Search Results (44)

A-site-ordered quadruple perovskite manganites, AMn₇O₁₂, show many interesting physical phenomena, including orbital and spin modulations, spin-induced multiferroic properties, and competitions between different magnetic ground states. Doping with Cu²⁺ can result in colossal magnetoresistance properties, ferrimagnetism, and additional structural modulations producing electric–dipole helicoidal textures. Many previous works have focused on large-concentration doping, reaching ACu₃Mn₄O₁₂ compositions. Small-concentration doping has been investigated in a limited number of systems, e.g., in BiCu_xMn_7−xO₁₂. In this work, we investigated solid solutions of NdCu_xMn_7−xO₁₂ with x = 0.1, 0.2, and 0.3, prepared at 6 GPa and 1500 K. Specific heat measurements detected three magnetic transitions at x = 0 (at T_N3 = 9 K, T_N2 = 12 K, and T_N1 = 84 K) and two transitions at x = 0.1 (at T_N2 = 10 K and T_N1 = 78 K), while only one transition was found at x = 0.2 (T_N1 = 72 K) and x = 0.3 (T_N1 = 65 K). Differential scanning calorimetry (DSC) measurements showed sharp and strong peaks near T_OO = 664 K at x = 0, corresponding to an orbital-order (OO) structural transition from I2/m to Im-3 symmetry. DSC anomalies were significantly broadened and their intensities were significantly reduced at x = 0.1–0.3, and structural transitions were observed near T_OO = 630 K at x = 0.1, T_OO = 600 K at x = 0.2, and T_OO = 570 K at x = 0.3. The x = 0.1 sample clearly showed double-peak features on the DSC curves near T_OO because of the presence of two close phases. High-resolution synchrotron powder X-ray diffraction studies gave strong evidence that phase separation phenomena took place in the x = 0.1–0.3 samples, where two I2/m phases with an approximate ratio of 1:1 were present (e.g., a = 7.47143 Å, b = 7.36828 Å, c = 7.46210 Å, and β = 90.9929° for one phase and a = 7.46596 Å, b = 7.37257 Å, c = 7.45756 Å, and β = 90.9328° for the second phase at x = 0.3). The Curie–Weiss temperature changed from negative (for x = 0, 0.1, and 0.2) to positive (for x = 0.3). T_OO, T_N1, the Curie–Weiss temperature, and magnetization (at 5 K and 70 kOe) changed almost linearly with x. Full article

In this study, a modified Curie–Weiss model was established for the magnetic susceptibility of high-purity molybdenum and Mo–La alloy powders. The elemental composition was analyzed by GDMS, and combined with the M–T and M–H data measured by SQUID, the temperature-independent contributions of weakly magnetic elements such as La and the paramagnetic contributions of impurity ions such as Fe, Co, and Ni were distinguished. Based on the parameters obtained from the nonlinear least squares fitting, the deviation between the magnetic susceptibility at room temperature calculated by the model and the experimental value was within 5%. The results show that this model can reasonably describe the influence of trace impurities on the magnetic susceptibility of the system and provides an effective method for the magnetic prediction of high-purity metal powders. Full article

Layered chalcogenides are interesting from the point of view of the formation of two-dimensional magnetic systems for relevant applications in spintronics. High-spin Mn²⁺ or Fe³⁺ cations with five unpaired electrons are promising in the search for compounds with interesting magnetic properties. In this study, a new layered modification of the Mn₂In₂Se₅ compound from the A₂B₂X₅ family (“225”) was synthesized and investigated. A phase transition to the polymorph with primitive trigonal lattice was recorded at a temperature of 711 °C, which was confirmed by simultaneous thermal analysis, X-ray powder diffraction at elevated temperatures, and sample annealing and quenching. The stability of Mn₂In₂Se₅ in air at high temperatures was investigated by thermal gravimetric analysis and powder X-ray diffraction. The new polymorph of Mn₂In₂Se₅ crystallizes in the Mg₂Al₂Se₅ structure type, as revealed by the Rietveld refinement against powder X-ray diffraction data. The crystal structure can be viewed as a close-packing of Se anions, in which indium and manganese cations are enclosed inside tetrahedral and octahedral voids, respectively, according to the A_MnB_InCB_InC_MnA… sequence. Magnetization measurements reveal an antiferromagnetic-like transition at a temperature of 6.3 K. The same magnetic properties are reported in the literature for the low-temperature R-centered trigonal polymorph. An approximation by the modified Curie–Weiss law yields a significant ratio of |θ|/T_N = 28, which indicates strong magnetic frustration. Full article

