In-Plane Polarized 0.7Pb(Mg1/3Nb2/3)O3–0.3PbTiO3 Thin Films

Ferroelectric 0.7Pb(Mg_1/3Nb_2/3)O₃–0.3PbTiO₃ (PMN-PT) thin films were deposited on ZrO₂/SiO₂/silicon substrates using a chemical-solution-deposition method. Using a thin PZT film as a seed layer for the PMN-PT films, phase-pure perovskite PMN-PT could be obtained via rapid thermal annealing at 750°C for 60 s. The electrical properties of in-plane polarized thin films were characterized using interdigitated electrode arrays on the film surface. Ferroelectric hysteresis loops are observed with much larger remanent polarizations (∼24 μC/cm²) than for through-the-thickness polarized PMN-PT thin films (10–12 μC/cm²) deposited on Pt/Ti/Si substrates. For a finger spacing of 20 μm, the piezoelectric voltage sensitivity of in–plane polarized PMN-PT thin films was ∼20 times higher than that of through-the-thickness polarized PMN-PT thin films.     

Flexible Dielectric Bi1.5Zn1.0Nb1.5O7 Thin Films on a Cu-Polyimide Foil

Flexible thin films of Bi_1.5Zn_1.0Nb_1.5O₇ (BZN) were deposited on a Cu/polyimide (PI) foil by aerosol deposition at room temperature. The BZN film thickness was in the range of 1.2–17.9 μm. Highly dense and nanocrystalline films were obtained without any heat treatment. The dielectric constant and loss of the film at 100 kHz were over 150 and 0.04, respectively. Furthermore, the as-deposited film showed markedly low leakage current densities of <10⁻⁹ A/cm² at 3.0 V. These reasonably high dielectric properties were due to the nanocrystallinity of the films. The results confirm the significant potential of the BZN films as passive components in flexible printed circuit board applications.     

Sol—Gel Fabrication of Pb(Zr0.52 Ti0.48)O3 Thin Films Using Lead Acetylacetonate as the Lead Source

Lead zirconium titanate (PZT) thin films of the morphotropic phase boundary composition [Pb(Zr_0.52Ti_0.43)O₃] were deposited on platinum-coated silicon by a modified sol-gel process using lead acetylacetonate as the lead source. The precursor solution for spin coating was prepared from lead acetylacetonate, zirconium n -butoxide, and titanium isopropoxide. The use of lead acetylacetonate instead of the widely used lead acetate trihydrate provided more stability to the PZT precursor solution. Films annealed at 700°C for 12 min formed well-crystallized perovskite phase of Pb(Zr_0.52Ti_0.48)O₃. Microstructures of these films indicated the presence of submicrometer grains (0.1 to 0.2 μm). The dielectric constant and loss values of these films measured at 10 kHz were approximately 1200 and 0.04, respectively, while the remanent polarization and coercive field were ∼ 13 μC/cm² and ∼ 35 kV/cm. Aging of the solution had almost no effect on the dielectric and ferroelectric properties of these films.     

Structural and Electric Properties of Sol–Gel-Derived Ba0.9Sr0.1TiO3 Multilayers

Crack-free Ba_0.9Sr_0.1TiO₃ (BST) and Mn-doped Ba_0.9Sr_0.1TiO₃ (BSTM) multilayers with thickness over 2 μm have been prepared by chemical solution deposition based on one single precursor. Both multilayers exhibit good performance as Bragg reflectors. Mn doping tends to suppress the leakage current in BST multilayers effectively by smoothing the layers and the reduction of the charge carries. The Mn-doped BST multilayer displays an excellent ferroelectric property, with an average remnant polarization ( P _r⁺– P _r⁻)/2 of 12.69 μC/cm² and an average coercive field ( E ⁺ – E ⁻ )/2 of about 72.95 kV/cm under an applied field of 440 kV/cm.     

Electrical and Pyroelectric Properties of Highly (001)-Oriented (Pb0.76Ca0.24)TiO3 Thin Films Grown by a Sol–Gel Process

Highly (001)-oriented (Pb_0.76Ca_0.24)TiO₃ (PCT) thin films were grown on Pt/Ti/SiO₂/Si substrates using a sol–gel process. The PCT film with a highly (001) orientation showed well-saturated hysteresis loops at an applied field of 800 kV/cm, with remanent polarization ( P _r) and coercive electric field ( E _c) values of 23.6 μC/cm² and 225 kV/cm, respectively. At 100 kHz, the dielectric constant and dielectric loss values of these films were 117 and 0.010, respectively. The leakage-current density of the PCT film was 6.15 × 10⁻⁸A/cm² at 5 V. The pyroelectric coefficient ( p ) of the PCT film was measured using a dynamic technique. At room temperature, the p values and figures-of-merit ( F _D) of the PCT film were 185 μC/m²K and 1.79 × 10⁻⁵ Pa^−0.5, respectively.     

