Dielectric relaxation and conduction mechanism in LaNi3/4M1/4O3 (M = Mo, W) at low temperature

In order to investigate the electrical transport in LaNi_3/4Mo_1/4O₃ and LaNi_3/4W_1/4O₃, the dc conductivity and dielectric properties in these polycrystalline materials are investigated in the temperature range from 163 K to 383 K and frequency range from 50 Hz to 1 MHz. The X-ray diffraction patterns of the samples show monoclinic phase at room temperature. The homogeneity of the samples is determined by energy dispersive analysis of X-ray (EDAX) attached with a scanning electron microscope. The temperature dependence of dc conductivity shows the semiconducting nature of the materials. The complex impedance plane plots show that the relaxation (conduction) mechanism in these materials is purely a bulk effect arising from the semiconductive grains. The frequency-dependent electrical data are also analyzed in the framework of ac conductivity formalism. The ac conductivity spectra follow the universal power law. The activation energies required for bulk conduction is 0.143 and 0.165 eV for LNM and LNW respectively. The scaling behaviour of loss tangent suggests that the relaxation describes the same mechanism at various temperatures.     

Structural and dielectric properties of Bi2Zn2/3Nb4/3O7 thin films prepared by pulsed laser deposition at low temperature for embedded capacitor applications

Bi₂Zn_2/3Nb_4/3O₇ thin films were deposited on Pt/TiO₂/SiO₂/Si(1 0 0) substrates at a room temperature under the oxygen pressure of 1-10 Pa by pulsed laser deposition. Bi₂Zn_2/3Nb_4/3O₇ thin films were then post-annealed below 200 °C in a rapid thermal process furnace in air for 20 min. The dielectric and leakage current properties of Bi₂Zn_2/3Nb_4/3O₇ thin films are strongly influenced by the oxygen pressure during deposition and the post-annealing temperature. Bi₂Zn_2/3Nb_4/3O₇ thin films deposited under 1 Pa oxygen pressure and then post-annealed at a temperature of 150 °C show uniform surface morphologies. Dielectric constant and loss tangent are 57 and 0.005 at 10 kHz, respectively. The high resolution TEM image and the electron diffraction pattern show that nano crystallites exist in the amorphous thin film, which may be the origin of high dielectric constant in the Bi₂Zn_2/3Nb_4/3O₇ thin films deposited at low temperatures. Moreover, Bi₂Zn_2/3Nb_4/3O₇ thin film exhibits the excellent leakage current characteristics with a high breakdown strength and the leakage current density is approximately 1 × 10⁻⁷ A/cm² at an applied bias field of 300 kV/cm. Bi₂Zn_2/3Nb_4/3O₇ thin films are potential materials for embedded capacitor applications.     

Dielectric relaxation behaviors of pure and Pr6O11-doped CaCu3Ti4O12 ceramics in high temperature range

Pure and Pr₆O₁₁-doped CaCu₃Ti₄O₁₂ (CCTO) ceramics were prepared by conventional solid-state reaction method. The compositions and structures were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The influences of Pr-ion concentration on dielectric properties of CCTO were measured in the ranges of 60 Hz-3 MHz and 290-490 K. The third phase of Ca₂CuO₃ was observed from the XRD of CCTO ceramics. From SEM, the grain size was decreased obviously with high valence Pr-ion (mixing valence of Pr³⁺ and Pr⁴⁺) substituting Ca²⁺. The room temperature dielectric constant of Pr-doped CCTO ceramics, sintered at 1323 K, was an order of magnitude lower than the pure CCTO ceramics due to the grain size decreasing and Schottky potential increasing. The dielectric spectra of Pr-doped CCTO were flatter than that of pure CCTO. The loss tangent of Pr-doped CCTO ceramics was less than 0.20 in 2 × 10²-10⁵ Hz region below 440 K. The complex impedance spectra of pure and Pr-doped CCTOs were fitted by ZView. From low to high frequency, three semicircles were observed corresponding to three different conducting regions: electrode interface, grain boundary and grain. By fitting the resistors R and capacitors C, the activation energies of grain boundary and electrode contact were calculated. All doped CCTOs showed higher activation energies of grain boundary and electrode than those of pure CCTO ceramics, which were concordant with the decreasing of dielectric constant after Pr₆O₁₁ doping.     