A site-ordered quadruple perovskites, AA′₃B₄O₁₂, can have 3d transition metals at A′ and B sites, and show complex magnetic interactions and behavior. Additional complexity appears when B site-ordered arrangements are realized in AA′₃B₂B′₂O₁₂. In this work, A site-ordered quadruple perovskites, RMn₃Ni₂Mn₂O₁₂ with R = Bi, Ce, and Ho, were prepared by a high-pressure, high-temperature method at about 6 GPa and about 1500 K. The R = Bi and Ce samples were found to crystallize in space group Im-3 with a disordered distribution of Ni²⁺ and Mn⁴⁺ cations in one B site. On the other hand, the R = Ho sample crystallized in space group Pn-3 and showed partial ordering of Ni²⁺ and Mn⁴⁺ cations between two B sites. The structural data (and bond valence sums) suggest that cerium has the oxidation state +3, which is unusual for such perovskites. Magnetic properties were investigated by magnetic susceptibility and specific heat measurements, which showed the presence of one magnetic transition near 36 K for R = Bi; there was evidence for the presence of two magnetic transitions near 27 K and 33 K for R = Ce, and near 10 K and 36 K for R = Ho. Curie–Weiss parameters were estimated for all samples from high-temperature magnetic measurements up to 750 K. The total effective magnetic moment for R = Ce also suggests the presence of Ce³⁺. A magnetic field of 90 kOe had the largest effect on the specific heat of the R = Ho sample, and almost no effects on the specific heat of the R = Bi sample. Full article

In this paper, we consider the problem of estimating the interaction parameter p of a p-spin Curie–Weiss model at inverse temperature $\beta$, given a single observation from this model. We show, by a contiguity argument, that joint estimation of the parameters $\beta$ and p is impossible, which implies that the estimation of p is impossible if $\beta$ is unknown. These impossibility results are also extended to the more general p-spin Erdös–Rényi Ising model. The situation is more delicate when $\beta$ is known. In this case, we show that there exists an increasing threshold function ${\beta }^{*}\left(p\right)$, such that for all $\beta$, consistent estimation of p is impossible when ${\beta }^{*}\left(p\right)>\beta$, and for almost all$\beta$, consistent estimation of p is possible for ${\beta }^{*}\left(p\right)<\beta$. Full article

In this work, the rare earth element Ce was incorporated into the A-site of Sr_0.4Ba_0.6Nb₂O₆ ferroelectric ceramics, which was prepared using the conventional solid state reaction method and sintered under different procedures. A comprehensive investigation was conducted to assess the impact of Ce doping and varying sintering procedures on both the relaxor characteristics and electrical properties of the ceramics. When sintered at 1300 °C for 4 h, the grains exhibited an isometric shape. However, when the sintering temperature increases and the holding time prolongs, the grain size increases and presents columnar crystal. The change tendency of dielectric constant is similar with that of the grain size, and the dielectric peak value of samples sintered at 1300 °C for 4 h is the lowest. But the sintering procedure has almost no influence on the Curie point, which notably decreases as the Ce content rises and is primarily governed by the composition. The diffuseness fitting results and the deviation from the Curie–Weiss law indicate that relaxor characteristics increase with the Ce content increasing. The polarization electric (P-E) loops become slimmer with increasing Ce content, verifying the relaxor behavior variation of samples. As a result, the P_max and P_r values decrease and the P_max − P_r value increases with increasing Ce content. Notably, the energy storage density and efficiency enhance obviously with higher Ce content, which is attributed to the relaxor behavior. Furthermore, at a Ce content of 4 mol%, the P-E loops and energy storage performance exhibit remarkable frequency and fatigue stability. Therefore, this study offers valuable insights into the investigation of relaxor behavior and the influence of rare earth elements on the properties of tungsten bronze-structured ferroelectrics. Full article

