Magnetoelectric Properties of Multiferroic Composites Based on BaTiO3 and Nickel-Zinc Ferrite Material.

The purpose of the present study was to learn the morphological, structural, ferroelectric, dielectric, electromechanical, magnetoelectric, and magnetic properties, and DC conductivity of BaTiO3-Ni0.64Zn0.36Fe2O4 (BT-F) multiferroic composites compacted via the free sintering method. The influence of the ferrite content in ceramic composite materials on the functional properties is investigated and discussed. X-ray diffraction studies confirmed the presence of two main phases of the composite, with strong reflections originating from BaTiO3 and weak peaks originating from nickel-zinc ferrite. BT-F ceramic composites have been shown to exhibit multiferroism at room temperature. All studied compositions have high permittivity values and low dielectric loss, while the ferroelectric properties of the BT component are maintained at a high level. On the other hand, magnetic properties depend on the amount of the ferrite phase and are the strongest for the composition with 15 wt.% of F (magnetization at RT is 4.12 emu/g). The magnetoelectric coupling between BT and F phases confirmed by the lock-in technique is the largest for 15 wt.% ferrite. In the present work, the process conditions of the free sintering method for obtaining BT-F multiferroic composite with good electrical and magnetic properties (in one material) were optimized. An improved set of multifunctional properties allows the expansion of the possibilities of using multiferroic composites in microelectronics.

Properties of PBZTS Ferroelectric Ceramics Obtained Using Spark Plasma Sintering.

In this paper, spark plasma sintering was used to obtain and investigate (Pb0.97Ba0.03)(Zr0.98Ti0.02)1-xSnxO3 (PBZTS) ceramic materials for x = 0, 0.02, 0.04, 0.06, and 0.08. Crystal structure, microstructure, dielectric and ferroelectric properties, and electrical conductivity tests of a series of samples were carried out. The SPS sintering method ensures favorable dielectric and ferroelectric properties of PBZTS ceramic materials. X-ray studies have shown that the material has a perovskite structure. The samples have a densely packed material structure with properly crystallized grains. The fine-grained microstructure of the PZBZTS material with high grain homogeneity allows the application of higher electric fields. Ceramic samples obtained by the SPS method have higher density values than samples obtained by the classical method (FS). The permittivity at room temperature is in the range of 245-282, while at the phase transition temperature is in the range of 10,259-12,221. At room temperature, dielectric loss factor values range from 0.006 to 0.036. The hysteresis loops of PBZTS ceramics have a shape typical for ferroelectric hard materials, and the remnant polarization values range from 0.32 to 0.39 µC/cm2. The activation energy Ea values of the PBZTS samples result mainly from the presence of oxygen vacancies. The PZT material doped with Ba and Sn and sintered via the SPS method has favorable physical parameters for applications in modern devices such as actuators or pulse capacitors.

Electrophysical Properties of the Three-Component Multiferroic Ceramic Composites.

Using the free (pressureless) sintering method, multiferroic ceramic composites based on two ferroelectric materials, i.e., BaTiO3 (B) and Pb0.94Sr0.06 (Zr0.46Ti0.54)0.99Cr0.01O3 (P), and magnetic material, i.e., zinc-nickel ferrite (F) were obtained. Three composite compositions (BP-F) were obtained with a constant 90/10 content (ferroelectric/magnetic) and a variable content of the ferroelectric component (B/P), i.e., 70/30, 50/50, and 30/70. Crystalline structure, microstructural, DC electrical conductivity, dielectric, and ferroelectric properties of multiferroic composites were investigated. The concept of a composite consisting of two ferroelectric components ensures the preservation of sufficiently high ferroelectric properties of multiferroic composites sintered by the free sintering method. Research has shown that the percentage of individual ferroelectric components in the composite significantly affects the functional properties and the entire set of physical parameters of the multiferroic BP-F composite. In the case of the dielectric parameters, the best results were obtained for the composition with a more significant amount of BaTiO3; i.e., permittivity is 1265, spontaneous polarization is 7.90 µC/cm2, and remnant polarization is 5.40 µC/cm2. However, the most advantageous set of performance parameters shows the composite composition of 50BP-F.

Effect of Chemical Composition on Magnetic and Electrical Properties of Ferroelectromagnetic Ceramic Composites.