Improved high-Q microwave dielectric resonator using ZnO-doped La(Co1/2Ti1/2)O3 ceramics

The microwave dielectric properties and the microstructures of ZnO-doped La(Co_1/2Ti_1/2)O₃ ceramics prepared by conventional solid-state route have been studied. Doped with ZnO (up to 0.75 wt%) can effectively promote the densification of La(Co_1/2Ti_1/2)O₃ ceramics with low sintering temperature. At 1320 °C, La(Co_1/2Ti_1/2)O₃ ceramics with 0.75 wt% ZnO addition possesses a dielectric constant (_r) of 30.2, a Q × f value of 73,000 GHz (at 8 GHz) and a temperature coefficient of resonant frequency (τ_f) of −35 ppm/°C.     

Dielectric and microwave properties of ZrO2 doped CaO-SiO2-B2O3 ceramic matrix composites

The behavior of dielectric and microwave properties against sintering temperature has been carried out on CaO-SiO₂-B₂O₃ ceramic matrix composites with ZrO₂ addition. The results indicated that ZrO₂ addition was advantageous to improve the dielectric and microwave properties. X-ray diffraction (XRD) patterns show that the major crystalline β-CaSiO₃ and a little SiO₂ phase existed at the temperature ranging from 950 °C to 1050 °C. At 0.5 wt% ZrO₂, CaO-SiO₂-B₂O₃ ceramic matrix composites sintered at 1000 °C possess good dielectric properties: ?_r = 5.85, tan δ = 1.59 × 10⁻⁴ (1 MHz) and excellent microwave properties: ?_r = 5.52, Q · f = 28,487 GHz (11.11 GHz). The permittivity of Zr-doped CaO-SiO₂-B₂O₃ ceramic matrix composites exhibited very little temperature dependence, which was less than ±2% over the temperature range of −50 to 150 °C. Moreover, the ZrO₂-doped CaO-SiO₂-B₂O₃ ceramic matrix composites have low permittivity below 5.5 over a wide frequency range from 20 Hz to 1 MHz.     

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.     

Dielectric properties of low-temperature sintered Ba0.6Sr0.4TiO3 thick films prepared by reactive sintering method

Screen printed Ba_0.6Sr_0.4TiO₃ (BST6/4) thick films were fabricated by reactive sintering at a low temperature below 900 °C. The dielectric properties in radio frequency range were measured on samples of sandwich structure MIM capacitors by impedance analyzer, while that in microwave frequency range were measured on samples of thick films without top and bottom electrodes by split-post dielectric resonator method. The thick films exhibited a low permittivity, while at the same time, maintained a high tunability. The permittivity and dielectric loss at 1 MHz were 228.8 and 0.007, respectively. The corresponding values measured at 9.9 GHz were 82.24 and 0.109, respectively. The tunability was as high as 72.4% (150 kV/cm, 10 kHz). This method provides a simple and effective route to obtain thick films with great potential in applications in Low Temperature Co-fired Ceramic (LTCC) and microwave tunable devices.     

Impedance and modulus analysis of the (Na0.6Ag0.4)2PbP2O7 compound

The electrical properties of the (Na_0.6Ag_0.4)₂PbP₂O₇ compound were studied using the complex impedance spectroscopy in the temperature range (502-667 K). Grain interior, grain boundary and electrode-material interface contributions to the electrical response are identified by the analysis of complex plan diagrams. The imaginary part of the modulus at several temperatures shows a double relaxation peaks, furthermore suggesting the presence of grains and grain boundaries in the sample. An analysis of the dielectric constants ?′, ?″ and loss tangent tan(δ) with frequency shows a distribution of relaxation times. The dc conductivity of the material is thermally activated with an activation energy about 0.8 eV which is in the vicinity of the that obtained from tan(δ) (E = 0.7 eV) and modulus (E_m = 0.68 eV) studies.     

