Planar and Parallel Dielectric Properties of Compositionally Graded (Ba,Sr)TiO3 Thin Films for Tunable Microwave Applications

Compositionally graded (Ba_x,Sr_{1 ? x})TiO₃ [BST] ferroelectric thin films have been received much attention in graded ferroelectric devices due to their unique properties, such as large pyroelectric coefficients, large polarization offset and small temperature coefficient of dielectric constant for microwave tunable devices. Compositionally graded BST thin films were deposited epitaxially on LaAlO₃ [LAO] and Nb-doped SrTiO₃ [STO:Nb] substrates by pulsed laser deposition. The planar and parallel dielectric properties of compositionally graded BST epitaxial thin films ware investigated in the frequency ranges of 100 Hz ～ 1 MHz as a function of the direction of the composition gradient with respect to the substrate at room temperature. The dielectric properties of the graded BST films depended strongly on the direction of the composition gradient with respect to the substrate. The graded ST → BT films grown on LAO and STO:Nb substrates exhibited a excellent dielectric properties than the graded BT → ST films.     

Lateral Epitaxial Growth of Ba0.6Sr0.4TiO3 Thin Films

We report a novel growth technique for epitaxial thin films by combination of selective heteroepitaxial growth and lateral homoepitaxial growth. Ba_0.6Sr_0.4TiO₃ (BST) thin films were deposited on the substrates having patterned SiO_x layers at 450°C using pulsed laser deposition. Post annealing was carried out thereafter for lateral epitaxial growth. The difference in the crystallization temperature of BST thin film on the amorphous masking layers and lattice-matched single crystalline substrate enables selective nucleation and heteroepitaxial growth from the regions of single crystalline substrates during the film deposition. Lateral homoepitaxial growth is expected from the crystallized BST thin film toward the amorphous BST on SiO_x during the post annealing process. In this paper, a study on the difference in nucleation and growth behavior of BST thin films on the amorphous masking layers and lattice-matched single crystal substrates is presented.     

AC and DC conductivity studies in pulsed laser ablated (Ba,Sr)TiO3 thin films

Abstract

A comparison of the ac conductivity of laser ablated (Ba, Sr)TiO₃ thin films was made for films grown at different substrate temperatures. The ac conductivity was studied as a function of frequency and ambient temperature ranging from room temperature to 460°C. Conductivity results from ac and dc measurements were compared in their an respective Arrhenius plots revealing interesting coincidences. The value of the activation energies computed from the Arrhenius plot of à _ac with 1000/T ranged from 0.97 to 1.3 eV in the high temperature region to 0.36 to 0.54 eV in the low temperature region for different samples. The activation energies obtained from pure dc measurement for fields greater than 100 kV/cm across the samples were in the range of 1.06 to 1.32 eV for different samples. The similarity in results suggests a common origin in the de conduction process in the concerned temperature range and was attributed to ionic conduction resulting from oxygen vacancy motion which has been observed to be significant at high temperatures and high fields. For high temperature grown samples the value of activation energy computed from the Arrhenius plots was comparatively less than those grown at lower substrate temperatures. The difference was attributed to the microstructure and the effect of grain boundaries on the motion of oxygen vacancies leading to the conduction process.     

Magnetron sputter-deposited multilayer (BaxSr1x)Ti1+yO3+z thin films for passive and active devices

Abstract

High permittivity (Ba_xSr_1?x)Ti_1+yO_3+z(BST) thin films are being investigated for integration into charge storage dielectrics and electric-field tunable elements for high frequency devices. For the latter application, it is desirable to have BST capacitors with high tunability and low losses. Therefore, we investigated the use of multilayer BST thin films consisting of very low dielectric loss BST/electrode interfacial layers ((Ba+Sr)/Ti = 0.73) sandwiching a high tunability, high permittivity primary BST layer ((Ba+Sr)/Ti = 0.9). BST capacitors with multiple layers of controlled composition can be effectively produced insitu by magnetron sputter deposition, using a single stoichiometric target and controlling the layer composition by changing the total process gas (Ar+O<₂) pressure. The layered BST film capacitors exhibit simultaneous low loss (tan Δ = 0.005), high tunability (76%), high charge storage energy density (34 J/cm³), low leakage, and high dielectric breakdown (>2.8 MV/cm).     

Contribution of dielectric and metallic losses in RF/microwave tunable varactors using (Ba,Sr)TiO3 thin films

Abstract

Recently, there has been significant interest in use of (Ba,Sr)TiO₃ (BST) thin films for tunable high frequency (RF and microwave) components. In a previous work we have shown that BST thin films grown by metalorganic chemical vapor deposition (MOCVD) exhibit films very low losses (as low as 0.003–0.004) and tunabilities over 50% at low operation voltages.

In order to integrate BST thin films in tunable devices, the objectives of this work are : (i) study the effect of bottom and top electrode on the performance of thin film based capacitors, (ii) correlate low frequency (10 kHz) and high frequency (45 MHz - 1 GHz) measurements, (iii) separate the contribution of dielectric losses and metallic losses at both low and high frequency and finally (iv) show the potential usefulness of series capacitors structures.     

