Investigations of structural, dielectric and ferroelectric behavior of europium substituted SrBi2Ta2O9 ferroelectric ceramics

Europium substituted samples of the compositions Sr_1−xEu_xBi₂Ta₂O₉ (x=0.0,0.025,0.050,0.10 and 0.20) were synthesized by solid state reaction method and studied for their structural, dielectric and ferroelectric properties. The X-ray diffractograms confirmed the formation of single phase layered perovskite structure in all the samples. The temperature variation of dielectric constant shows that the Curie temperature (T_c) decreases on increasing concentration of europium. The dielectric loss reduces significantly with europium addition. The P-E studies of the Eu-substituted SBT ceramics show that the remanent polarization increases with increasing concentration of europium.     

Electrical properties of pulsed laser-deposited SrxBiyTa2O9 thin films on Bi/Sr ratios

The dependence of the electrical properties of Sr_xBi_yTa₂O₉ thin films on the (Bi/Sr ratio 1.6, 2.3, 2.8, 3.4) has been investigated. The Sr_xBi_yTa₂O₉ ferroelectric thin films were synthesized on Pt/Ti/SiO₂/Si substrates using the pulsed laser deposition method. Saturation polarization (P_st) and coercive field (2E_c) depend on the Bi/Sr ratio. P_st increases while E_c decreases with an increase in Bi/Sr ratio. Atomic Force Microscopy images show that the grain size grows with increasing Bi/Sr ratio. It is observed that the impedance behavior in Sr_xBi_yTa₂O₉ thin film, conforms to the Constant Phase Element (CPE) model. It is believed that the diffuse charges at the grain boundary build up a surface polarization because the impedance behavior close to pure capacitor with grain size increased.     

Structural distortion and phase transition studies of Aurivillius type Sr1−xPbxBi2Nb2O9 ferroelectric ceramics

In this paper, effects of lead doping on the lattice response and phase transitions of Sr_1−xPb_xBi₂Nb₂O₉ (x=0.0-0.5 in steps of 0.1) ferroelectric ceramics are reported. It is observed that structure attains more tetragonality with doping of lead up to 40%. Increased orthorhombic distortion is observed for undoped SBN and 50 at.% lead substituted SBN. Phase transitions for all samples were studied using Curie temperature measurements and are explained in terms of lattice response of these ceramics. Sample with x=0.5 shows decreased tetragonal strain and Curie temperature. Relationship of polarization with lattice response is discussed.     

Properties of vanadium-doped SrBi4Ti4O15 ferroelectric ceramics

Using the standard solid-state reaction method, several vanadium-doped ferroelectric ceramics of type SrBi_4−x/3Ti_4−xV_xO₁₅ (SBTV−x) were synthesized. The vanadium doping content, x, rangs from 0.00 to 0.06. The crystal structure of SrBi₄Ti₄O₁₅ is not affected by V-doping. The electric breakdown voltage of the samples increases with V content. Meanwhile, V-doping results in a notable enlargement of remnant polarization (2P_r). The 2P_r of STBV−0.03 reaches a very large value, which is over 50 μC/cm² and is nearly twice greater than that at zero doping. The Curie temperatures of V-doped samples decrease slightly in comparison with that of SrBi₄Ti₄O₁₅. V-doping can improve the electric properties of SrBi₄Ti₄O₁₅ without sacrificing its thermal stableness.     

Properties of vanadium-doped SrBi4Ti4O15 ferroelectric ceramics

Using the standard solid-state reaction method, several vanadium-doped ferroelectric ceramics of type SrBi_4−x/3Ti_4−xV_xO₁₅ (SBTV-x) were synthesized. The vanadium doping content, x, ranges from 0.000 to 0.06. The crystal structure of SrBi₄Ti₄O₁₅ is not affected by V-doping. The electric breakdown voltage of the samples increases with V content. Meanwhile, V-doping results in a notable enlargement of remnant polarization (2P_r). The 2P_r of STBV-0.03 reaches a very large value, which is over 50 μC/cm² and is nearly twice greater than that at zero doping. The Curie temperatures of V-doped samples decrease slightly in comparison with that of SrBi₄Ti₄O₁₅. V-doping can improve the electric properties of SrBi₄Ti₄O₁₅ without sacrificing its thermal stableness.     