In this paper, ferroelectric-ferrimagnetic ceramic composites based on multicomponent PZT-type (PbZr1-xTixO3-type) material and ferrite material with different percentages in composite compositions were obtained and studied. The ferroelectric component of the composite was a perovskite ceramic material with the chemical formula Pb0.97Bi0.02(Zr0.51Ti0.49)0.98(Nb2/3Mn1/3)0.02O3 (P), whereas the magnetic component was nickel-zinc ferrite with the chemical formula Ni0.5Zn0.5Fe2O4 (F). The process of sintering the composite compounds was carried out by the free sintering method. Six ferroelectric-ferrimagnetic ceramic P-F composite compounds were designed and obtained with different percentages of its components, i.e., 90/10 (P90-F10), 85/15 (P85-F15), 80/20 (P80-F20), 60/40 (P60-F40), 40/60 (P40-F60), and 20/80 (P20-F80). X-ray diffraction patterns, microstructural, ferroelectric, dielectric, magnetic properties, and DC electrical conductivity of the composite materials were investigated. In this study, two techniques were used to image the microstructure of P-F composite samples: SB (detection of the signals from the secondary and backscattered electron detectors) and BSE (detection of backscattered electrons), which allowed accurate visualization of the presence and distribution of the magnetic and ferroelectric component in the volume of the composite samples. The studies have shown that at room temperature, the ceramic composite samples exhibit good magnetic and electrical properties. The best set of physical properties and performance of composite compositions have ceramic samples with a dominant phase of ferroelectric component and a small amount of the ferrite component (P90-F10). Such a composition retains the high ferroelectric properties of the ferroelectric component in the composite while also acquiring magnetic properties. These properties can be prospectively used in new types of memory and electromagnetic converters.

The Effect of Mixed Doping on the Microstructure and Electrophysical Parameters of the Multicomponent PZT-Type Ceramics.

This work shows the influence of admixture on the basic properties of the multicomponent PbZr1-xTixO3 (PZT)-type ceramics. It presents the results of four compositions of PZT-type material with the general chemical formula, Pb0.99M0.01((Zr0.49Ti0.51)0.95Mn0.021Sb0.016W0.013)0.9975O3, where, in the M position, a donor admixture was introduced, i.e., samarium (Sm3+), gadolinium (Gd3+), dysprosium (Dy3+) or lanthanum (La3+). The compositions of the PZT-type ceramics were obtained through the classic ceramic method, as a result of the synthesis of simple oxides. The X-ray diffraction (XRD) pattern studies showed that the obtained multicomponent PZT materials have a tetragonal structure with a P4mm point group. The microstructure of the obtained compositions is characterized by a well crystallized grain, with clearly visible grain boundaries. The composition with the admixture of lanthanum has the highest uniformity of fine grain microstructure, which positively affects its final dielectric and piezoelectric properties. In the multicomponent PZT-type ceramic, materials utilize the mixed (acceptor and donor) doping of the main compound. This dopiong method has a positive effect on the set of the electrophysical parameters of ceramic materials. Donor dopants W6+ (at positions B) and M3+ = Sm3+, Gd3+, Dy3+, and La3+ (at positions A) increase the dielectric and piezoelectric properties, while the acceptor dopant Sb3+ (at positions B) increases the time and temperature stability of the electrophysical parameters. In addition, the suitable selection of the set of admixtures improved the sinterability of the ceramic samples, as well as resulted in obtaining the required material with good piezoelectric parameters for the poling process. This research confirms that all ceramic compositions have a set of parameters suitable for applications in micromechatronics, for example, as actuators, piezoelectric transducers, and precision microswitches.

Comparison of Electrophysical Properties of PZT-Type Ceramics Obtained by Conventional and Mechanochemical Methods.

In the paper, the multicomponent PZT-type ceramics with Pb(Zr0.49Ti0.51)0.94Mn0.015Sb0.01W0.015Ni0.03O3 composition have been obtained by conventional and mechanochemical methods. With conventional ceramic technology, PZT-type ceramics have been synthesized by the method of calcination powder (850 °C/4 h). Instead of this step, the mechanochemical synthesis process for different milling periods (15 h, 25 h, 50 h, 75 h) has been applied for a second batch of samples. To obtain the dense PZT-type ceramic samples, powders have been sintered by free sintering method at conditions of 1150 °C/2 h. Studies have shown that the perovskite structure of the PZT-type material is formed during mechanochemical activation of powders during the technological process at low temperature. The application of the mechanochemical synthesis to obtain the PZT-type materials also allows shortening of the technological process, and the useful electrophysical properties of ceramic samples are not reduced at the same time. The presented results have confirmed that the investigated materials can be used in microelectronic applications, especially as elements of actuators and piezoelectric transducers.

