Polymorphic phase transition-induced electrical behavior of BiCoO3-modified (K0.48Na0.52)NbO3 lead-free piezoelectric ceramics

(1 − x)(K_0.48Na_0.52)NbO₃-xBiCoO₃ [KNN-xBC] lead-free piezoelectric ceramics were prepared by the conventional solid-state sintering method. The effects of the BiCoO₃ addition on the phase structure, dielectric, piezoelectric and ferroelectric properties of KNN-xBC ceramics were systematically investigated. The polymorphic phase transition (PPT) from rhombohedral to orthorhombic phase around room temperature was identified in the composition range of 0.01 ≤ x ≤ 0.02, and the improved electrical properties were induced by this PPT. The KNN-0.01BC ceramics near PPT exhibit optimum electrical properties: d₃₃ ∼ 165 pC/N, k_p ∼ 0.40, P_r ∼ 31.0 μC/cm², and E_c ∼ 12.6 kV/cm. These results indicate that the enhanced piezoelectric properties for alkali niobate can be achieved by forming the coexistence of rhombohedral and orthorhombic phases.     

X-ray diffraction and dielectric studies across morphotropic phase boundary in (1 − x) [Pb(Mg0.5W0.5)O3]-xPbTiO3 ceramics

We present here the results of comprehensive X-ray diffraction and dielectric studies on several compositions of (1 − x)[Pb(Mg_0.5W_0.5)O₃]-xPbTiO₃ (PMW-xPT) solid solution across the morphotropic phase boundary. Rietveld analysis of the powder X-ray diffraction data reveals cubic (space group Fm3m) structure of PMW-xPT ceramics for the compositions with x ≤ 0.42, tetragonal (space group P4mm) structure for the compositions with x ≥ 0.72 and coexistence of the tetragonal and cubic phases for the intermediate compositions (0.46 ≤ x ≤ 0.68). Temperature dependence of the dielectric permittivity above room temperature exhibits diffuse nature of phase transitions for the compositions in the cubic and two phase region while the compositions with tetragonal structure at room temperature exhibit sharp ferroelectric to paraelectric phase transition. The PMW-xPT compositions with coexistence of tetragonal and cubic phases at room temperature exhibit two anomalies in the temperature dependence of the dielectric permittivity above room temperature. Using results of structural and dielectric studies a partial phase diagram of PMW-xPT ceramics is also presented.     

High permittivity and low dielectric loss of the Ca1−xSrxCu3Ti4O12 ceramics

The Ca_1−xSr_xCu₃Ti₄O₁₂ (CSCTO) giant dielectric ceramics were prepared by conventional solid-state method. X-ray diffraction patterns revealed that a small amount of Sr²⁺ (x < 0.2) had no obvious effect on the phase structure of the CSCTO ceramics, while with increasing the Sr²⁺ content, a second phase of SrTiO₃ appeared. Electrical properties of CSCTO ceramics greatly depended on the Sr²⁺ content. The Ca_0.9Sr_0.1Cu₃Ti₄O₁₂ ceramics exhibited a higher permittivity (71,153) and lower dielectric loss (0.022) when measured at 1 kHz at room temperature. The ceramics also performed good temperature stability in the temperature range from −50 °C to 100 °C at 1 kHz. By impedance spectroscopy analysis, all compounds were found to be electrically heterogeneous, showing semiconducting grains and insulating grain boundaries. The grain resistance was 1.28 Ω and the grain boundary resistance was 1.31 × 10⁵ Ω. All the results indicated that the Ca_0.9Sr_0.1Cu₃Ti₄O₁₂ ceramics were very promising materials with higher permittivity for practical applications.     

Low-firable high-K dielectric in the Zrx(Zn1/3Nb2/3)1−xTiO4 ceramic system

Composite ceramics in the solid solution of Zr_x(Zn_1/3Nb_2/3)_1−xTiO₄ (x = 0.1-0.4) have been prepared by the mixed oxide route. Formation of solid solution was confirmed by the X-ray diffraction patterns. The microwave dielectric properties, such as dielectric constant (?_r), Q × f value and temperature coefficient of resonant frequency (τ_f) have been investigated as a function of composition and sintering temperature. With x increasing from 0.1 to 0.4, the dielectric constant decreases from 70.9 to 43.2, and the τ_f decreases from 105 to 55 ppm/°C. The Q × f value, however, increases with increasing x value to a maximum 26,600 GHz (at 6 GHz) at x = 0.3, and then decreases thereafter. For low-loss microwave applications, a new microwave dielectric material Zr_0.3(Zn_1/3Nb_2/3)_0.7TiO₄, possessing a fine combination of microwave dielectric properties with a high ?_r of 51, a high Q × f of 26,600 GHz (at 6 GHz) and a τ_f of 70 ppm/°C, is suggested.     

