Dielectric Properties of Bi4−x La x Ti3O12 (0 ≤ x ≤ 2) Ceramics

The dielectric properties of the Bi_4–x La _x Ti₃O₁₂ (0 x 2) ceramics were characterized and discussed together with the P-E relation (polarization vs. electric field). With increasing x, the P-E relation changed from normal ferroelectric hysteresis loops to pure linear relation, which indicated that La³⁺ substitution for Bi³⁺ in Bi₄Ti₃O₁₂ induced a phase transition from ferroelectric to paraelectric state at ambient temperature. Low loss dielectric ceramics with temperature stable dielectric constant were obtained for x > 1.2 in Bi_4–x La _x Ti₃O₁₂ at 1 MHz. And the loss increased in all the compositions when the ceramics were measured at microwave frequencies.     

Preparation and Properties of Bi4 − x Nd x Ti3O12 Thin Films by Chemical Solution Deposition

Neodymium-modified Bi₄Ti₃O₁₂, (Bi, Nd)₄Ti₃O₁₂ (BNT) ferroelectric thin films have been prepared on Pt/TiO_x/SiO₂/Si substrates using metal-organic precursor solutions by the chemical solution deposition method. The BNT precursor films crystallized into the Bi layered perovskite Bi₄Ti₃O₁₂ (BIT) as a single-phase above 600C. The synthesized BNT films revealed a random orientation having a strong 117 reflection, whereas non-substituted BIT thin films exhibited a random orientation with strong 00l diffractions. Among Bi_{4 – x}Nd_xTi₃O₁₂ [x = 0.0, 0.5, 0.75, 1.0] thin films, Bi_3.25Nd_0.75Ti₃O₁₂ thin films showed a well-saturated P-E hysteresis loop with the highest P_r (22 C/cm²) and a low E_c (69 kV/cm) at an applied voltage of 5 V. The Nd-substitution with the optimum amount for the Bi site in the BIT structure was effective not only for promoting the 117 preferred orientation but also for improving the microstructure and ferroelectric properties of the resultant films.     

Scaling Effect on the Dielectric Constant in Ba(Ti x Zr1−x )O3 Thin Films

Recent work on PZT and BST thin films reveal a thickness dependence of the dielectric constant for a film thickness below 100 nm. This effect is commonly attributed to an interfacial layer between the electrode and the dielectric film (dead layer). In this contribution we report on the influence of the film thickness on the dielectric constant of Ba(Ti_xZr_{1 – x})O₃ thin films with different Zr-contents (x = 0–30 at.%). The films were prepared by chemical solution deposition (CSD) with thickness between 30 and 350 nm.The electrical characterization was performed in a temperature range between 25 and 200C. Results were interpreted with respect to the formation of a serial dead layer capacitance.     

Synthesis and Ferroelectric Response of Bi 4−x Nd x Ti 3 O 12 Thin Films

Nd doped Bi 4 Ti 3 O 12 layered materials were synthesized using a solution chemistry route. Thin films were deposited by spin coating. Powder and thin film samples were characterized by x-ray diffraction and Raman spectroscopy. Ferroelectric response of Bi 4 m x Nd x Ti 3 O 12 thin film (x = 0.95), deposited on Pt substrate is reported.     

Temperature-Stable High-ε Dielectrics Ceramics Based on (1 − x) Ba5NdTi3Ta7O30/xBi4Ti3O12

Modification of Ba₅NdTi₃Ta₇O₃₀ dielectric ceramics was investigated through introducing Bi₄Ti₃O₁₂. With increasing of Bi₄Ti₃O₁₂ content, the dielectric constant increased, and the temperature coefficient of the dielectric constant changed from negative to positive. The small temperature coefficient ( < 50 ppm/°C) combined with high dielectric constant ( = 178) and low dielectric loss (tan = 0.007 at 1 MHz) was achieved in the composition x = 0.6.     

Raman Scattering Study of the Pb(Hf x Ti1−x )O3 Ceramics

Raman spectroscopy was used to study the long wavelength vibrations of tetragonal perovskite (space group P4mm) Pb(Hf_xTi_1–x)O₃ (PHT) (0.10 x 0.50) samples at room temperature and at 20 K. For x 0.40, Raman spectra collected from the PHT samples were very similar to the previous spectra collected from the PZT samples with the same value of x, except the mode at around 190 cm^–1, whose frequency was decreasing with increasing x in PHT ceramics. Correspondingly, the latter feature was taken as a sign of the mass effect (Hf versus Zr) while the similarity of the remaining parts of the Raman spectra was assumed to be due to the almost identical ionic radii difference between Ti⁴⁺ and Zr⁴⁺ and between Ti⁴⁺ and Hf⁴⁺ ionic radii. The behaviour of the mode at around 280 cm^–1 revealed that a phase transition occurred once x was changing from 0.40 to 0.50.     