Photoluminescence properties of Sr1-xSi2O2N2: Eux as green to yellow-emitting phosphor for blue pumped white LEDs

This study evaluated potential applications of green to yellow-emitting phosphors (Sr_1−xSi₂O₂N₂: Eu²⁺_x) in blue pumped white light emitting diodes. Sr_1-xSi₂O₂N₂: Eu²⁺_x was synthesized at different Eu²⁺ doping concentrations at 1450 °C for 5 h under a reducing nitrogen atmosphere containing 5% H₂ using a conventional solid reaction method. The X-ray diffraction patterns of the prepared phosphor (Sr_1-xSi₂O₂N₂: Eu²⁺_x) were indexed to the SrSi₂O₂N₂ phase and an unknown intermediate phase. The photoluminescence properties of these phosphors (Sr_1−xSi₂O₂N₂: Eu²⁺_x) showed that the samples were excited from the UV to visible region due to the strong crystal field splitting of the Eu²⁺ ion. The emission spectra under excitation of 450 nm showed a bright color at 545-561 nm. The emission intensity increased gradually with increasing Eu²⁺ doping concentration ratio from 0.05 to 0.15. However, the emission intensity decreased suddenly when the Eu²⁺ concentration ratio was >0.2. As the doping concentration of Eu²⁺ was increased, there was a red shift in the continuous emission peak. These results suggest that Sr_1-xSi₂O₂N₂: Eu₂⁺_x phosphor can be used in blue-pumped white light emitting diodes.     

Ferroelectric properties of Pr and Nb co-substituted Sr0.8Bi2.2Ta2O9 thin films

Thin film of both A- and B-site co-substituted Sr_0.8Bi_2.2Ta₂O₉ (SBT) by Pr³⁺ and Nb⁵⁺, i.e. Sr_0.8Pr_0.1Bi_2.1Ta_1.5Nb_0.5O₉ (SPBTN) was fabricated on Pt/Ti/SiO₂/Si substrates by metalorganic decomposition method. The Nb⁵⁺ substitution at B-site and Pr³⁺ substitution at A-site enhanced the remanent polarization and reduced the coercive field of the films, respectively. The remanent polarization (2P_r) value of the SPBTN film was 22 μC/cm². The coercive field (2E_c) value of the SPBTN film was 102 kV/cm, which was much lower than that of SBTN (165 kV/cm). The effects of substitution on structural and ferroelectric properties of SBT were discussed in detail. As a result, the A- and B-sites co-substitution may be one of the promising ways to improve ferroelectric properties of SBT.     

Effect of Bi2O3 on EPR, optical transmission and DC conductivity of vanadyl doped alkali bismuth borate glasses

Glasses with composition xBi₂O₃·(30−x)M₂O·70B₂O₃ (M=Li, Na) containing 2 mol% V₂O₅ have been prepared over the range 0≤x≤15 (x is in mol%). The electron paramagnetic resonance spectra of VO²⁺ of these glasses have been recorded in the X-band (≈9.3 GHz) at room temperature (RT≈300 K). Spin Hamiltonian parameters, g_∥, g_⊥, A_∥, A_⊥, dipolar hyperfine coupling parameter, P, and Fermi contact interaction parameter, K, have been calculated. The molecular orbital coefficients, α² and γ², have been calculated by recording the optical transmission spectra. In xBi₂O₃·(30−x)Li₂O·70B₂O₃ glasses there is decrease in the tetragonality of the V⁴⁺O₆ complex for x up to 6 mol% whereas for x≥6 mol%, tetragonality increases. In xBi₂O₃·(30−x)Na₂O·70B₂O₃ glasses there is increase in the tetragonality of the V⁴⁺O₆ complex with increasing x. The 3d_xy orbit expands with increase in Bi₂O₃:M₂O ratio. Values of the theoretical optical basicity, Λ_th, have also been reported. The DC conductivity increases with increase in temperature. The order of conductivity is 10⁻⁵ ohm⁻¹ m⁻¹ at low temperature and 10⁻³ ohm⁻¹ m⁻¹ at high temperature. The DC conductivity decreases and the activation energy increases with increase in Bi₂O₃:M₂O ratio.     