Rhombohedral-monoclinic phase transition related to grain orientation in Zr-rich Pb(ZrxTi1−x)O3 thin films

Pb(Zr_xTi_1−x)O₃ thin films with mixed orientations of (1 1 1) and (1 0 0) were prepared on Pt/Ti/SiO₂/Si substrate by sol-gel technique. The compositions of PZT thin films are chosen as x = 0.55 and x = 0.58. Both of the compositions are in the rhombohedral phase region of the Pb(Zr_xTi_1−x)O₃ phase diagram, but the former is near the monoclinic phase existence region, and the latter is far from the monoclinic phase existence region. Rhombohedral-monoclinic phase transitions are reported in both of the thin films. The results show that the phase transition is related to the grain orientation. Phase transitions in the films are clearly identified: rhombohedral phase transforms to M_B phase in (1 1 1)-oriented grains, and rhombohedral phase transforms to M_A phase in (1 0 0)-oriented grains. The remnant polarization is determined by the content of (1 1 1)-oriented grains. It is shown that the remnant polarization is greater in the film with higher content of (1 1 1)-oriented grains.     

Synthesis, structural and microwave dielectric properties of Al2W3−xMoxO12 (x = 0-3) ceramics

Low dielectric ceramics in the Al₂W_3−xMo_xO₁₂ (x = 0-3) system have been prepared through solid state ceramic route. The phase purity of the ceramic compositions has been studied using powder X-ray diffraction (XRD) studies. The microstructure of the sintered ceramics was evaluated by Scanning Electron Microscopy (SEM). The crystal structure of the ceramic compositions as a result of Mo substitution has been studied using Laser Raman spectroscopy. The microwave dielectric properties of the ceramics were studied by Hakki and Coleman post resonator and cavity perturbation techniques. Al₂Mo_xW_3−xO₁₂ (x = 0-3) ceramics exhibited low dielectric constant and relatively high unloaded quality factor. The temperature coefficient of resonant frequency of the compositions is found to be in the range −41 to −72 ppm/°C.     

Improving the piezoelectric thermal stability by tailoring phase transition behavior in the new (1 − x)[0.65PbMg1/3Nb2/3O3-0.35PbTiO3]-xBiZn1/2Ti1/2O3 perovskite solid solutions

The phase transition behavior and its effect on thermal stability of the piezoelectric properties of the (1 − x)[0.65PbMg_1/3Nb_2/3O₃-0.35PbTiO₃]-xBiZn_1/2Ti_1/2O₃ ceramics with 0 ≤ x ≤ 0.06 were investigated. The phase transition from the monoclinic to tetragonal phase was determined by the dielectric constant and elastic constant measurements. The temperature independent piezoelectric response with −d₃₁ = 188 pC/N was obtained from 175 to 337 K for the composition with x = 0.02. The enhanced thermal stability of piezoelectric response was achieved by shifting the monoclinic-tetragonal phase transition to the lower temperature.     

Crystal structure and microwave dielectric properties of ZnTi(Nb1−xTax)2O8 ceramics

The crystal structure and microwave dielectric properties of ZnTi(Nb_1−xTa_x)₂O₈ (0 ≤ x ≤ 1) ceramics sintered at 1200 °C for 2 h were investigated. For x < 0.5, solid solution phases with the α-PbO₂ structure, typical of ZnTiNb₂O₈, were obtained, whereas for 0.5 ≤ x < 1, mixtures of two solid solutions each respectively based on the α-PbO₂ structure and a trirutile structure, were obtained. The relative amount of the trirutile-structured phases increased as the Ta content increased in a given region, and the end member ZnTiTa₂O₈ formed a single phase with the trirutile structure. The microwave dielectric properties were closely related to the crystal structures. A material with a near zero temperature coefficient of resonant frequency could be obtained for x = 0.8, and its dielectric constant and quality factor (Q × f) were 40.5 and 41,000 GHz, respectively.     