Improved dielectric and non-ohmic properties of Ca2Cu2Ti4O12 ceramics prepared by a polymer pyrolysis method

Non-ohmic and dielectric properties of Ca₂Cu₂Ti₄O₁₂ (CaCu₃Ti₄O₁₂/CaTiO₃ composite) ceramics prepared by a polymer pyrolysis method (PP-ceramic samples) are investigated. The PP-ceramics show a highly dense structure and improved non-ohmic and dielectric properties compared to the ceramics obtained by a solid state reaction method (SSR-ceramic samples). ?′ (tan δ) of the PP-ceramic samples is found to be higher (lower) than that of the SSR-ceramic samples. Interestingly, the PP-ceramic sintered at 1050 °C for 10 h exhibits the high ?′ of 2530 with weak frequency dependence below 1 MHz, the low tan δ less than 0.05 in the frequency range of 160 Hz-177 kHz, and the little temperature coefficient, i.e., |Δ?′| ≤ 15 % in the temperature range from −55 to 85 °C. These results indicate that the CaCu₃Ti₄O₁₂/CaTiO₃ composite system prepared by PP method is a promising high-?′ material for practical capacitor application.     

Study on magnetic and dielectric properties of YMnO3 ceramics

The magnetic and dielectric properties were investigated in the hexagonal YMnO₃ ceramics synthesized by sol-gel method. An antiferromagnetic order about 70 K and a weak ferromagnetic order at 5 K have been detected in YMnO₃ ceramics. In addition, we observed also the exchange-bias (EB) effect at low temperatures and it may originate from exchange coupling at the interface between ferromagnetic and antiferromagnetic orders for the co-existence of these two orders in some temperature region in hexagonal YMnO₃. Furthermore, the dielectric measurements showed two thermally activated relaxation behaviors following the Arrhenius law in 290-430 K and above 500 K in YMnO₃ ceramics and they can be explained as the dipolar effects associated with the charge carrier hopping between Mn²⁺ and Mn³⁺ and oxygen vacancy, respectively.     

On the mechanism of current-transport in Cu/CdS/SnO2/In-Ga structures

The structural and optical properties of CdS films deposited by evaporation were investigated. X-ray diffraction study showed that CdS films were polycrystalline in nature with zinc-blende structure and a strong (1 1 1) texture. The study has been made on the behavior of Cu/n-CdS thin film junction on SnO₂ coated glass substrate grown using thermal evaporation method. The forward bias current-voltage (I-V) characteristics of Cu/CdS/SnO₂/In-Ga structures have been investigated in the temperature range of 130-325 K. The semi-logarithmic lnI-V characteristics based on the Thermionic emission (TE) mechanism showed a decrease in the ideality factor (n) and an increase in the zero-bias barrier height (Φ_Bo) with the increasing temperature. The values of n and Φ_Bo change from 8.98 and 0.29 eV (at 130 K) to 3.42 and 0.72 eV (at 325 K), respectively. The conventional Richardson plot of the ln(I_o/T²) vs q/kT shows nonlinear behavior. The forward bias current I is found to be proportional to I_o(T)exp(AV), where A is the slope of ln(I)-V plot and almost independent of the applied bias voltage and temperature, and I_o(T) is relatively a weak function of temperature. These results indicate that the mechanism of charge transport in the SnO₂/CdS/Cu structure in the whole temperature range is performed by tunneling among interface states/traps or dislocations intersecting the space-charge region. In addition, voltage dependent values of resistance (R_i) were obtained from forward and reverse bias I-V characteristics by using Ohm's law for each temperature level.     