Dielectric properties Ca-substituted barium strontium titanate ferroelectric ceramics

The dielectric and ferroelectric properties of Ba_1−xSr_xTiO₃ (BST) (x=0.10,0.20,0.30,0.40 and 0.60) ceramics and Ba_1−2xSr_xCa_xTiO₃ (BSCT) (x=0.10,0.20,0.30) ceramics have been investigated. The low temperature phase transitions of BST ceramics vanish after Ca²⁺ substitution while the high temperature transition is diffused and relaxed, which becomes more obvious with increasing x. Ca²⁺ substitution obviously decreases the dielectric constant maximum, K_m, of BST ceramics and changes the temperature of dielectric constant maximum, T_m, of BST ceramics. The shift of T_m in BST is attributed mainly to the Sr²⁺ and Ba²⁺ concentration. BST ceramics exhibit almost normal ferroelectric characteristics, while a typical relaxor behavior was observed in BSCT ceramics. The relaxor behavior observations may be understood by a random electric field induced domain state.     

Microwave solid synthesis and electrical properties of Aurivillius-type oxide-ion conductor

A new oxide-ion conductor of Aurivillius-type structure, namely BISRVOX (Bi₂Sr_xV_1−xO_{5.5-(3x/2)-δ}, 0≤x≤0.20), was successively synthesized by the microwave-assisted solid state reaction. 25 min of microwave irradiation was found to be quite sufficient to ensure the completion of reaction. Powder X-ray diffraction and differential thermal analysis showed better structural properties for the microwave-prepared samples compared to those obtained from the conventional solid synthesis route. Interestingly, the highly conducting γ-phase was effectively stabilized for x≥0.10. AC impedance spectroscopy evidenced the superiority of the microwave heating over conventional solid synthesis routes in exhibiting high oxide-ion performance.     

High-throughput screening of ferroelectric materials for non-volatile random access memory using multilayer perceptrons

During the last several years, the development of combinatorial technology has enabled synthesis of a huge amount of chemical compounds in a short time. The large number of variables makes the direct human interpretation of data derived from combinatorial experimentation for high-throughput screening (HTS) very difficult. Artificial neural networks using multilayer perceptrons (MLP) have been successfully applied to the regression problems with various material data. In this work, MLP model was applied to HTS of ferroelectric materials including Bi_4−xLa_xTi₃O₁₂ (BLT) and Bi_4−xCe_xTi₃O₁₂ (BCT). The model using MLP was made to predict the ferroelectric properties of whole feasible experimental conditions. Once a neural network model with high accuracy and good generalization performance was established, we could predict the expected optimal reaction conditions with the best characteristics. The highest gradient value obtained using MLP model is higher than the maximum value found from experiments, thereby accelerating the discovery of the optimal compositions and post-annealing time of BCT and BLT.     

Evolution from relaxor-like dielectric to ferroelectric in Ba[(Fe0.5Nb0.5)1−xTix]O3 solid solutions

Ba[(Fe_0.5Nb_0.5)_1−xTi_x]O₃ (x=0.2,0.4,0.6,0.8,0.85,0.9 and 0.95) solid solutions were synthesized by a standard solid-state reaction technique. X-ray diffraction at room temperature and dielectric characteristics over a broad temperature and frequency range were evaluated systematically. The structure of Ba[(Fe_0.5Nb_0.5)_1−xTi_x]O₃ solid solutions changed from cubic to tetragonal with increasing x. A Debye-like dielectric relaxation following the Arrhenius law similar to that in Ba(Fe_0.5Nb_0.5)O₃ was observed at lower temperature in the composition range 0.2≤x≤0.8, while the relaxor ferroelectric, diffused ferroelectric and normal ferroelectric behavior were observed for x=0.85,0.9 and 0.95, respectively. The process of the evolution of relaxor-like dielectric to ferroelectric suggested the changing from dilute polar micro-domains to polar micro-domains, polar micro/macro-domains and then polar macro-domains in the present ceramics.     

Ionic conductivity of substituted Li7TaO6 phases

Lithium ion conductivity in solid solutions of Li₇Ta_1-xNb_xO₆, Li₇Ta_1-xBi_xO₆, Li_7+xTa_1-xZr_xO₆ and Li_7-2xCa_xTaO₆ has been measured as a function of temperature and composition using the complex impedance method. At 200°C the conductivities of Li₇Ta_0.7Nb_0.3O₆, Li_7.4Ta_0.6Zr_0.4O₆ and Li_6.6Ca_0.2TaO₆ are 4.3 × 10^-4(ωcm)^-1, 3.0 × 10^-4(ωcm)^-1, 4.0 × 10^-4(ωcm)^-1 and 1.6 × 10^-4(ωcm)^-1 respectively. The results are discussed in relation to structural properties.     