Relationships between Zr substitution for Ti and microwave dielectric properties in Mg(ZrxTi1−x)O3 ceramics

The influence of Zr substitution for Ti on the microwave dielectric properties and microstructures of the Mg(Zr_xTi_1−x)O₃(MZ_xT) (0.01 ≤ x ≤ 0.3) ceramics was investigated. The quality factors of Mg(Zr_xTi_1−x)O₃ ceramics with x = 0.01-0.05 were improved because the solid solution of a small amount of Zr⁴⁺ substitution in the B-site could increase density and grain size. An excess of Zr⁴⁺ resulted in the formation of a great deal of secondary phase that declined the microwave dielectric properties of MZ_xT ceramics. The temperature coefficient of resonant frequency (τ_f) of Mg(Zr_xTi_1−x)O₃ ceramics slightly increased with increasing Zr content, and the variation in τ_f was attributed to the formation of secondary phases.     

Dielectric and tunability properties of La-doped BaTiO3 ceramics

La-doped BaTiO₃ (x = 0.001; 0.0025; 0.005; 0.01; 0.025) ceramics were prepared via conventional solid state reaction and sintered at 1300 °C for 6 h, resulting in dense single phase ceramics with homogeneous microstructures. The temperature dependence of dielectric permittivity of the ceramics has been investigated. The results show a decrease of T_C with lanthanum addition. The degree of diffuseness of phase transition is more pronounced for high La content, implying the existence of a composition-induced phase transition of the ceramics. The dc-tunability at room temperature was investigated and experimental data were discussed in terms of the Johnson model completed with a Langevin term that describes “extrinsic” contribution to the non-linear ?(E) dependences.     

Microwave dielectric properties of temperature stable Li2ZnxCo1−xTi3O8 ceramics

The Li₂Zn_xCo_1−xTi₃O₈ (x = 0.2-0.8) solid solution system has been synthesized by the conventional solid-state ceramic route and the effect of Zn substitution for Co on microwave dielectric properties of Li₂CoTi₃O₈ ceramics has also been investigated. The microwave dielectric properties of these ceramics show a linear variation between the end members for all compositions. The optimized sintering temperatures of Li₂Zn_xCo_1−xTi₃O₈ ceramics increase with increasing content of Zn. The specimen with x = 0.4 sintered at 1050 °C/2 h exhibits an excellent combination of microwave dielectric properties with ?_r = 27.7, Q_u × f = 57,100 GHz and τ_f = −1.0 ppm/°C.     

Ferroelectric relaxor behavior and dielectric spectroscopic study of 0.99(Bi0.5Na0.5TiO3)-0.01(SrNb2O6) solid solution

0.99(Bi_0.5Na_0.5TiO₃)-0.01(SrNb₂O₆) was prepared by simple solid state reaction route. Material stabilized in rhombohedral perovskite phase with lattice constants a = 3.9060 Å, α = 89.86° and a_h = 5.4852 Å, c_h = 6.7335 Å for hexagonal unit cells. Density of material was found 5.52 g_m/cm³ (92.9% of theoretical one) in the sample sintered at 950 °C. The temperature dependent dielectric constant exhibits a broad peak at 538 K (?_m = 2270) at 1 kHz that shows frequency dependent shifts toward higher temperature - typical relaxor behavior. Modified Curie-Weiss law was used to fit the dielectric data that exhibits almost complete diffuse phase transition characteristics. The dielectric relaxation obeys the Vogel-Fulcher relationship with the freezing temperature 412.4 K. Significant dielectric dispersion is observed in low frequency regime in both components of dielectric response and a small dielectric relaxation peak is observed. Cole-Cole plots indicate polydispersive nature of the dielectric relaxation; the relaxation distribution increases with increase in temperature.     

Structure and electrical properties of MnO2-doped Sr2−xCaxNaNb5O15 lead-free piezoelectric ceramics

Lead-free piezoelectric ceramics Sr_2−xCa_xNaNb₅O₁₅ + y wt% MnO₂have been prepared by the conventional solid state reaction method. Our results reveal that Ca²⁺and Mn ions have entered into the Sr₂NaNb₅O₁₅ lattices to form a solid solution with tungsten-bronze structure. The substitution of Ca²⁺ induces a decrease in piezoelectric coefficient d₃₃, electromechanical coupling factors k_p and k_t, while, the addition of Mn ions decreases the sintering temperature and effectively promotes the densification of the ceramics. The effect of substitution of Ca²⁺and Mn ions on the structure, electrical properties and diffused phase changing were investigated systematically. For the ceramic with x = 0.05 and y = 0.5, the piezoelectric, dielectric and ferroelectric properties become optimum, giving a piezoelectric coefficient d₃₃ = 190 pC/N, electromechanical coupling factors k_p = 13.4% and k_t = 36.5%, ?_r = 2123, loss tangent tan δ = 0.038, remanent polarization P_r = 4.76 μC/cm², coercive field E_c = 12.68 kV/cm, and Curie temperature T_c = 260 °C.     