Effect of Bottom Electrode Materials and Annealing Treatments on the Electrical Characteristics of Ba0.47Sr0.53TiO3 Film Capacitors

The dielectric constant and leakage current density of Ba_0.47Sr_0.53TiO₃ (BST) thin films deposited by radio-frequency magnetron sputtering on various bottom electrode materials (Pt, Ir, IrO₂/Ir, Ru, RuO₂/Ru) before and after annealing in O₂ and N₂ ambient were investigated. Improvement in crystallinity of BST films deposited on various bottom electrodes was observed with annealing. The refractive index, dielectric constant, loss tangent, and leakage current of the films were also strongly dependent on annealing conditions. A BST thin film deposited on an Ir bottom electrode at 500°C, after 700°C annealing in O₂ for 20 min, had a dielectric constant of 593 ± 5%, a loss tangent of 0.019 ± 10% at 100 kHz, a leakage current of (2.1 ± 13%) 10⁻⁸ A/cm² at an electric field of 100 kV/cm with a delay time of 30 s, and a charge storage density of 53 ± 5% fC/μm² at an applied field of 150 kV/cm. Based on the dielectric constant, leakage current, and reliability, the optimum material for the bottom electrode with annealing was Ir. Interdiffusion of Ru and Ti at the interface between the BST film and Ru electrode was observed in 500°-700°C annealed samples. The 10 year lifetime of time-dependent dielectric breakdown (TDDB) studies indicated that BST on Pt, Ir, IrO₂/Ir, Ru, and RuO₂/Ru had long lifetime over 10 years of operation at a voltage bias of 1 V.     

Microstructure Evolution of Pulsed Laser-Deposited (Ba, Sr)TiO3 Films on MgO for Microwave Applications

To develop low-loss tunable microwave circuits, based on the field dependence of dielectric permittivity, phase pure (Ba_0.5, Sr_0.5)TiO₃ doped with 1% W (BST) thin films 0.3-μm thick were deposited on single crystal MgO wafers by pulsed laser deposition. The BST films were characterized by X-ray θ–2θ scans and pole figure analysis, field emission scanning electron microscopy (FESEM), and cross-sectional transmission electron microscopy (TEM), coupled with selected-area electron diffraction (SAED). Although, the X-ray θ–2θ scan indicated an epitaxial nature of BST with an out-of-plane orientation of (100), the pole figure analysis confirmed the presence (4–6%) of (111)-oriented grains in a matrix of (100) textured grains. The columnar grains exhibited an in-plane (i.e., along the plane perpendicular to the growth direction) grain size that was thickness-dependent. The cross-sectional TEM, coupled with SAED in the thickness direction, corroborated the pole figure analysis. Additionally, from X-ray analysis, it was observed that the textured films were under in-plane tension. The deposited film was characterized at microwave frequencies (1–20 GHz) using interdigitated electrodes deposited on top of the film. The film was characterized by a relatively low dielectric Q of 5–7. A 17% change in the capacitance was observed when applying a 40 V bias. From the observed microstructure, a preliminary understanding of its evolution and its relationship with the microwave dielectric properties is discussed, and some ideas to obtain truly epitaxial BST films are presented.     

Populations and Emission Properties of the 5I6 and 5I7 Levels in Ho3+ Doped into PbO–Bi2O3–Ga2O3 Glasses

Emission properties of PbO–Bi₂O₃–Ga₂O₃ glasses doped with Ho³⁺ were investigated for fiber-optic amplification at the 1.18 μm wavelength region. When the glasses were doped with Ho³⁺ ions only, there was a weak emission at 1.18 μm with a lifetime of ∼200 μs. However, when Yb³⁺ ions were codoped, the lifetime of the 1.18 μm emission increased to 630 μs together with a significant increase in intensity. A similar enhancement in the intensity and lifetimes was realized for the 2.05 μm emission. These effects are due to energy transfer from the Yb³⁺:²F_5/2 to the Ho³⁺:⁵I₆ level. Devitrification of the ternary PbO–Bi₂O₃–Ga₂O₃ glasses was efficiently suppressed by adding 10 mol% GeO₂. Optimum Ho³⁺ concentration was ∼0.4 mol%, whereas Yb³⁺ ions can be added up to the solubility limit.     