Temperature-dependent Fe Mössbauer spectroscopy and local structure of the mullite-type Bi2(FexGa1−x)4O9 (0.1≤x≤1) solid solution

The Bi₂(Fe_xGa_1−x)₄O₉ oxide solid solution possessing a mullite-type structure has been investigated by ⁵⁷Fe Mössbauer spectroscopy in dependence of composition (0.1≤x≤1) and temperature (293≤T/K≤1073). The spectra have been fitted with two doublets for tetrahedrally and octahedrally coordinated high-spin Fe³⁺ ions, respectively. The experimental areas of the subspectra were used to determine the distribution of iron on the two inequivalent structural sites. The fraction of iron cations occupying the octahedral site is found to increase with decreasing Fe content and the cation distribution is almost independent of temperature. The unusual temperature dependence of the quadrupolar splitting, QS, observed for the octahedral site with dQS/dT>0 is discussed in connexion with structural data for Bi₂Fe₄O₉. The temperature dependence of Mössbauer isomer shifts and signal intensities is examined in the context of local vibrational properties of iron on the two inequivalent sites of the mullite-type lattice structure.     

Crystal structure and ferroelectric property of Bi4Si3O12-added Bi4−xSmxTi3O12

We synthesized Bi_4?xSm_xTi₃O₁₂ (x=0.55, 0.65, 0.80) and y mol% Bi₄Si₃O₁₂-added Bi_4?xSm_xTi₃O₁₂ (x=0.65; y=5, 10, 15, 20) by a solid-state reaction, and investigated a relationship between the ferroelectric properties and crystal structures in these samples. From the P–E hysteresis measurements, it was clarified that the Bi_3.35Sm_0.65Ti₃O₁₂ showed better ferroelectric properties than the others with different Sm content, and the sample began to exhibit larger remanent polarization by adding Bi₄Si₃O₁₂. In order to examine an effect of the Bi₄Si₃O₁₂-addition from a structural point of view, we measured synchrotron X-ray diffractions of the samples at room temperature and 1000 K, and analyzed their crystal and electronic structures with the Rietveld technique and the maximum entropy method. As a result, it was suggested that the Bi₄Si₃O₁₂-addition made distortions of the Ti-O₆ octahedra larger and had an effect on the TiO bond strengths.     

Comparison of piezoelectricity in Ta and La substituted lead calcium titanate ceramics

This paper reports the experimental investigations on the effect of La³⁺ and Ta⁵⁺ substitution on the structural characteristics and dielectric and piezoelectric properties of lead calcium titanate (PCT) ceramic. The PCT samples with A-site and B-site substitution having the composition formula Pb_0.76−x/2La_xCa_0.24(Ti_0.98Mn_0.02)_1−x/2O₃ and Pb_0.76Ca_0.24Mn_0.02Ti _0.98−5x/4Ta_xO₃, x=0 and 0.02, respectively_, were prepared using conventional solid-state reaction method. Phase formation and structural analysis were studied using X-ray diffraction and scanning electron microscopy, respectively. Dielectric constant (ε′) and loss tangent (tan δ) as a function of frequency were measured at room temperature as well as elevated temperature. Both ε′ and tan δ decreased with increase in frequency at room temperature. Curie temperature decreased with La and Ta doping in PCT ceramics due to a decrease in the tetragonality of PCT ceramics. Piezoelectric charge coefficients (d₃₃, d₃₁) increased with La³⁺ substitution due to reorientation of the grains and decreased with Ta⁵⁺ substitution because of the increase in porosity. Figure of merit d_hg_h increased and decreased with La and Ta substitution, respectively. A good ferroelectric behaviour is obtained for La substitution, while no hysteresis is obtained for Ta substitution.     