Microwave dielectric properties of (Zn1−xMgx)TiO3 (ZMT) ceramics for dielectric resonator antenna application

Present investigation provides experimental studies on cylindrical dielectric resonator antennas (CDRAs) fabricated from (Zn_1−xMg_x)TiO₃ (ZMT) ceramic material with different substitution of Mg in place of Zn (x = 0.1, 0.2, 0.3, 0.4 and 0.5) along with measurement of material permittivity in C-band of microwave frequencies. The dielectric properties of the ZMT ceramic materials with different x values (x = 0.1-0.5) have been measured at microwave frequencies using Hakki-Coleman method modified by Courtney. The value of dielectric constant and loss tangent decreases with the increase in Mg content. The dielectric constant is minimum for x = 0.3 and loss tangent is minimum for x = 0.5. The variations of return loss and input impedance versus frequency and radiation patterns of CDRAs at their respective resonant frequencies are studied experimentally. The measured results for resonant frequency and return loss bandwidth of the CDRAs are also compared with theoretical ones. The measured resonant frequencies of all the four CDRAs are nearly in agreement with respective theoretical values and the values of input resistance at respective resonant frequencies of the CDRAs match well with the coaxial feed impedance of 50 Ω. The designed CDRAs have broad beam, low side lobe and cross-polarized lobe levels.     

Microstructure, ferroelectric, and piezoelectric properties of (1 − x − y)Bi0.5Na0.5TiO3-xBaTiO3-yBi0.5Ag0.5TiO3 lead-free ceramics

Lead-free (1 − x − y)Bi_0.5Na_0.5TiO₃-xBaTiO₃-yBi_0.5Ag_0.5TiO₃ (BNT-BT-BAT-x/y, x = 0-0.10, y = 0-0.075) piezoelectric ceramics were synthesized by conventional oxide-mixed method. The microstructure, ferroelectric, and piezoelectric properties of the ceramics were investigated. Results show that a morphotropic phase boundary (MPB) between rhombohedral and tetragonal phases of BNT-BT-BAT-x/0.04 ceramics is formed at x = 0.06-0.08. The addition of BAT has no obvious change on the crystal structure of BNT-BT ceramics while it causes the grain size of the ceramics to become more homogenous. Near the MPB, the ceramics with x = 0.06 and y = 0.05-0.06 possess optimum electrical properties: P_r ∼ 42.5 μC/cm², E_c ∼ 32.0 kV/cm, d₃₃ ∼ 172 pC/N, k_p ∼ 32.6%, and k_t ∼ 52.6%. The temperature dependences of k_p and polarization versus electric hysteresis loops reveal that the depolarization temperature (T_d) of BNT-BT-BAT-0.06/y ceramics decreases with increasing y. In addition, the polar and non-polar phases may coexist in the BNT-BT-BAT-x/y ceramics above T_d.     

Piezoelectric and dielectric properties of Dy2O3-doped (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free ceramics

(Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ + x wt% Dy₂O₃ with x = 0-0.3 ceramics were synthesized by conventional solid-state processes. The effects of Dy₂O₃ on the microstructure, the piezoelectric and dielectric properties were investigated. X-ray diffraction pattern confirmed that the coexistence of tetragonal and rhombohedral phases in the (Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ composition was not changed by adding 0.05-0.3 wt% Dy₂O₃. SEM images indicate that all the ceramics have pore-free microstructures with high density, and that doping of Dy₂O₃ inhibits the grain growth of the ceramics. The addition of Dy₂O₃ shows the double effects on decreasing the piezoelectric and dielectric properties for 0 < x < 0.15 when Dy³⁺ ions substitute B-site Ti⁴⁺ ions, and increasing the properties for 0.15 < x < 0.3 when Dy³⁺ ions enters into A-site of the perovskite structure. The optimum electric properties of piezoelectric constant d₃₃ = 170 pC/N and the dielectric constant ?_r = 1900 (at a frequency of 1 kHz) are obtained at x = 0.3.     

