Relaxor Behavior of (Sr0.8Ba0.2)TiO3 Ceramic Solid Solution Doped with Bismuth

The dielectric properties of (Sr_0.8Ba_0.2)_1-1.5xBi_xTiO₃ ceramics in the range 0 x 0.18 are investigated. A ferroelectric relaxor behavior is observed. The degree of the diffuseness and the relaxation of the phase transition increases as the Bi content increases. A random electric field is suggested to be responsible for the relaxor behavior observations. The dependence of the diffuseness on the grain size is presented.     

Effect of raw material on properties of Ba0.55Sr0.45TiO3/MgO composites

The effect of raw material on properties of Ba_0.55Sr_0.45TiO₃/MgO composites was studied. The Ba_0.55Sr_0.45TiO₃ was prepared by BaCO₃, SrCO₃, TiO₂ and BaTiO₃, SrTiO₃. The MgO was prepared by heavy magnesium oxide, light magnesium oxide and basic magnesium carbonate, respectively. The crystalline phases of all ceramics were the same. Whereas, the grain size, lattice parameters, microwave dielectric properties and tunability of the samples were different. Overall, the Ba_0.55Sr_0.45TiO₃/MgO composites, in which BST were prepared from BaCO₃, SrCO₃ and TiO₂, and MgO was prepared by heavy magnesium oxide, exhibited excellent properties of ?_r = 141.55, Q × f = 905 GHz and n_r = 7.16% (E = 3 kV/mm).     

MOCVD of (Ba,Sr)TiO3: Nucleation and Growth

(Ba_0.7Sr_0.3)TiO₃ and SrTiO₃ thin films were deposited on Pt electrodes in a planetary multi-wafer MOCVD reactor. The nucleation behavior and the size of the stable nuclei were investigated by different SPM techniques. Characteristic differences were observed for different deposition temperatures, i.e. a homogeneous nucleation of small BST grains on the larger Pt grains at 565°C and a dominating nucleation at the grain boundaries at 655°C. The micro structural evolution after further film growth was investigated by HRTEM and revealed randomly oriented grains (typical inplane size 10–20 nm) with a high density of twins at 565°C and (100)-oriented defect free grains of only slightly increased size at 655°C. For SrTiO₃ the inplane grain size was increased, however, the (100) texture was less perfect. As the electrical properties like permittivity and also leakage current depend on film thickness the final discussions of the electrical properties are based on thickness series (5 nm–100 nm films) and evaluated within the phenomenological dead layer model.     

Multilayer Ceramic Capacitors with Thin (Ba,Sr)TiO3 Layers by MOCVD

Barium strontium titanate ((Ba,Sr)TiO₃; BST) thin films were prepared on platinum-coated MgO substrates at 650°C by metalorganic chemical vapor deposition (MOCVD). Perovskite single phased BST thin films were obtained. Dielectric constant at 1 kHz–100 mV was 1000. Multilayer ceramic capacitor with twelve BST dielectric layers of 0.26 m thick was formed on the MgO substrate. Capacitance and dissipation factor (tan) at 1 kHz–100 mV were 32 nF and 1.5% respectively. Capacitance per unit volume of 33 F/mm³ provided 10 to 20 times larger volumetric efficiency than the conventional multilayer ceramic capacitors. Temperature coefficient of capacitance was –4000 ppm/°C. The leakage current at 1 V was 2.3×10^-9 A that yielded an acceptable CR product of 12.8 M-F. MOCVD was proposed as one of the promising manufacturing technologies for multilayer ceramic capacitors of high performance with sub-micron thick dielectric layers.     

Electrical Properties of the Titanium Modified SBN Ceramic System

The electrical properties of the Sr_0.3Ba_0.7Nb₂O₆ system modified with different concentrations of titanium, following the general formula Sr_0.3Ba_0.7Nb_2–y Ti _y O_6–y/2 for charge compensation, are studied. The investigation is carried out in samples prepared by the conventional ceramic method. The X-ray diffraction analysis shows tetragonal tungsten bronze monophasic compounds in all cases. Dielectric measurements show a typical ferroelectric behavior with diffuse phase transition, where the transition temperature and the maximum permittivity decrease with increasing titanium content. The remanent polarization is obtained from hysteresis measurements in the ferroelectric region, while at high temperatures, two processes (a conductive and a ferroelectric process) are overlapping. The diffuse character of the ferroelectric-paraelectric phase transition is also studied and the diffusivity coefficient calculated in all cases.     

