Composition Limits and Magnetic Properties of Sintered Y2.66Gd0.34FexAl0.677Mn0.09O12 Garnets

Single-phase garnet solid solutions can be synthesized between the composition limits of x =4.18 and x =4.22 in Y_2.66Gd_0.34Fe _x Al_0.677Mn_0.09O₁₂ at temperatures between 1340° and 1500°C in O₂. Solid solutions occur only on the Y₂O₃-excess side of the stoichiometric garnet composition. Electromagnetic properties and microstructural features of sintered garnets depend critically on small changes in Fe content in the vicinity of the garnet solid-solution region. An intergranular spinel-type second phase exists for compositions when x >4.22 and has a deleterious effect on remanent induction and magnetic loss at 3 GHz. The relative density of powder compacts sintered for 16 h at 1500°C in O₂ increases with increasing Fe content (i.e. as x increases) in the garnet solid solution.     

Enhanced Dispersion Frequency of Hot-Pressed Z-Type Magnetoplumbite Ferrite with the Composition 2CoO·3Ba0.5Sr0.5O·10.8Fe2O3

The high-frequency magnetic properties of strontium-partially-substituted Z-type magnetoplumbite with the composition 2CoO·3Ba_1-x.Sr_xO.yFe₂O₃ were studied using a hot-pressing technique. The best properties were obtained for a sample hot-pressed in oxygen, having x and y values of 0.5 and 10.8, respectively. The resonant frequency of that sample, corresponding to a μ" maximum reaching 2.5 GHz, was significantly larger than the value of 1.4 GHz previously reported for unsubstituted Z with the composition 2CoO·3BaO·12Fe₂O₃. This result implies that a new ferrite material, applicable in the gigahertz region, has been obtained.     

Synthesis and Properties of Multiferroic La-Modified BiFeO3 Ceramics

Multiferroic Bi_{(1− x )}La _x FeO₃ was synthesized by a modified Pechini approach. Optimal conditions for the synthesis of single-phase Bi_{(1− x )}La _x FeO₃ powder were reported. A conventional sintering process was used to fabricate Bi_{(1− x )}La _x FeO₃ ceramics. Ferroelectric and magnetic loops measured at room temperature indicate the coexistence of ferroelectricity and magnetism. The La modification of BiFeO₃ has a beneficial effect on the ferroelectric and magnetic properties. The ceramic samples show a stable dielectric constant and quite low dielectric loss between 100 Hz and 10 MHz. The piezoelectric constants of Bi_{(1− x )}La _x FeO₃ ceramics were first reported.     

Electromechanical Properties of Pb(Yb1/2Nb1/2)O3-PbZrO3-PbTiO3 Ceramics

The electromechanical and electric-field-induced strain properties of x Pb(Yb_1/2Nb_1/2)O₃· y PbZrO₃·(1− x − y )PbTiO₃ ( x = 0.12, 0.25, 0.37; y = 0.10–0.40) ceramics have been studied systematically as a function of Pb(Yb_1/2Nb_1/2)O₃ (PYN) content and PbZrO₃/PbTiO₃ (PZ/PT) ratio. In addition, the effect of MnO₂ on the electromechanical properties of 0.12Pb(Yb_1/2Nb_1/2)O₃·0.40PbZrO₃·0.48PbTiO₃ was also investigated. The maximum transverse strain values of 1.6 × 10⁻³ for x = 0.12, 1.45 × 10⁻³ for x = 0.25, and 1.36 × 10⁻³ for x = 0.37 were obtained at the compositions which were regarded as the morphotropic phase boundary (MPB). The transverse strain was maximized at the MPB composition. The value of the maximum electromechanical coupling coefficient was 0.69 for y = 0.40 and x = 0.12 composition. In the 0.12Pb(Yb_1/2Nb_1/2)O₃·0.40PbZrO₃·0.48PbTiO₃ composition, the temperature of the maximum dielectric constant decreased and the grain size increased with an addition of MnO₂. The electromechanical coupling coefficient decreased while the mechanical quality factor rapidly increased with an addition of MnO₂. These resulted mainly from the acceptor effect of manganese ions that were produced by doping MnO₂ into the perovskite structure.     