ABO₃ perovskite materials with small cations at the A site, especially with ordered cation arrangements, have attracted a lot of interest because they show unusual physical properties and deviations from general perovskite tendencies. In this work, A-site-ordered quadruple perovskites, RMn₃Ni₂Mn₂O₁₂ with R = Nd, Sm, Gd, and Dy, were synthesized by a high-pressure, high-temperature method at about 6 GPa. Annealing at about 1500 K produced samples with additional (partial) B-site ordering of Ni²⁺ and Mn⁴⁺ cations, crystallizing in space group Pn–3. Annealing at about 1700 K produced samples with disordering of Ni²⁺ and Mn⁴⁺ cations, crystallizing in space group Im–3. However, magnetic properties were nearly identical for the Pn–3 and Im–3 modifications in comparison with ferromagnetic double perovskites R₂NiMnO₆, where the degree of Ni²⁺ and Mn⁴⁺ ordering has significant effects on magnetic properties. In RMn₃Ni₂Mn₂O₁₂, one magnetic transition was found at 26 K (for R = Nd), 23 K (for R = Sm), and 22 K (for R = Gd), and two transitions were found at 10 K and 36 K for R = Dy. Curie–Weiss temperatures were close to zero in all compounds, suggesting that antiferromagnetic and ferromagnetic interactions are of the same magnitude. Full article

Ceramic capacitors have received great attention for use in pulse power systems owing to their ultra-fast charge–discharge rate, good temperature stability, and excellent fatigue resistance. However, the low energy storage density and low breakdown strength (BDS) of ceramic capacitors limit the practical applications of energy storage technologies. In this work, we present a series of relaxor ferroelectric ceramics (1−x) [0.94 Bi_0.5Na_0.5TiO₃ –0.06BaTiO₃]– x Sr_0.7Bi_0.2TiO₃ (1-x BNT-BT- x SBT; x = 0, 0.20, 0.225, 0.25, 0.275 and 0.30) with improved energy storage performances by combining relaxor and antiferroelectric properties. XRD, Raman spectra, and SEM characterizations of BNT-BT-SBT ceramics revealed a rhombohedral–tetragonal phase, highly dynamic polar nanoregions, and a reduction in grain size with a homogeneous and dense microstructure, respectively. A high dielectric constant of 1654 at 1 kHz and low remnant polarization of 1.39 µC/cm² were obtained with the addition of SBT for x = 0.275; these are beneficial for improving energy storage performance. The diffuse phase transition of these ceramics displays relaxor behavior, which is improved with SBT and confirmed by modified the Curie–Weiss law. The combining relaxor and antiferroelectric properties with fine grain size by the incorporation of SBT enables an enhanced maximum polarization of a minimized P-E loop, leading to an improved BDS. As a result, a high recoverable energy density W_rec of 1.02 J/cm³ and a high energy efficiency η of 75.98% at 89 kV/cm were achieved for an optimum composition of 0.725 [0.94BNT-0.06BT]-0.275 SBT. These results demonstrate that BNT-based relaxor ferroelectric ceramics are good candidates for next-generation ceramic capacitors and offer a potential strategy for exploiting novel high-performance ceramic materials. Full article