The resistance degradation of (Ba0.5Sr0.5)TiO3 thin films

Abstract

The leakage current and dielectric properties of (Ba_0.5Sr_0.5)TiO₃(BST) thin films prepared by pulsed laser deposition (PLD) were investigated. It was found that leakage currents for positive bias voltage were higher than that for negative bias voltage, which was attributed to the lattice mismatch between bottom Pt electrode and BST thin film. The time-dependent breakdown process under positive voltage was observed, which was interpreted as the increase of the internal electric field in the film near the bottom electrode. However, the internal electric field can be decreased and eventually recovered by applying negative bias voltage. It was found that internal electric field near the interface can influence the capacitance of the BST thin film capacitor. An explanation for the thickness effect of BST thin films was given.     

Phase Transformation and Temperature Dependence of Relative Permittivity for A-site Substituted Sr(Y0.5Ta0.5)O3Perovskites

A-site cation substitution with Ba²⁺ or Ca²⁺ ions was made for the ordered complex perovskite Sr(Y_0.5Ta_0.5)O₃ to correlate the structure evolution and the change in the temperature coefficient of relative permittivity (TC_r) with the cation substitution. The crystal symmetry of the solid solutions at room temperature changed as monoclinic rhombohedral cubic with the corresponding A-site cation species of Ca²⁺ Sr²⁺ Ba²⁺. On heating, the rhombohedral phase of Sr(Y_0.5Ta_0.5)O₃ was firstly transformed to the cubic phase with a lower symmetry (F43m or F432) at 1000°C and further to the ideal cubic phase (Fm3m) at 1300°C. The similar phase transformation behavior at elevated temperatures was observed for each of the Ba²⁺-substituted perovskites, both the phase transformation temperatures being lowered with increasing Ba²⁺ content. TC_r of the ordered perovskites monotonously increased over the temperature range where the phase transformation regions from monoclinic to rhombohedral or from rhombohedral to cubic (F43m or F432) occurred. On the other hand, a subtle symmetry change in the cubic phase from F43m (F432) to Fm3m caused a remarkable change in the TC_r from positive to negative at the transformation temperature. These results suggested that the positive TC_r is essentially correlated to the relaxation of the tilting of the BO₆ octahedra in the perovskite structure on heating.     

Ceramics Materials Based on (Ba, Sr)TiO3 Solid Solutions for Tunable Microwave Devices

Structure and electrical properties at radio frequencies as well as within the 3.5–35 GHz frequency range have been investigated for ceramic samples of the (1–y)(Ba_xSr_{1 – x})TiO₃ · yMgO (BSM) system where x = 0.4–0.6; y = 0.15–0.30. For the compositions studied the bulk ferroelectrics were synthesized with the dielectric constant of 400–600 and high tunability coefficient. We indicated that the quality factor of the samples was in the range of 100–1000 within the frequency band of 3.5–35 GHz. The phase correlations and unit cell constants of the perovskite phase of the BSM samples were studied. The low loss factor and high tunability of the bulk material allowed us using the BSM ferroelectric ceramic layer for tunable accelerating structures of the Argonne Dielectric Wakefield Accelerator and for high power switches design and development for the future linear colliders.     

Growth,Microwave Properties and Microstructure of Ba0.05Sr0.95TiO3 Thin Films

Charged defects were found to have a significant influence over the microwave properties of Ba_0.05Sr_0.95TiO₃ thin films.     

Tunability and leakage currents of (Ba,Sr)TiO3 ferroelectric ceramics with various additives

The Ba_xSr_{1 − x} TiO₃ ferroelectric ceramics with magnesium (BSM) and neodymium (BSN) additives were studied. Measurements were made of tunability, dielectric losses (tan δ), leakage currents, the correlations between current-voltage I(U) and capacitance-voltage C(U) characteristics. I(U) characteristics of high quality BSM ceramics have four regions: Ohmic, where the conductivity is linear; the horizontal region (or negative differential resistivity); the exponential dependence; and the vertical current enhancement. These BSM samples (∼20% Mg additives) were distinguished by highest breakdown strength (more than 1000 V), low tan δ (less than 10^{− 3} at 1 MHz) and high tunability (up to 10% at E _max∼2 V/μm).     