The Li2O–Nb2O5–TiO2 Composite Microwave Dielectric Ceramics with Adjustable Permittivities

A group of new y M-phase/(1− y ) Li_{2+ x} Ti_{1−4 x} Nb_{3 x} O₃ composite ceramics with adjustable permittivities for low-temperature co-fired ceramic applications was initially investigated in the study. The 0.5 M-phase/0.5 Li_{2+ x} Ti_{1−4 x} Nb_{3 x} O₃ ( x =0.01, 0.02, 0.04, 0.06, 0.081) composite ceramics were first investigated to find the appropriate "Li₂TiO₃ss" composition ( x value). The best dielectric properties of ɛ_r=40.1, Q × f values up to 9318 GHz, τ_f=25 ppm/°C, were obtained for the ceramics composites at x =0.02. Based on the good dielectric properties, the suitable "Li₂TiO₃ss" composition with x =0.02 was mixed with the Li_1.0Nb_0.6Ti_0.5O₃ powder as the ratio of y "M-phase"/(1− y ) "Li₂TiO₃ss" ( y =0.2, 0.4, 0.5, 0.6, 0.8). By adjusting the y values, the group of composite ceramics could exhibit largely are adjustable permittivities varying from ∼20 to ∼60, while Q × f and τ_f values relatively good. Nevertheless, in this study, because there are interactions between the M-phase and Li₂TiO₃ss during sintering process, their microwave dielectric properties could not be predicted precisely by the empirical model.     

Photoluminescence of Rare-Earth-Doped Ca-α-SiAlON Phosphors: Composition and Concentration Dependence

Rare-earth-doped Ca-α-SiAlON phosphors, with the compositions of (Ca_{1−3/2 x} RE _x ) _{m /2}Si_{12− m − n} Al _m+n O _n N_{16− n} (RE=Ce, Sm, and Dy, 0.5≤ m =2 n ≤3.0), were prepared by sintering at 1700°C for 2 h under 10 atm N₂. The concentration of rare earths varied from 3 to 30 at.% with respect to Ca. The photoluminescence (PL) properties were investigated as functions of the composition of the host matrix (i.e., m ) and the concentration of rare earths (i.e., x ). The results show that the emission properties can be optimized by tailoring m and x . The Ce³⁺ luminescence originating from the 4 f –5 d interconfigurational transitions is greatly affected by the environment surrounding the Ce³⁺ ions, which differs from the Sm³⁺ or Dy³⁺ luminescence arising from the 4 f –4 f intraconfigurational transitions. X-ray diffraction and scanning electron microscopy were used to explain the composition and concentration dependence of PL properties.     

Microstructure and Microwave Dielectric Properties of (1−x)Ca(Mg1/3Ta2/3)O3/xCaTiO3 Ceramics

Dense (1− x )Ca(Mg_1/3Ta_2/3)O₃/ x CaTiO₃ ceramics (0.1≤ x ≤0.9) were prepared by a solid-state reaction process. The crystal structures and microstructures were characterized by X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Single-phase solid solutions were obtained in the entire composition range. Long-range 1:2 ordering of B-site cations and oxygen octahedra tilting lead to the monoclinic symmetry with space group P 2₁/ c for x =0.1. For x above 0.1, the long-range ordering was destroyed and the crystal structure became the orthorhombic with space group Pbnm . The microwave dielectric properties showed a strong dependence on the composition and microstructure. The dielectric constant and temperature coefficient of resonant frequency increased nonlinearly as the CaTiO₃ content increased while the Qf values decreased approximately linearly. Good combination of microwave dielectric properties was obtained at x =0.45, where ɛ_r=45.1, Qf =34 800 GHz, and τ_f=17.4 ppm/°C.     

Low-Temperature Sintering and Electromagnetic Properties of Copper-Modified Z-type Hexaferrite

The influence of the substitution of copper for cobalt on the low-sintering densification, microstructure, lattice parameters, and electromagnetic properties of planar Z-type hexaferrites, which have a stoichiometric composition of Ba₃Co_{2(10.8− x )}-Zn_0.4Cu_{2 x} Fe₂₄O₄₁, were investigated. The experimental results show that densification of the copper-substituted hexaferrite is dependent on the amount of copper substitution and sintering temperatures. XRD analysis reveals that the solid solubility of copper in Z-type hexaferrite is limited to x ≤ 0.30. At the same time, the lattice parameters ( a and c ) of Z-type hexaferrites with copper substitution showed a small change, that is, decrease of a parameter in the basal plane and increase of the c axial. Moreover, the microstructure becomes more homogeneous and intragranular pores decrease considerably, but the temperature-stable range of the Z-type phase formation is narrow. The copper-substituted hexaferrites, with x = 0.20 and sintered at ∼1125°C for 4 h, resulted in a high density sample of ∼4.68 g/cm³ as the optimal value, good magnetic properties, and the enormous potentiality for fabrication of multilayer chip inductors used in hyper-frequencies.     