Microwave Dielectric Properties of Ferroelectric Pb(Zr1 − x Ti x )O3 Thin Films Using Interdigital Capacitors

Ferroelectric Pb(Zr_{1 ? x} Ti _x )O₃ (PZT) films were deposited on (001) MgO single crystals using sol-gel method. Structural properties and surface morphologies of PZT films were investigated using an X-ray diffractometer and a scanning electron microscopy, respectively. The dielectric properties of PZT films were investigated with the dc bias field of 0–135 kV/cm using interdigitated capacitors (IDC) which were fabricated on PZT films using a thick metal layer by photolithography and etching process. The small signal dielectric properties of PZT films were calculated by a modified conformal mapping method with low and high frequency data, such as capacitance measured by an impedance gain/phase analyzer at 100 kHz and reflection coefficient (S-parameter) measured by a HP 8510C vector network analyzer at 1–20 GHz. The IDC on PZT films exhibited about 67% of capacitance change with an electric field of 135 kV/cm at 10 GHz. These PZT thin films can be applied to tunable microwave devices such as phase shifters, tunable resonators and tunable filters.     

Microstructural and Electrical Properties of (Ba x Sr 1 − x )Ti 1 + y O 3 + z Thin Films Prepared by RF Magnetron Sputtering

The electrical and microstructural properties of (Ba x Sr 1 m x )Ti 1+y O 3+z (BST) thin films prepared by RF magnetron sputtering were investigated as a function of deposition temperature over the range of 100 C to 650 C. Films deposited above approximately 350 C on Pt/TiO 2 /SiO 2 /Si substrates were polycrystalline with relative permittivites of 100 nm thick BST thin films varying from 100 at 350 C to 600 at 650 C. For deposition temperatures below approximately 350 C, the electrical properties were strongly influenced by the presence of a less crystalline BST layer. Films deposited at 250 C were comprised of a multilayer polycrystalline/less crystalline BST structure. The less crystalline BST layer strongly affected both measured dielectric permittivity and leakage properties. Leakage characteristics of Pt/BST(250C)/Pt capacitors exhibited a power law dependence on voltage or an exponential dependence on square root of the applied voltage depending on whether the top Pt electrode adjacent ot the polycrystalline BST layer was biased at a high or low electric potential, respectively. Mechanisms for the observed leakage behavior are discussed.     

Synthesis and Dielectric Characterization of Pyrochlore-Free Pb1−x Ba x (Zn1/3Nb2/3)O3 Ceramics

The dielectric properties and synthesis of pyrochlore-free lead zinc niobate ceramics with Ba substituting for Pb were investigated. Ba partial substitution for Pb was effective in stabilizing the perovskite structure in PZN ceramics, where the minimum amount of Ba substitution needed was about 20 mol%. The dielectric loss and the temperature coefficient of dielectric constant of PZN were reduced markedly with Ba substitution, while the dielectric constant was greater than 110. Good dielectric properties were obtained for the composition of Pb_0.3Ba_0.7(Zn_1/3Nb_2/3)O₃: = 133.5, tan = 0.0009, = –811 ppm/°C.     

Investigation of dielectric and relaxor ferroelectric properties in Ba(Zr x Ti1−x )O3 ceramics

Barium zirconate titanate Ba(Zr _x Ti_1?x )O₃ (BZT x?=?0.1, 0.15, 0.2, 0.25) ceramics doped with Nb₂O₅ have been prepared by a traditional solid phase reaction. The temperature dependence of dielectric permittivity has been investigated. The results show that the phase transition temperature T _c is depressed and the diffuse phase transition behavior is enhanced with increasing Zr content. The Cole–Cole plot has been discussed and the cause of the deviation has been analyzed. The temperature dependence of inverse dielectric constants was investigated. A modified Curie–Weiss law can be used to describe the diffuseness of a phase transition, and diffusion factor increases with the Zr content.     

Piezoelectric and Dielectric Properties of Pb(Zr x Ti1 − x )O3-Pb(Ni1/3Sb1/3Nb1/3)O3 Piezoelectric Ceramics

In this paper, piezoelectric and dielectric properties of 0.9PbZr_xTi_1–xO₃-0.1PbNi_1/3Sb_1/3Nb_1/3O₃ were studied as a function of Zr/Ti mole ratio(x) for application to piezoelectric actuator. Also, microstructure and crystalline phase are investigated by using SEM and XRD, respectively. As a results, the substitution of Sb5+ to B-site increases the piezoelectric and dielectric properties, and when Zr/Ti mole ratio is 49/51 and ternary mole ration is 0.1(0.9PbZr_0.49Ti_0.51O₃-0.1PbNi_1/3Sb_1/3Nb_1/3O₃), the corresponding composition were found belonging to the Morphotropic Phase Boundary region with electromechanical coupling coefficient(k_p), mechanical quality factor (Q_m), permittivity(_r) and piezoelectric strain constant(d₃₃) equaled to 63%, 360, 2000 and 470 pC/N, respectively. Sintering temperature was about 1150_C and Curie temperature was determined around 290_C.     

