sb2 semimetal single crystals

Weak antilocalization (WAL) effect is commonly observed in low-dimensional systems, three-dimensional (3D) topological insulators and semimetals. Here, we report the growth of high-quality Ta_0.7Nb_0.3Sb₂ single crystals via the chemical vapor transport (CVT). Clear sign of the WAL effect is observed below 50 K, probably due to the strong spin−orbital coupling in 3D bulk. In addition, it is worth noting that a relatively large MR of 120% appears under 1 T magnetic field at T = 2 K. Hall measurements and two-band model fitting results reveal high carrier mobility (>1000 cm²·V⁻¹·s⁻¹ in 2–300 K region), and off-compensation electron/hole ratio of ~8:1. Due to the angular dependence of the WAL effect and the fermiology of the Ta_0.7Nb_0.3Sb₂ crystals, interesting magnetic-field-induced changes of the symmetry of the anisotropic magnetoresistance (MR) from two-fold (≤ 0.6 T) to four-fold (0.8–1.5 T) and finally to two-fold (≥ 2 T) are observed. This phenomenon is attributed to the mechanism shift from the low-field WAL dominated MR to WAL and fermiology co-dominated MR and finally to high-field fermiology dominated MR. All these signs indicate that Ta_0.7Nb_0.3Sb₂ may be a topological semimetal candidate, and these magnetotransport properties may attract more theoretical and experimental exploration of the (Ta,Nb)Sb₂ family.