The Effect of Sr Substitution on Phase Formation and Magnetic Properties of Y-type Hexagonal Ferrite

The effect of Sr substitution in Y-type hexagonal ferrite of composition Ba_{2– x} Sr _x Zn_1.2Co_0.4Cu_0.4Fe₁₂O₂₂ was investigated. x varied from 0 to 2.0. The samples were prepared by the solid-state reaction method. Phase formation was characterized by powder X-ray diffraction. The microstructure was observed via scanning electron microscopy and magnetic properties were measured using an impedance analyzer and vibrating sample magnetometer (VSM). Results reveal that Sr²⁺ cannot completely substitute for Ba²⁺ ions in Y-type hexagonal ferrites. The maximum solubility of Sr in the Y-type ferrite is about 1.8. With Sr above 1.8, the lattice mismatch induced by the difference in ionic radii of Ba²⁺ and Sr²⁺ ions prevents the formation of Y-type phase. While Sr content is equal or less than 1.0, the magnetic properties may be enhanced. As x >1.0, because of the internal stress resulting from the lattice mismatch, demagnetizing field significantly degrades initial permeability.     

Physical and Dielectric Properties of (1–x)PbZrO3·xBaTiO3 Thin Films Prepared by Chemical Solution Deposition

Physical and dielectric properties of (1– x )PbZrO₃· x BaTiO₃ thin films prepared by a chemical coating process have been investigated as a function of BaTiO₃ ( x ) content (0≤ x ≤0.2). Changing the molar ratio between propylene glycol and water prior to the deposition optimized the chemical precursors. (1– x )PbZrO₃- x BaTiO₃ thin films that contained a majority of perovskite phase, but also contained large amounts of other phases, were fabricated. These films could withstand fields of 250 kV/cm at 1 kHz. The microstructure of the thin films was found to depend on the BaTiO₃ content. The phase transition from antiferroelectric to ferroelectric was gradually induced as the BaTiO₃ content increased. A maximum dielectric constant of ∼809 was obtained at the composition of x = 0.1. A maximum dielectric constant of ∼809 was obtained at the composition of x = 0.1. A thin film at the low-field antiferroelectric-ferroelectric phase boundary with x = 0.05 exhibited the highest P _sat and P _r values. The maximum values of these were 45 and 31 μC/cm², respectively.     

Microstructure and Magnetic Properties of (Co-Fe)-Al-O Thin Films

(Co-Fe)-Al-O soft magnetic thin films were fabricated by cosputtering Co-Fe alloy and Al₂O₃ ceramic targets using an inductively coupled RF (radio frequency) sputtering system. The microstructure and magnetic properties of various (Co-Fe)/(Al-O) thin-film compositions were systematically characterized. A specimen with the composition (Co₇₂Fe₁₇Al₁₁)-O exhibited excellent high-frequency magnetic properties, with a value >300 for the real part of the permeability and >2 GHz for the self-resonant frequency. High-resolution transmission electron images revealed nanometer-order Al₂O₃ amorphous phases separating the Co-Fe alloy nanograins. The excellent high-frequency magnetic properties were derived from the particular microstructure of these thin films.     

Contribution of Structure to Temperature Dependence of Resonant Frequency in the (1 −x)La(Zn1/2Ti1/2)O3·xATiO3 (A = Ca, Sr) System

The crystal structure and microwave dielectric properties of the (1 − x ) La(Zn_1/2Ti_1/2)O₃· x SrTiO₃ and (1 − x )La(Zn_1/2Ti_1/2)O₃· x CaTiO₃ system were investigated. X-ray powder diffraction showed that cation ordering disappeared at x > 0.3 for both systems. However, infrared spectra demonstrated that short-range cation ordering could exist at x = 0.4. Permittivity and the temperature coefficient of the resonant frequency (τ_f) of both systems exhibited nonmonotonic variations with composition. Both systems exhibited a τ_f of zero at the same composition of x = 0.5 although the τ_f of SrTiO₃ was about two times larger than that of CaTiO₃. The behavior of the permittivity and τ_f were described by the tilting of oxygen octahedra and cation ordering. The relation between τ_f and cation ordering of La(Zn_1/2Ti_1/2)O₃ was discussed in conjunction with the experimental results on metal halides. It is suggested that cation ordering induced a negative τ_f and suppressed the increase of permittivity for compositions between x = 0 to x = 0.5 for (1 − x )La(Zn_1/2Ti_1/2)O₃· x SrTiO₃ and (1 − x )La(Zn_1/2Ti_1/2)O₃· x CaTiO₃ systems.     