Electrostrictive materials based on (Na_0.5Bi_0.5)TiO₃ are promising lead-free candidates for high-precision actuation applications, yet their properties require further improvement. This study aims to enhance the electromechanical properties of a predominantly electrostrictive composition, 0.685(Na_0.5Bi_0.5)TiO₃-0.065BaTiO₃-0.25SrTiO₃, by using templated grain growth. Textured ceramics were prepared with 1~9 wt% NaNbO₃ templates. A high Lotgering factor of 95% was achieved with 3 wt% templates and sintering at 1200 °C for 12 h. Polarization and strain hysteresis loops confirmed the ergodic nature of the system at room temperature, with unipolar strain significantly improving from 0.09% for untextured ceramics to 0.23% post-texturing. A maximum normalized strain, S_max/E_max (d₃₃*), of 581 pm/V was achieved at an electric field of 4 kV/mm for textured ceramics. Textured ceramics also showed enhanced performance over untextured ceramics at lower electric fields. The electrostrictive coefficient Q₃₃ increased from 0.017 m⁴C⁻² for untextured ceramics to 0.043 m⁴C⁻² for textured ceramics, accompanied by reduced strain hysteresis, making the textured 0.685(Na_0.5Bi_0.5)TiO₃-0.065BaTiO₃-0.25SrTiO₃ composition suitable for high-precision actuation applications. Dielectric properties measured between −193 °C and 550 °C distinguished the depolarization, Curie–Weiss and Burns temperatures, and activation energies for polar nanoregion transitions and dc conduction. Dispersive dielectric constants were found to observe the “two” law exhibiting a temperature dependence double the value of the Curie–Weiss constant, with shifts of about 10 °C per frequency decade where the non-dispersive THz limit was identified. Full article

A new double perovskite compound with nominal composition Y${}_2$MgRuO${}_6$ is synthesized by the floating zone technique. X-ray diffraction measurements reveal a monoclinic crystal structure with space group $P{2}_1/n$ and monoclinic angle $\beta$ = 90.178(1)${}^{\circ }$ as crystallographically expected for a double perovskite. A composition of Y${}_{1.880\left(8\right)}$Mg${}_{0.953\left(4\right)}$Ru${}_{1.047\left(4\right)}$O${}_{6-\delta }$ is revealed by our single crystal X-ray diffraction measurement. The magnetic susceptibility of this compound does not show indications of magnetic ordering down to the lowest temperature. A Curie–Weiss fit for the paramagnetic part above 300 K yields an effective moment that indicates an S = 1 Ru${}^{4+}$ state. We attribute the occurrence of the S = 1 state and the lack of magnetic order to the presence of the $B/B^{\prime }$-site disorder. Full article

Dielectric materials are highly desired for pulsed power capacitors due to their ultra-fast charge-discharge rate and excellent fatigue behavior. Nevertheless, the low energy storage density caused by the low breakdown strength has been the main challenge for practical applications. Herein, we report the electric energy storage properties of (1 − x) Bi_0.5(Na_0.8K_0.2)_0.5TiO₃-xBi_0.2Sr_0.7TiO₃ (BNKT-BST; x = 0.15–0.50) relaxor ferroelectric ceramics that are enhanced via a domain engineering method. A rhombohedral-tetragonal phase, the formation of highly dynamic PNRs, and a dense microstructure are confirmed from XRD, Raman vibrational spectra, and microscopic investigations. The relative dielectric permittivity (2664 at 1 kHz) and loss factor (0.058) were gradually improved with BST (x = 0.45). The incorporation of BST into BNKT can disturb the long-range ferroelectric order, lowering the dielectric maximum temperature T_m and inducing the formation of highly dynamic polar nano-regions. In addition, the T_m shifts toward a high temperature with frequency and a diffuse phase transition, indicating relaxor ferroelectric characteristics of BNKT-BST ceramics, which is confirmed by the modified Curie-Weiss law. The rhombohedral-tetragonal phase, fine grain size, and lowered T_m with relaxor properties synergistically contribute to a high P_max and low P_r, improving the breakdown strength with BST and resulting in a high recoverable energy density W_rec of 0.81 J/cm³ and a high energy efficiency η of 86.95% at 90 kV/cm for x = 0.45. Full article