The microwave properties of Li doped 0.7(Ba,Sr)TiO3-0.3MgO thick film interdigital capacitors on the alumina substrates

The crystalline and electrical properties of Li doped 0.7(Ba,Sr)TiO₃-0.3MgO thick film interdigital capacitors have been investigated. Screen printing method was employed to fabricate Li doped 0.7(Ba,Sr)TiO₃-0.3MgO thick films on the alumina substrates. (Ba,Sr)TiO₃ materials have high dielectric permittivity (>500 @ 1 MHz) and low loss tangent (0.01 @ 1 MHz) in the epitaxial thin film form. To improve dielectric properties and reduce sintering temperature, MgO and Li were added, respectively. 10 μm thick films were screen printed on the alumina substrates and then interdigital capacitors with seven fingers of 200 μm finger gap were patterned with Ag electrode. Current-voltage characteristics were analyzed with elevated temperature range. Up to 50 °C, the thick films showed positive temperature coefficient of resistivity (dρ/dT) of 6.11 × 10⁸ Ω cm/°C, then film showed negative temperature coefficient of resistivity (dρ/dT) of −1.74 × 10⁸ Ω cm/°C. From the microwave measurement, the relative dielectric permittivity of Li doped 0.7(Ba,Sr)TiO₃-0.3MgO thick films interdigital capacitors were between 313 at 1 GHz and 265 at 7 GHz.     

MOCVD growth of barium-strontium titanate films using newly developed barium and strontium precursors

We report on metal-organic chemical vapor deposition (MOCVD) of the Ba_xSr_1 − xTiO₃ (BST) films (with x ≈ 0.5) on SrTiO₃ substrates. This research comprises the development of new chemical precursors, modification of the MOCVD apparatus towards stoichiometric oxide growth and undesirable phase suppression, as well as establishing optimum growth conditions. The grown BST films were characterized by the set of experimental techniques, including high-resolution X-ray diffraction (HRXRD) and high-resolution scanning electron microscopy. The newly synthesized organo-metallic precursors exhibit better properties than the available precursors and, in particular, show low melting points of about 80 °C. By using these precursors, we succeeded to grow sub-micron thick BST films of high crystalline quality. Optimum growth temperature was found to be 740 °C. The symmetric and asymmetric HRXRD profiles, as well as wide-angle X-ray diffraction scans, taken from the films grown under optimal conditions, reveal epitaxial orientation relations between the film and the substrate.     

Pyroelectric properties of BST/PLT composite thick films with addition of xPbO–(1 − x)B2O3 glass

The Ba_xSr_1−xTiO₃ (BST)/Pb_1−xLa_xTiO₃ (PLT) composite thick films (20 μm) with 12 mol% amount of xPbO–(1 − x)B₂O₃ glass additives (x = 0.2, 0.35, 0.5, 0.65 and 0.8) have been prepared by screen-printing the paste onto the alumina substrates with silver bottom electrode. X-ray diffraction (XRD), scanning electron microscope (SEM) and an impedance analyzer and an electrometer were used to analyze the phase structures, morphologies and dielectric and pyroelectric properties of the composite thick films, respectively. The wetting and infiltration of the liquid phase on the particles results in the densification of the composite thick films sintered at 750 °C. Nice porous structure formed in the composite thick films with xPbO–(1 − x)B₂O₃ glass as the PbO content (x) is 0.5 ≥ x ≥ 0.35, while dense structure formed in these thick films as the PbO content (x) is 0.8 ≥ x ≥ 0.65. The volatilization of the PbO in PLT and the interdiffusion between the PLT and the glass lead to the reduction of the c-axis of the PLT phase. The operating temperature range of our composite thick films is 0–200 °C. At room temperature (20 °C), the BST/PLT composite thick films with 0.35PbO–0.65B₂O₃ glass additives provided low heat capacity and good pyroelectric figure-of-merit because of their porous structure. The pyroelectric coefficient and figure-of-merit F_D are 364 μC/(m² K) and 14.3 μPa^−1/2, respectively. These good pyroelectric properties as well as being able to produce low-cost devices make this kind of thick films a promising candidate for high-performance pyroelectric applications.     

纳米晶钛酸锶钡(Ba0.5Sr0.5TiO3)粉体的微波水热合成

采用微波水热法合成了纳米晶钛酸锶钡(Ba0.5Sr0.5TiO3)粉体,通过XRD、TEM、SEM等分析手段表征粉体,研究了微波水热合成反应温度、时间和前驱物浓度对反应产物形貌、粒度的影响,获得了制备纳米晶钛酸锶钡粉体的最优工艺参数.实验结果表明:在微波水热反应温度为195℃、反应时间20～30min、前驱物浓度为0.16mol/L时获得的粉体粒径小而且均匀,粉体平均粒度为60nm.