Bismuth/Samarium Cosubstituted Ba6−3xNd8+2xTi18O54 Microwave Dielectric Ceramics

Modification of the microwave dielectric properties in Ba_{6−3 x} Nd_{8+2 x} Ti₁₈O₅₄ ( x = 0.5) solid solutions by Bi/Sm cosubstitution for Nd was investigated. A large increase in the dielectric constant and near-zero temperature coefficient combined with high Qf values were obtained in modified Ba_{6−3 x} Nd_{8+2 x} Ti₁₈O₅₄ solid solutions where an enlarged solid solution limit of Bi in Ba_{6−3 x} Nd_{8+2 x} Ti₁₈O₅₄ was observed. Excellent microwave dielectric characteristics (ɛ= 105, Qf = 4110 GHz, and very low τ_f) were achieved in the composition Ba_{6−3 x} (Nd_0.7Bi_0.18Sm_0.12)_{8+2 x} Ti₁₈O₅₄.     

Preparation and Spontaneous Polarization–Magnetization of a New Ceramic Ferroelectric–Ferromagnetic Composite

Ceramic composites with the composition of x PMZNT·(1 – x )NiCuZn have been prepared using a standard ceramic technique, in which x varies as 0, 0.1, 0.2, 0.4, 0.6, 0.9, and 1.0. PMZNT is the abbreviated form of 0.92Pb(Mg_1/3Nb_2/3)O₃·0.04Pb(Zn_1/3Nb_2/3)O₃·0.04PbTiO₃ (PMN-PZN-PT). NiCuZn is the abbreviated form of Ni_0.2Cu_0.2Zn_0.6Fe₂O₄. The presence of ferroelectric PMZNT phase and ferromagnetic NiCuZn ferrite phase has been confirmed using X-ray diffractometry. Ferroelectric hysteresis loops and magnetic hysteresis loops have been observed and studied. In polarization–electric-field curves, the remnant polarization and coercive fields display little asymmetric characterization because of the existence of the internal electric field. When the amount of NiCuZn ferrite phase increases, the coercive field increases. Meanwhile, the saturation magnetization decreases and the coercivity of the composites increases with the increase of phase fraction of PMZNT, because the interaction between magnetic grains (or magnetic connectivity) is weakened by the existence of nonmagnetic PMZNT phase distributed in the magnetic phases. Under an applied magnetic and electric field, the magnetization and polarization of the composites can be easily tuned. The sintered composites possess high density and fine-grained microstructure. The average grain size of NiCuZn ferrite grains is slightly larger than that of the PMZNT grains.     

Suppression of Liquid Film Migration and Improvement of Dielectric Properties in Niobium-Doped Strontium Titanate

In an attempt to improve the dielectric properties of SrTiO₃-based boundary-layer capacitors (BLCs), the effects of infiltrant composition on the liquid film migration and dielectric properties in 0.2-mol%-Nb₂O₅-doped SrTiO₃ were investigated. Powder compacts were sintered at 1480°C for 5 h in 5H₂·95N₂ and infiltrated with 80Bi₂O₃·20( x CaO–(1 – x )BaO) at 1300°C for various times in air. When the value of x was 0, 0.2, 0.7, and 1.0, liquid film migration occurred, which formed a new solid-solution layer containing solute species. On the other hand, when x = 0.5, no liquid film migration was observed. The effective dielectric constant was the highest in the sample with x = 0.5 (no liquid film migration), and it decreased as the migration distance increased. In addition, the loss tangent was the lowest, <1%, in the sample with x = 0.5. Agreement between the estimated effective dielectric constants and the measured values showed that the suppression of liquid film migration improved the dielectric constant. The agreement further indicated that the prediction of the dielectric constant in SrTiO₃-based BLCs was possible using a two-layer model with a liquid-infiltrated layer and a SrTiO₃-based oxidized layer.     

Microwave Dielectric Properties of CaTiO3-CaAl1/2Nb1/2O3 Ceramics Doped with Li3NbO4

The microwave dielectric properties of CaTi_{1− x} (Al_1/2Nb_1/2) _x O₃ solid solutions (0.3 ≤ x ≤ 0.7) have been investigated. The sintered samples had perovskite structures similar to CaTiO₃. The substitution of Ti⁴⁺ by Al³⁺/Nb⁵⁺ improved the quality factor Q of the sintered specimens. A small addition of Li₃NbO₄ (about 1 wt%) was found to be very effective for lowering sintering temperature of ceramics from 1450–1500° to 1300°C. The composition with x = 0.5 sintered at 1300°C for 5 h revealed excellent dielectric properties, namely, a dielectric constant (ɛ_r) of 48, a Q × f value of 32 100 GHz, and a temperature coefficient of the resonant frequency (τ_f) of −2 ppm/K. Li₃NbO₄ as a sintering additive had no harmful influence on τ_f of ceramics.     