Slow Dielectric Relaxation in Pb(Zr,Ti)O3 and (Ba,Sr)TiO3 Ferroelectric Thin Films

An impedance analysis of Ni/Pb(Zr,Ti)O₃/Pt thin-film structures based on measurements at the frequencies from 100 Hz to 100 MHz, along with the data of Grazing Angles XRD, TEM and photo-electric study, is used to obtain electronic structure of the PZT thin films deposited by sol-gel method on silicone substrates. Both slow capacitance relaxation and charging/discharging currents versus time under step-voltage excitation have been studied in (Ba,Sr)TiO₃ thin films between SrRuO₃ electrodes.     

Processing and properties of nanocrystalline Pb(Sc0.5Ta0.5)O3, Pb(Sc0.5nb0.5)O3 and Pb(Mg1/3Nb2/3)O3 films produced by RF-sputtering from ceramic targets

Abstract

Nanocrystalline thin films of different relaxor materials, namely Pb(Sc_0.5Ta_0.5)O₃ (PST), Pb(Sc_0.5Nb_0.5)O₃(PSN), Pb(Mg_1/3Nb_2/3)O₃(PMN) have been produced by RF-sputtering to investigate whether it will affect their dielectric properties if their grain size is reduced to the dimensions known from their nanodomains. The XRD shows that the amorphous film crystallizes in pyrochlore structure at lower temperatures and short times. Annealing at higher temperatures and far longer time intervals leads to an increasing amount of perovskite phase with a grain size in the nanometer range. These results including dielectric measurements will be presented and discussed.     

Iridium thin film as a bottom electrode for high dielectric (Ba,Sr)TiO3 capacitors

Abstract

We propose Ir thin films as new electrode materials for high dielectric BST capacitors. Ir was found to be superior to Pt in a number of aspects such as resistivity, adhesion and surface roughness. The Pt/BST/Ir/SiO₂/Si capacitors showed leakage currents as low as Pt/BST/Pt/SiO₂/Si ones, but higher capacitance resulted. For endurance properties with +5V unipolar pulse trains, the dielectric constant of BST films on Ir decreased by only 10% below its initial value after switching of 10⁹ cycles while that on Pt degraded by 30% after 10⁸ cycles. Ir bottom electrode effects on BST film properties were well explained by the formation of IrO₂ phases on the surface of Ir electrodes.     

Optimum Reflection-Type Phase Shifter Using (Ba,Sr)TiO3 Thin Film

In this paper, in order to obtain a large differential phase shift with a little change in applied voltage, a ferroelectric reflective load circuit has been designed on top of barium strontium titanate (Ba,Sr)TiO₃ [BST] thin film. The design of the ferroelectric reflection-type phase shifter is based on a reflection theory of terminating circuit, which has a reflection-type analogue phase shifter with two ports terminated in symmetric phase-controllable reflective networks. To achieve large amounts of phase shift in low bias-voltage range, the effects of change of capacitance and transmission line connected with two coupled ports of a 3-dB 90° branch-line hybrid coupler have been investigated. A large phase shift with a small capacitance change in the parallel terminating circuit has been demonstrated in the paper.     

Microwave frequency conversion in coplanar waveguide on bilayered substrate with (Ba,Sr)TiO3 film

Abstract

Experimental and simulated spectra of microwave (30GHz) signal at the output of the coplanar waveguide (CPW) based on Ba_xSr_1-xTiO₃ film are presented and discussed. The modulation of Ba_xSr_1-xTiO₃ film dielectric constant by the application of high frequency (f ≈ 20MHz) control signal results in the generation of side frequency components in the output signal spectrum. The analysis of experimental data is performed on the basis of considering the CPW section with tunable effective dielectric constant as a phase modulator     

Distributed phase shifters using (Ba,Sr)TiO3 thin films on sapphire and glass substrates

Abstract

Sol-gel solutions were synthesized by using various alkoxides of polyhydric alcohol, carboxylate and stabilizer. Stability of modified sol-gel solution was good enough to keep its properties after at least three months although that of ordinary sol-gel solution is not good.

SBT films were fabricated on Pt(200nm)/Ti(20nm)SiO₂(500nm)/Si substrate at under 700°C by using modified sol-gel solution. Range of drying temperature was 200 to 400°C and that of RTA was 550 to 700°C. At high drying temperature, decrease of crystallinity for SBT films was observed accompanied by nucleation of Sr carbonate. On the other hand, SBT film dried at under 250°C and crystallized at 700°C shows high crystallinity of layer perovskite.