Ferroelectric Bi4Ti3O12 and Bi4−x La x Ti3O12 ceramics prepared by a new sol-gel route

Ceramics of bismuth titanate, Bi₄Ti₃O₁₂ (BIT) and the La-doped series, Bi_4?x La _x Ti₃O₁₂ (xBLT) with x?=?0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, and 0.75, have been synthesized by a new sol-gel process based on ethylene glycol. La-doping is found to reduce the temperature of the formation of pure Bi-layer-structured phase from 600 °C in BIT and low La-doped xBLT (x?=?0.1–0.3) to 500 °C in high La-doped xBLT (x?=?0.4–0.75). Increasing the La-content in the xBLT ceramics decreases the contribution of the space charge polarization to the apparent dielectric permittivity. The ceramics of xBLT prepared by this sol-gel route exhibit improved dielectric properties, with a higher room temperature dielectric constant and lower losses up to high temperatures.     

Improved Temperature Stability of Microwave Properties in Tunable Devices Using Substituted Ba 1− x Sr x TiO 3

An improvement in ferroelectric device technology has become possible through optimization of the properties of the ferroelectric materials used to make the devices. The improvements discussed herein impact true time delay line and phase shifter performance by enhancing control over dielectric constant and extending the temperature range of tunability and device operation. Figures of merit were obtained for substituted-Ba 1 m x Sr x TiO 3 materials which have lower, less varying dielectric constant and adequate, less varying tunability at 1 MHz over the mil spec ( m 50 °C to 100 °C) range. For the sample whose figure of merit varies the least, dielectric constant and losses at 20 GHz and room temperature are reported. Dielectric constant and losses at 1 kHz are discussed.     

Ferroelectric Characteristics of Bi 4−x La x Ti 3 O 12 Thin Films Crystallized at Low Temperetures

Recently, Bi 4 m x La x Ti 3 O 12 (BLT) has received much attention because it enables low crystallization temperature with a large remanent polarization. BLT films were prepared using a metal organic decomposition technique followed by a rapid thermal annealing (RTA) and a furnace annealing. The annealing of BLT was performed in the temperature range from 550 to 700C. In particular, BLT film annealed at 600C using the RTA tool and the furnace shows good ferroelectric characteristics. The BLT film annealed at 600C exhibits a large value of remanent polarization (22 w C/cm 2 at 250kV/cm), and a low leakage current density (7 2 10 m 7 A/cm 2 at 250kV/cm), a good endurance characteristics for up to 3.2 2 10 11 cycles at 250kV/cm at 85C. From an accelerated imprint test, the lifetime of hysteresis integrity is estimated to be over 10 years at 85C. In conclusion, BLT is the one of the promising material to achieve the high density FeRAMs.     

Microstructure dependence of microwave dielectric characteristics in Ba6-3x Sm8+2x Ti18O54 (x = 2/3) ceramics

Effects of microstructures on the microwave dielectric characteristics of Ba_6-3x Sm_8+2x Ti₁₈O₅₄ (x?=?2/3) ceramics were investigated by controlling the sintering process and the annealing condition. The dielectric constant was sensitive to the porosity in ceramics, but insensitive to the annealing process. Q f value varied with both the annealing atmosphere and the sintering temperature, which indicates the strong reliance of dielectric loss on defects and grain boundaries. τ _f value exhibited a complex dependence on the sintering temperature. The orientation of grains is responsible for the variation of τ _f .     

Synthesis of (Ba0.5Sr0.5)(Ti1 − x Zr x )O3 ceramics: Effect of Zr content on room temperature electrical properties

The phase formation behavior and room temperature dielectric properties of bulk perovskite solid solution composition (Ba_0.5Sr_0.5)(Ti_1 − x Zr _x )O₃ have been investigated. The samples with different Zr-content were prepared through solid state reaction. The XRD investigation showed that Zr⁺⁴ is systematically dissolved in Ba_0.5Sr_0.5TiO₃ lattice up to about 60 atm.% substitution, having cubic Pm3m structure. Eighty atom percent Zr substituted composition showed to contain a cubic phase similar to that of x = 0.6 composition and a tetragonal (I4/mcm) phase. That is the solid solution breaks around at 80 atm.% Zr substitutions. Ba_0.5Sr_0.5ZrO₃ was having orthorhombic Imma structure. Decrease in grain sizes were observed with increase in Zr content. The permittivity of the ceramics decreased with the increase in Zr substitution. The frequency dependency of dielectric loss in the frequency range 10 Hz to 10 MHz, were improved with Zr substitution in the ceramics. The room temperature ac and dc conductivity also decreased significantly with the increase in Zr-content.     