Phase Structure and Electrical Properties of (K0.48Na0.52)(Nb0.95Ta0.05)O3-LiSbO3 Lead-Free Piezoelectric Ceramics

(1− x )(K_0.48Na_0.52)(Nb_0.95Ta_0.05)O₃– x LiSbO₃ [(1− x )KNNT− x LS] lead-free piezoelectric ceramics were prepared by the conventional solid-state sintering method. A morphotropic phase boundary (MPB) between orthorhombic and tetragonal phases was identified in the composition range of 0.03< x <0.05. The ceramics near the MPB exhibit a strong compositional dependence and enhanced electrical properties. The (1− x )KNNT– x LS ( x =0.04) ceramics exhibit good electrical properties ( d ₃₃=250 pC/N, k _p=45.1%, k _t =46.3%, T _c=348°C, T _{o − t} =74°C, P _r=25.9 μC/cm², E _c=10.7 kV/cm, ɛ_r∼1352, tan δ∼3%). These results show that (1− x )KNNT– x LS ceramic is a promising lead-free piezoelectric material.     

A Novel Temperature-Compensated Microwave Dielectric (1−x)(Mg0.95Ni0.05)TiO3−xCa0.6La0.8/3TiO3 Ceramics System

The microstructure and microwave dielectric properties of a (1− x )(Mg_0.95Ni_0.05)TiO₃− x Ca_0.6La_0.8/3TiO₃ ceramics system have been investigated. The system was prepared using a conventional solid-state ceramic route. In order to produce a temperature-stable material, Ca_0.6La_0.8/3TiO₃ was added for a near-zero temperature coefficient (τ_f). With partial replacement of Mg²⁺ by Ni²⁺, the dielectric properties of the (1− x )(Mg_0.95Ni_0.05)TiO₃− x Ca_0.6La_0.8/3TiO₃ ceramics can be promoted. The microwave dielectric properties are strongly correlated with the sintering temperature and the composition. An excellent Q × f value of 118,000 GHz can be obtained for the system with x =0.9 at 1325°C. For practical application, a dielectric constant (ɛ_r) of 24.61, a Q × f value of 102,000 GHz, and a temperature coefficient of resonant frequency (τ_f) of −3.6 ppm/°C for 0.85(Mg_0.95Ni_0.05)TiO₃−0.15Ca_0.6La_0.8/3TiO₃ at 1325°C are proposed. A parallel-coupled line band-pass filter is designed and simulated using the proposed dielectric to study its performance.     

Low-Fired (Zn,Mg)TiO3 Microwave Dielectrics

A dielectric ceramic comprised of (Zn_{1- x} Mg _x )TiO₃ ( x = 0 to x = 0.5) with low sintering temperature and promising microwave properties was prepared by applying a semichemical synthesis route and a microbeads milling technique. X-ray diffractometry and thermal analyses results indicated that the phase stability region of the hexagonal (Zn,Mg)TiO₃ extended to higher temperatures as the amount of magnesium increased. The dielectric properties in this system exhibited a significant dependence on the sintering conditions, especially near the phase decomposition temperature. From 950°C, the temperature compensation characteristics occurred as the phase composition changed from hexagonal (Zn,Mg)TiO₃ to two phases: (Zn,Mg)₂TiO₄ and rutile. The magnesium content for zero temperature coefficient (tau_f) was ~3 mol% at 950°C; however, tau_f increased with the sintering temperatures because of the shift of the decomposition temperature.     

Phase Structure and Dielectric Properties of Bi2O3-ZnO-Nb2O5-Based Dielectric Ceramics

Phase structures and dielectric properties of the compounds with formulas BixZn_2/3Nb_4/3O_4+3x/2 (group M), Bi_xZn_8/3-x Nb_4/3O_6+x/2 (group V), and Bi_xZn_2-2x/3Nb_2-x/3O₇ (group W) have been investigated. Initial results indicate that a cubic pyrochlore structure is the predominant phase of these compound. Most of the measured ceramic specimens exhibit dielectric properties suitable as temperatures-stable and temperature-compensating dielectrics in the capacitor industry. The values of the dielectric constant K are 80-160, while those of the temperature coefficient are–500 to + 160 ppm/°C. The composition limits of the single pyrochlore phase are determined mainly by Bi₂O₃ additives.