Film structure and ferroelectric properties of in situ grown SrBi2Ta2O9 films

Ferroelectric SrBi₂Ta₂O₉ (SBT) films were grown by pulsed-laser deposition (PLD) at different substrate temperatures and fluences. A correlation between film structure and ferroelectric properties is established. The dielectric function ε^′ of thin SBT films shows a Curie–Weiss behavior well below the peak temperature T_max and relaxor-like behavior in the vicinity of T_max. Domain walls have a strong influence on the dielectric and ferroelectric properties and on the polarization fatigue of SBT films below 100 °C. The formation of ferroelectric phases is favored at lower substrate temperatures by incorporating Bi₂O₃ template layers into the structure. Received: 18 March 1999 / Accepted: 19 March 1999 / Published online: 5 May 1999     

Synthesis and ferroelectric properties of bismuth layer-structured (Bi7−xSrx)(Fe3−xTi3+x)O21 solid solutions

Bismuth layer-structured (Bi_7−xSr_x)(Fe_3−xTi_3+x)O₂₁ (BSFT) ceramics were synthesized and the ferroelectric properties and crystal structure were investigated. X-ray powder diffraction profiles and refinement of the lattice parameters indicated single phase BSFT was obtained in the composition range 0-1.5. The lattice parameter b of BSFT remained almost constant, while a slight decrease in the lattice parameter a was observed by the Sr and Ti substitution for Bi and Fe, respectively, which indicated an increase in the orthorhombicity. The dependence of the BSFT lattice parameter on temperature implied a phase transition from the orthorhombic to the tetragonal phase, which was in good agreement with the Curie temperature. The remnant polarization P_r, of BSFT was significantly improved by the Sr and Ti substitution for Bi and Fe, and ranged from 9 to 16 μC/cm², although no remarkable variation in the coercive field E_c was observed. As a result, a well-saturated P-E hysteresis loop of BSFT ceramic was obtained at x=0.5 with a P_r of 30 μC/cm at an applied voltage of 280 kV/cm.     

Enhanced ferroelectric, magnetic and magnetoelectric properties of Bi1−xCaxFe1−xTixO3 solid solutions

We report on the enhanced electromechanical, magnetic and magnetoelectric properties of Bi_1−xCa_xFe_1−xTi_xO₃ solid solutions. The crystal structure of the x≈0.25 compounds are close to the rhombohedral-orthorhombic phase boundary, and the solid solutions are characterized by increased electromechanical properties due to the polarization extension near the polar-nonpolar border. The homogenous weakly ferromagnetic state is established at x>0.15 doping. The chemical doping shifts the magnetic transition close to room temperature, thus enlarging the magnetic susceptibility of the compounds. The solid solutions at the morphotropic phase boundary exhibit a nearly twofold increase in piezoelectric response, whereas the magnetoelectric coupling shows five times enhancement in comparison with the parent bismuth ferrite.     

Sr位Nd掺杂对SrBi$lt;sub$gt;2$lt;/sub$gt;Nb$lt;sub$gt;2$lt;/sub$gt;O$lt;sub$gt;9$lt;/sub$gt;性能的影响及机理研究

采用传统固相法制备了（Sr_1-3x/2A_x/2Nd_x）Bi₂Nb₂O₉（x=0,0.05,0.1和0.2）陶瓷,并系统研究了Nd离子取代Sr离子对SrBi₂Nb₂O₉性能的影响及其作用机理.研究结果表明：Sr_1-3x/2A_x/2Nd_xBi₂Nb₂O₉的介电常数和介电损耗随温度变化的行为具有明显的离子松弛极化特征.Nd³⁺对Sr²⁺的部分取代,导致Sr_1-3x/2A_x/2Nd_xBi₂Nb₂O₉剩余极化强度P_r稍有下降,但其压电系数d₃₃却有所增加,根据铁电热力学理论,这是Nd³⁺对Sr²⁺取代导致材料介电常数增大所致.Sr_1-3x/2A_x/2Nd_xBi₂Nb₂O₉的居里温度（T_C）没有随Nd含量的增加而变化,拉曼光谱技术分析表明这是其NbO₆八面体畸变程度没有发生变化所致.Nd³⁺取代Sr²⁺提高了材料的介电常数ε_r、压电系数d₃₃、机电耦合系数K_p,同时降低了机械品质因数Q_m,但是谐振频率温度系数C值没有改变. 关键词： 压电陶瓷 介电性能 压电性能 拉曼光谱