Electrophysical Properties of PMN-PT-Ferrite Ceramic Composites.

Ferroelectromagnetic composites based on (1-x)PMN-(x)PT (PMN-PT) powder and Ni-Zn ferrite powder were obtained and are described in this work. As a ferroelectric component, we used (1-x)PMN-(x)PT solid solution (with x = 0.25, 0.28, 0.31, 0.34, 0.37, 0.40), synthesized using the sol-gel method. As a magnetic component, we used nickel-zinc ferrite, obtained using classic ceramic technology. The six compositions of PMN-PT used have rhombohedral symmetry, tetragonal one and mixture of these phases (morphotropic phase area), depending on x. The final ceramic composite samples were obtained using the classic methods involving the calcination route and pressureless final sintering (densification). The properties of the obtained ceramic composite samples were investigated, including microstructure SEM (scanning electron microscope), dielectric properties, electromechanical properties, and DC (Direct Current) electrical conductivity. Results showed that the microstructures of the PP-F composite samples characterized by larger grains were better crystallized, compared with the microstructures of the PMN-PT ceramic samples. The magnetic properties do not depend on the ferroelectric component of the composite samples, while the insertion of ferrite into the PMN-PT compound reduces the values of remnant and spontaneous polarization, as well as the coercive field. The dielectric measurements also indicated that the magnetic subsystem influences the dielectric properties. The present results show that the PP-F ceramic composite has good dielectric, magnetic, and piezoelectric properties, which predisposes this type of material to specific applications in microelectronics and micromechatronics.

Ferroelectromagnetic Properties of PbFe1/2Nb1/2O3 (PFN) Material Synthesized by Chemical-Wet Technology.

In this work, PbFe1/2Nb1/2O3 (PFN) ceramic samples synthesized by chemically wet method (precipitation from the solution) were obtained. Due to the tendency to form powder agglomerates, the synthesized powder was subjected to ultrasound. The sintering was carried out under various technological conditions, mainly through controlling the sintering temperature. -X-ray powder-diffraction (XRD), scanning electron microscope (SEM) microstructure analysis, as well as the examinations of dielectric, ferroelectric, and magnetic properties of the PFN ceramics were carried out. Studies have shown that hard ceramic agglomerates can be partially minimized by ultrasound. Due to this treatment, closed porosity decreases, and the ceramic samples have a higher density. Optimization and improvement of the technological process of the PFN material extends the possibility of its use for the preparation of multiferroic composites or multicomponent solid solutions based on PFN. Such materials with functional properties find applications in microelectronic applications, e.g., in systems integrating ferroelectric and magnetic properties in one device. The optimal synthesis conditions of PFN ceramics were determined to be 1050 °C/2 h.

Electrophysical Properties of the PMN⁻PT⁻PS Solid Solution.

The (1 - y) ((1 - x)Pb(Mg1/3Nb2/3)O3⁻xPbTiO3)⁻yPbSnO3 solid solution (PMN⁻PT⁻PS) was obtained and investigated in the present paper. For the analysis of the influence of the PbSnO3 component on the electrophysical parameters, the compositions from the rhombohedral phase, tetragonal phase, and a mixture of these phases were selected. The six compositions of the PMN⁻PT have been obtained using sol⁻gel methods (for values of x equal to 0.25, 0.28, 0.31, 0.34, 0.37, and 0.40). The ceramic samples of the 0.9(PMN⁻PT)⁻0.1(PS) solid solution have been obtained using the conventional ceramic route. X-ray diffraction (XRD), energy dispersive spectrometry (EDS), and microstructure measurements were performed, as well as tests regarding the dielectric, ferroelectric, piezoelectric properties and electric conductivity of the PMN⁻PT⁻PS ceramic samples versus temperature. Results of the measurements show that the obtained PMN⁻PT⁻PS materials have good electrophysical properties and are well suited for use in micromechatronic and microelectronic applications.