The aim of this study was to investigate the magnetic properties of mixed nanocrystalline Zn/manganese oxide compounds synthesized by a hydrothermal method. These compounds are designed as (ZnO)_1−n(MnO)_n, where index n ranges from 0.05 to 0.60. The results of magnetic measurements, including AC magnetic susceptibility as a function of temperature (up to 160 K) and frequency (from 7 Hz up to 9970 Hz), as well as DC magnetization in magnetic fields up to 9 T and temperature up to 50 K, are reported. We observed various types of magnetic behavior depending on the nominal weight content of MnO. Samples with a low nominal content (up to n = 0.10) of MnO exhibited Curie–Weiss behavior at higher temperatures. For samples with high nominal weight contribution (from n = 0.30 to 0.60), spin-glass-like or/and weak ferromagnetic behavior is observed. Full article

Raman spectroscopy and magnetic properties of the natural single crystalline diamonds irradiated with high fluences of fast reactor neutrons have been investigated. Raman spectra transformations were studied in the range from moderate levels up to radiation damage leading to diamond graphitization. The selection of fast neutrons irradiated diamonds for magnetic measurements was carried out according to Raman scattering data on the basis of the intensity criterion and the spectral position of the “1640” band. It was found that in natural diamonds irradiated with neutrons with an extremely high subcritical fluence F = 5 × 10²⁰ cm⁻², the transition from a diamagnetic to a ferromagnetic state is observed at the Curie–Weiss temperature of ≈150 K. The energy of the exchange magnetic interaction of uncompensated spins is estimated to be ≈1.7 meV. The differential magnetic susceptibility estimated from the measurements of magnetic moment for temperature 2 K in the limit of B ≈ 0 is χ_diff ≈ 1.8 × 10⁻³ SI units. The nature of magnetism in radiation-disordered single-crystal hydrogen- and metal-free natural diamond grains was discussed. Full article

In a wavefunction-only philosophy, thermodynamics must be recast in terms of an ensemble of wavefunctions. In this perspective we study how to construct Gibbs ensembles for magnetic quantum spin models. We show that with free boundary conditions and distinguishable “spins” there are no finite-temperature phase transitions because of high dimensionality of the phase space. Then we focus on the simplest case, namely the mean-field (Curie–Weiss) model, in order to discover whether phase transitions are even possible in this model class. This strategy at least diminishes the dimensionality of the problem. We found that, even assuming exchange symmetry in the wavefunctions, no finite-temperature phase transitions appear when the Hamiltonian is given by the usual energy expression of quantum mechanics (in this case the analytical argument is not totally satisfactory and we relied partly on a computer analysis). However, a variant model with additional “wavefunction energy” does have a phase transition to a magnetized state. (With respect to dynamics, which we do not consider here, wavefunction energy induces a non-linearity which nevertheless preserves norm and energy. This non-linearity becomes significant only at the macroscopic level.) The three results together suggest that magnetization in large wavefunction spin chains appears if and only if we consider indistinguishable particles and block macroscopic dispersion (i.e., macroscopic superpositions) by energy conservation. Our principle technique involves transforming the problem to one in probability theory, then applying results from large deviations, particularly the Gärtner–Ellis Theorem. Finally, we discuss Gibbs vs. Boltzmann/Einstein entropy in the choice of the quantum thermodynamic ensemble, as well as open problems. Full article

The DC and AC magnetic susceptibilities of an opal matrix-based nanocomposite with pyrochlore-structured ytterbium titanate particles up to 60 nm in size have been studied in the range of magnetic fields up to 30 kOe. The measurements were performed at temperatures from 2 to 200 K. The temperature dependence of the nanocomposite Yb₂Ti₂O₇ has been found to deviate significantly from the Curie–Weiss law. From the frequency dependence of the AC susceptibility measured in the range from 10 Hz to 10 kHz, the spin relaxation times have been determined, and two relaxation times have been found to be required for the description of the frequency dependence of the susceptibility. The field dependence of the AC susceptibility has been measured. This dependence is proved to be described by the modified Cole–Cole formula. The characteristic fields of the magnetic field dependence of the real part of the susceptibility are determined, the value of the characteristic field being found to increase with increasing temperatures. Full article