Multiferroic behavior in glass-crystal nanocomposites containing Te2NiMnO6

Nanocomposites containing nanocrystals of Te₂NiMnO₆ were synthesized by suitable heat treatment of a glass with composition 2 TeO₂·NiO·MnO (molar ratio). The crystallites had dimensions in the range 17-41 nm. X-ray diffraction data of the specimens were analyzed by using a TREOR computer programme. Lattice parameters extracted by this method indicated that the crystal symmetry was monoclinic. The nanocomposites exhibited weak ferromagnetism in the temperature range 2-300 K. They also showed ferroelectric hysteresis at room temperature with a remanent polarization of 0.015 μC/cm². The specimens showed a magnetodielectric (MD) behavior with dielectric constant increasing as a function of applied magnetic field. The MD parameter obtained in the present system was 0.55%.     

Epitaxial 0.65PbMg1/3Nb2/3O3-0.35PbTiO3 (PMN-PT) thin films grown on LaNiO3/CeO2/YSZ buffered Si substrates

Ferroelectric PMN-PT thin films with a thickness of 600 nm were epitaxially grown on buffered Si (0 0 1) substrates at a substrate temperature that ranged from 550 to 700 °C using pulsed laser deposition (PLD). LaNiO₃ (LNO) electrode thin films with a resistivity of ∼1900 μΩ cm were epitaxially grown on CeO₂/YSZ buffered Si (0 0 1) substrates. The PMN-PT thin films grown at 600 °C on LNO/CeO₂/YSZ/Si substrates had a pure perovskite and epitaxial structure. The PMN-PT films exhibited a high dielectric constant of about 1818 and a low dissipation factor of 0.04 at a frequency of 10 kHz. Polarization-electric-field (P-E) hysteresis characteristics, with a remnant polarization of 11.1 μC/cm² and a coercive field of 43 kV/cm, were obtained in the epitaxial PMN-PT films.     

Charge compensation, electrical and dielectric behavior of lanthanum doped CaCu3Ti4O12

Mechanism of charge compensation on lanthanum, (La³⁺) substitution on Ca site in calcium copper titanate (CaCu₃Ti₄O₁₂), and its effect on resulting electrical and dielectric properties has been studied in the present investigation. For this purpose samples were prepared according to two stoichiometries viz. La_xCa_(1−3x/2)Cu₃Ti₄O₁₂ (x ≤ 0.09) and La_xCa_(1−x)Cu₃Ti₄O₁₂ (x = 0.03) by solid state ceramic route. The former represents ionic compensation while the later is in accordance with electronic compensation. Nature of charge carriers is identified by measuring Seebeck coefficient which is found to be negative in the entire range of measurement. In order to understand the mechanism of conduction, ac conductivity is measured as a function of temperature and frequency. Space charge polarization is the dominant polarization mechanism phenomenon at low frequency and high temperature while orientation polarization dominates at low temperature and high frequency. Impedance analysis confirms the formation of internal barrier layers which is responsible for high dielectric constant in these samples.     

Mg-substituted ZnNb2O6-TiO2 composite ceramics for RF/microwaves ceramic capacitors

Microstructure and microwave dielectric properties of Mg-substituted ZnNb₂O₆-TiO₂ microwave ceramics were investigated. Mg acted as a grain refining reagent and columbite phase stabilization reagent. With an increasing Mg content, the amount of ixiolite (Zn, Mg) TiNb₂O₈ decreased, and the amount of (Zn_0.9Mg_0.1)_0.17Nb_0.33Ti_0.5O₂ and columbite increased. ZnO-Nb₂O₅-1.75TiO₂-5 mol.%MgO exhibited excellent dielectric properties (at 950 °C): ?_r = 35.6, Q × f = 16,000 GHz (at 5.6 GHz) and τ_f = −10 ppm/°C. The material was applied successfully to make RF/microwaves ceramic capacitor, whose self-resonance frequency was 19 GHz at low capacitance of 0.13 pF.     