Dielectric properties of Cu substituted Ni0.5−xZn0.3Mg0.2Fe2O4 ferrites

Dielectric properties of Cu substituted Ni-Zn-Mg ferrite samples having the general formula Ni_0.5−xCu_xZn_0.3Mg_0.2Fe₂O₄ (where x = 0.0, 0.1, 0.2, 0.3, 0.4, and 0.5) synthesized by Pramanik method are reported. The single phase formation of the ferrites was confirmed by XRD technique. The lattice parameter is found to increase with increase in Cu content. Average grain size, obtained from SEM micrographs, is found to increase with increase in Cu content. Dielectric parameters were measured as a function of frequency at room temperature as well as at higher temperatures. The variation in dielectric constant (?′) with temperature at four different fixed frequencies viz. 1 kHz, 10 kHz, 100 kHz, and 1 MHz was also studied. The room temperature dielectric constant (?′) and dielectric loss (tan δ) are found to decrease with increase in frequency. The ac conductivity (σ_ac) is found to increase with increase in the frequency.     

Dielectric and magnetic behavior of BaCd2−xSrxFe16O27 W-type hexagonal ferrites

We have prepared BaCd_2−xSr_xFe₁₆O₂₇ (x = 0, 0.5, 1, 1.5 and 2.0) W-type hexagonal ferrites by standard ceramic method. In this work, the structural, dielectric and magnetic properties have been studied of the prepared samples. The XRD analysis of the samples reveals single phase behavior sintered at 1400 °C for 6 h. The saturation magnetization (M_s) shows increasing behavior with the increasing concentration of Sr²⁺. While the coercivity (H_c) decreases rapidly up to 409 G for x = 1.5 and then increases for (x > 1.5) due to the preference of Cd²⁺ for tetrahedral sites and the number of spin-down magnetic ions. The real and imaginary parts of the dielectric constant (?′,?″) and dielectric loss tangent (tan δ) are determined in the frequency range 0.1-10⁷ Hz. It is observed that both the real and imaginary parts of the dielectric constant and tan δ decrease with the increasing concentration of Sr²⁺, which is due to the contribution of Cd²⁺ ions in addition to Fe³⁺ and Fe²⁺ ions to interfacial polarization.     

Effects of lanthanum doping on the preferred orientation, phase structure and electrical properties of sol-gel derived Pb1-3x/2Lax (Zr0.6Ti0.4)O3 thin films

Pb_1-3x/2La_x (Zr_0.6Ti_0.4)O₃ thin films (0 ≤ x ≤ 0.08) were prepared on the Pt (1 1 1)/Ti/SiO₂/Si (1 0 0) substrates by a sol-gel method. The morphology, preferred orientation, phase structure, dielectric and ferroelectric properties of the films have been investigated. Our results show that lanthanum doping is favorable to enhance crystalline and obtain (1 0 0)-preferred orientation of the films. Meanwhile, it is suggested that the films undergo a structure change from “rhombohedral” phase to monoclinic phase as the lanthanum-doped content is increased to x ≈ 0.05. Results of dielectric properties and ferroelectric properties indicate that lanthanum doping contributes to improve film dielectric constant and dielectric loss while it brings about a striking decrease in remnant polarization value. Possible explanations for the variations of electrical properties have been discussed in terms of preferred orientation, phase structure and large lattice distortion.     

AC conductivity and dielectric properties of GeSexTl0.3 amorphous thin films

AC conductivity and dielectric properties have been studied for amorphous thin films with different thicknesses of glassy system GeSe_xTl_0.3 with X = 3, 4 that prepared with thermal evaporation technique. The measurements are taken at temperature range (303-403 K) and frequency range (10²-10⁵ Hz).AC conductivity σ_ac(ω) is found to be proportional to ω^s where s < 1. The temperature dependence of the ac conductivity and the parameter s can be discussed with the aim of the correlated barrier-hopping (CBH) model.The dielectric constant ?′and the dielectric loss ?″ showed frequency and temperature dependence. The maximum barrier height W_M calculated from the dielectric measurements according to Giuntini equation are in good agreement with that proposed by the theory of hopping of charge carriers over a potential barrier as suggested by Elliott in the case of chalcogenide glasses.