SBT film derived from conventional sol-gel solution used to show strong crystal orientation of c-axis. In case of modified sol-gel solution, RTA temperature and amount of added stabilizer influenced crystal orientation of film. So it was possible that to control crystal orientation of SBT films by adjust RTA condition and amount of stabilizer. Stability of sol-gel solution and property of SBT films were influenced by component of solvent, electric properties of SBT films especially I-V property were improved.

Using low temperature deposition process at 650°C, SBT films derived from modified sol-gel solution show superior ferroelectric properties to SBT thin films derived from conventional MOD solution.     

Microwave Performance of Distributed Analog Phase Shifter Using Ferroelectric (Ba,Sr)TiO3 Thin Films

This work presents the design, fabrication and microwave performance of distributed analog phase shifter (DAPS) fabricated on (Ba,Sr)TiO₃ (BST) thin films for X-band applications. Ferroelectric BST thin films were deposited on MgO substrates by pulsed laser deposition. The DAPS consists of high impedance coplanar waveguide (CPW) and periodically loaded tunable BST interdigitated capacitors (IDC). In order to reduce the insertion loss of DAPS and to remove the alteration of unloaded CPW properties according to an applied dc bias voltage, BST layer under transmission lines were removed by photolithography and RF-ion milling. The measured results are in good agreement with the simulated results at the frequencies of interest. The measured differential phase shift based on BST thin films was 24° and the insertion loss decreased from ?1.1 dB to ?0.7 dB with increasing the bias voltage from 0 to 40 V at 10 GHz.     

Dielectric and Mechanical Losses in (Ba,Sr)TiO3 Systems

In the application of tuneable microwave devices of ferroelectric (BaSr)TiO₃ systems the two critical parameters needed for optimal device performance are high tunability and low dielectric loss. The dielectric loss of the materials is strongly dependent on microstructure. This paper is concerned with an investigation of the variation in the dielectric and mechanical losses in Ba _x Sr_{1 – x} TiO₃ systems (x = 0.5, 0.6, 0.7 and 1.0) with microstructure (grain sizes from 1 m to 50 m). The magnitude of the loss peak and sharpness of the anomaly in the dielectric constant/elastic modulus observed for the phase transitions in Ba _x Sr_{1 – x} TiO₃, depend not only on the composition and but also on the grain size. A relaxation peak has been observed in large grain material, which is indication of interactions between different configurations of domain walls and the diffusion of oxygen vacancies in the domains.     

Effect of excess TiO2 on the phase evolution and densification of sol-gel derived (Ba,Sr)TiO3 powders

Nanoscaled (Ba_2/3Sr_1/3)Ti_{1 + x} O₃ powders have been prepared by sol-gel technique. Their phase evolution and densification behaviors have been studied by differential thermal analysis (DTA) and high temperature dilatometer, respectively. It is found the addition of 2 mol%-excess amount of TiO₂ lowers the activation energy required for the formation of the perovskite phase by about 130 kJ/mol and thus lowers the crystallization temperature of BST powders. However, the excess amount of TiO₂ makes the nano-powder difficult to sinter. Transmission electron microscopy reveals that a metastable nano-porous layer has formed on the surface of TiO₂-excess nanopowder and this may account for the slow densification rate.     

Measurement of Microwave Dielectric Properties of (Sr,Ba)Nb2O6 Thin Films

(001) oriented (Sr,Ba)Nb₂O₆ (SBN) thin films were deposited on MgO (001) single crystal substrates by the pulsed laser deposition method. Structural properties of SBN films were investigated using X-ray diffractometer. The microwave dielectric properties of SBN films were examined by calculating the scattering parameter obtained using a HP 8510C vector network analyzer with the frequency range 0.5–20 GHz at room temperature under the dc bias field of 0–80 kV/cm for interdigital capacitors (IDT) and coplanar waveguide (CPW) device based on SBN/MgO layer structure. Thick metal electrode patterns were fabricated by dc sputtering deposition, photolithography and etching process. The IDT device based on (001) oriented SBN films exhibited about 40% capacitance tunability with an electric field change of 80 kV/cm at room temperature, and the dielectric quality factor was about 20 at 12 GHz with no dc bias.