Phase pure synthesis of BiFeO3 nanopowders using diverse precursor via co-precipitation method

Amorphous powder of BiFeO₃ (BFO) was synthesized at low-temperature (80 °C) by co-precipitation method. Optimal synthesis conditions for phase pure BFO were obtained. Powders were calcined in the temperature range from 400 to 600 °C for 1 h. Iso-statically pressed powder was sintered at 500 °C for 2 h. Differential scanning calorimetric thermo-gram guided for phase transition, crystallization and melting temperatures. X-ray diffraction confirmed the amorphous nature of as synthesized powder and phase formation of calcined powders. Calcination at temperature ≥400 °C resulted in nano crystalline powders with perovskite structure. Average crystallite size increased with the increase in calcination temperature. Scanning electron microscopic studies revealed dense granular microstructure of the sintered samples. The sintered samples exhibited high dc resistivity at room temperature which decreased with the increase in temperature. Dielectric constant, dielectric loss tangent and ac conductivity measurements were carried out in the frequency range (10 Hz to 2 MHz). The samples responded weak electric and magnetic polarization at room temperature with unsaturated and hysteresis free loops, respectively.     

Role of Al2O3 layer in oxidation resistance of Cu-Al dilute alloys pre-annealed in H2 atmospheres

Copper was alloyed with small amounts of Al (0.2, 0.5, 1.0 and 2.0 mass%) to improve the oxidation resistance. Copper (6 N) and the Cu-Al alloys were oxidized at 773-1173 K in 0.1 MPa oxygen atmosphere after hydrogen annealing at 873 K. Continuous very thin Al₂O₃ layers were formed on the surface of all Cu-Al dilute alloys during the hydrogen annealing. Oxidation resistance of Cu-Al alloys was improved especially for Cu-2.0Al at 773-973 K, while it decreases on increasing the oxidation temperature. Cu-Al alloys followed the parabolic rate law at 1173 K, but most of other cases do not at and below 1073 K. Oxidation resistance for Cu-Al alloys was found relevant to the maintenance of the thin Al₂O₃ layer at the Cu₂O/Cu-Al alloy interface.     

Elucidating the dielectric properties of Mg2SnO4 ceramics at microwave frequency

This study investigated the potential applications of microwave dielectric properties of Mg₂SnO₄ ceramics in mobile communication. Mg₂SnO₄ ceramics were prepared using a conventional solid-state method. The X-ray diffraction patterns of the Mg₂SnO₄ ceramics revealed no significant variation of phase with sintering temperature. A maximum density of 4.62 g/cm³, a dielectric constant (?_r) of 8.41, a quality factor (Q × f) of 55,100 GHz, and a temperature coefficient of resonant frequency (τ_f) of −62 ppm/ °C were obtained when Mg₂SnO₄ ceramics were sintered at 1550 °C for 4 h.     

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.     

A new temperature stable microwave dielectric ceramics: ZnTiNb2O8 sintered at low temperatures

The phases, microstructure and microwave dielectric properties of ZnTiNb₂O₈-xTiO₂ composite ceramics with different weight percentages of BaCu(B₂O₅) additive prepared by solid-state reaction method have been investigated using the X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy-dispersive spectroscopy (EDS). The results showed that the microwave dielectric properties were strongly dependent on densification, grain sizes and crystalline phases. The sintering temperature of ZnTiNb₂O₈ ceramics was reduced from 1250 °C to 950 °C by doping BaCu(B₂O₅) additive and the temperature coefficient of resonant frequency (τ_f) was adjusted from negative value of −52 ppm/°C to 0 ppm/°C by incorporating TiO₂. Addition of 2 wt% BaCu(B₂O₅) in ZnTiNb₂O₈-xTiO₂ (x = 0.8) ceramics sintered at 950 °C showed excellent dielectric properties of ?_r = 38.89, Q × f = 14,500 GHz (f = 4.715 GHz) and τ_f = 0 ppm/°C, which represented very promising candidates as LTCC dielectrics for LTCC applications.