Chemical Vapor Deposition of Ru Bottom Electrode for Ferroelectric Bi4 − x La x Ti3O12 Capacitors

Ruthenium films formed by metalorganic chemical vapor deposition were investigated, taking account of the application to the bottom electrode of ferroelectric capacitors. Ruthenium films were deposited using a liquid-type source of Ru[EtCp]₂ in a cold-wall type reactor with infrared lamps. A smooth and flat Ru film was successfully formed on a SiO₂-covered Si substrate without a seed layer. As the deposition temperature increased to 400°C, the crystallinity of the Ru film improved and the film exhibited high c-axis orientation. After forming a Bi_{4 ? x} La _x Ti₃O₁₂ (BLT) film by a sol-gel technique, a Pt/BLT/Ru capacitor was fabricated on the Ru film. Good hysteresis loops with 2P _r = 20 μC/cm² and 2V _c = 3.4 V were successfully obtained and the ferroelectric property did not depend on the deposition temperature of Ru in the temperature range from 325°C to 400°C. On the contrary, the leakage current density was significantly suppressed down to 1/100 as the deposition temperature of Ru increased from 325°C to 400°C.     

Low-temperature sintering and dielectric properties of the Bi(Nb1−x Ta x )O4 system

Low-temperature sintering and dielectric properties of the Bi(Nb_1?x Ta _x )O₄ (x?=?0.1, 0.3, and 0.5) system was investigated as a function of the zinc borosilicate (ZBS) glass content with a view to applying this system to LTCC technology. The addition of 7 wt% ZBS glass ensured a successful sintering below 900°C. The complete solid solution of Bi(Nb, Ta)O₄ with an orthorhombic structure was formed and the high temperature form of Bi(Nb, Ta)O₄ with a triclinic structure was not observed. The second phase of Bi₂SiO₅ was observed for all compositions. The non-relative liquid phase sintering (NLPS) occurred and the one-stage sintering was conducted. The Q?×?f values were improved by the addition of Ta. Bi(Nb_0.7Ta_0.3)O₄ with 7 wt% ZBS glass sintered at 900°C demonstrated 35.8 in the dielectric constant (? _r), 2,200 GHz in the quality factor (Q?×?f ₀), and ?48 ppm/°C in the temperature coefficient of resonant frequency (τ _f).     

Evaluation of Chemical Solution Deposited Ba x Sr 1−x TiO 3 Thin Films on LaAlO 3 in Tunable Microwave Devices

Epitaxial Ba x Sr 1 m x TiO 3 (BST) films grown on LaAlO 3 by several deposition methods have been tested in coupled microstrip phase shifters (CMPS) at frequencies from 10 to 24 GHz. To date the best performance for the devices has been achieved using Pulsed Laser Deposition (PLD). However, recently chemical solution deposition (CSD) methods such as sol-gel and Metal-Organic Chemical Liquid Deposition (MOCLD) have shown advances in fabricating BST films for tunable microwave applications. CSD processes promise improvements in cost, speed and area covered during BST film deposition. This paper compares over 35 BST films used in identical CMPS circuits. In this study, the highest measured figures of merit of phase shift per dB of loss for PLD, MOCLD and sol-gel CMPS are 49, 47 and 41°/dB respectively. While other phase shifter designs using BST films have surpassed these values, these data base of identical circuits allows us to compare the BST films. X-ray diffraction characterization for many of the BST films is also given.     

Structure and microwave dielectric properties of Sm(2−x)/3Li x TiO3

The structural evolution, and microwave dielectric properties of ceramics (x = 0.0 ≤ x ≤ 0.5) were investigated in this work. X-ray diffraction (XRD) results show that samples with x > 0.3 exhibit a single perovskite phase. Impurity phases of Sm₂Ti₂O₇ and TiO₂ appear and their amount increases with the decrease of x when x ≤ 0.3. TEM observation indicates that the A-site is ordered in x = 0.5, but not in x = 0.3). The dielectric constant decreases with the increase of x for 0.1 ≤ x ≤ 0.4 and then increases with further increase in x up to x = 0.5. The Q×f value decreases with the decrease of x due to the increased occurrence of Sm₂T₂O₇ secondary phase, defects and twinning boundaries. The temperature coefficient of resonant frequency is negative and its absolute value decreases greatly with the decrease of x value.