Surface Chemical and Leakage Current Density Characteristics of Nanocrystalline Ag–Ba0.5Sr0.5TiO3 Thin Films

Nanocrystalline x Ag–(1− x )Ba_0.5Sr_0.5TiO₃ (Ag–BST, 0≤ x ≤0.1, where x is the mole fraction of Ag) thin films have been deposited on Pt/Ti/SiO₂/Si substrates by a sol–gel method. The films have been characterized by X-ray diffraction (XRD), scanning electron microscopy, and X-ray photoelectron spectroscopy (XPS). The core-level XPS of oxygen (O1 s ) of the Ag–BST films indicate that an optimum amount of Ag ( x =0.02 or 2 mol%) enhances the binding energy of oxygen, possibly through a mechanism in which the electrophilic oxygen dissociates from the Ag surface and fills the oxygen vacancies. Similarly, the binding energy of Ag (Ag3 d ) shows a shift toward a higher value with increasing Ag up to 4 mol%, probably because of the chemical shift of Ag in BST along the surface layers, surface relaxation, or changes in the Fermi level of small Ag particles in the solid solution range of Ag in BST films ( x ≤0.04). The leakage current density of 2 mol% Ag-added BST (∼10⁻⁶ A/cm²) is less by about an order of magnitude than pure BST at an electric field of 200 kV/cm. A defect model is proposed to explain the observed leakage current density of Ag–BST films satisfactorily.     

Hot Forging Characteristics of Fine-Grained ZrO2 and Al2O3/ZrO2 Ceramics

Preliminary results indicate that large strains (∼80%) and strain rates (0.001 s⁻¹) can be obtained without tearing (or cracking) in fine-grain ZrO₂ (0.3 μm) and Al₂O₃/ZrO₂ (1 μm) ceramics. Alumina develops crystallographic and morphological texture as previously reported by Heuer et al.¹     

Multiferroic BiFeO3 Thin Films Buffered by a SrRuO3 Layer

Multiferroic BiFeO₃ thin films of huge polarization have been successfully realized by using SrRuO₃ as a buffer layer on a Pt/TiO₂/SiO₂/Si substrate. They consist of a single perovskite phase and are nearly randomly orientated, where the SrRuO₃ buffer layer lowers the crystallization temperature and improves the crystallinity of BiFeO₃. With increasing deposition temperature during magnetron sputtering, they undergo an apparent grain growth and reduction in surface roughness. The multiferroic thin films deposited on the SrRuO₃-buffered Pt/TiO₂/SiO₂/Si substrate at higher temperatures show much improved polarization and reduced coercive field, together with a lowered leakage current. A huge remnant polarization (2 P _r) of 150 μC/cm² and a coercive field (2 E _c) of 780 kV/cm were measured for the BiFeO₃ film deposited at 650°C.     

Characterization of the Piezoelectric Properties of Pb0.98Ba0.02(Mg1/3Nb2/3)O3–PbTiO3 Epitaxial Thin Films

Pb(Mg_1/3Nb_2/3)O₃–PbTiO₃ (PMN–PT) (70/30) thin films were deposited by pulsed laser deposition using two growth strategies: adsorption controlled deposition from lead-rich targets (∼25–30 mass%) and lower-temperature deposition ( T _d≤600°C) from targets containing a small amount of excess lead oxide (≤3 mass %). The substrates used were (001) SrRuO₃/LaAlO₃. Typical remanent polarization values ranged between 12 and 14 μC/cm² for these films. The longitudinal piezoelectric coefficient ( d _33,f) was measured using in situ four-circle X-ray diffraction, and the transverse coefficient ( d _31,f or e _31,f) was measured using the wafer flexure method. d _33,f and e _31,f coefficients of ∼300–350 pm/V and ∼−11 C/m² were calculated, respectively. In general, the piezoelectric coefficients and aging rates were strongly asymmetric, suggesting the presence of a polarization bias. The large, extremely stable piezoelectric response that results from poling parallel to the preferred polarization direction is attractive for miniaturized sensors and actuators.     

Pyroelectric and Dielectric Properties of Mn Modified 0.82Bi0.5Na0.5TiO3–0.18Bi0.5K0.5TiO3 Lead-Free Thick Films

MnO-doped 0.82Bi_0.5Na_0.5TiO₃–0.18Bi_0.5K_0.5TiO₃(NBT–KBT) thick films with thickness about 40 μm have been prepared using screen printing on Pt electroded alumina substrates. The strong pyroelectric coefficient of 3.8 × 10⁻⁴ C·(m²·°C)^–1 was observed in 1.0 mol% MnO-doped-thick films, and the calculated detectivity figure of merit as high as 1.1 × 10⁻⁵ Pa^−0.5, which can be comparable to that of the commonly used lead based materials. The enhancement of the pyroelectric performances is attributed to the reductions in dielectric constant and loss and the improvements in the pyroelectric coefficient, which can be ascribed to the Mn acts as a hard dopant in the NBT–KBT lattice, creating oxygen vacancies and pinning the residual domains.     

Film Synthesis of Y3Al5O12 and Y3Fe5O12 by the Spray–Inductively Coupled Plasma Technique

Thin films of yttrium aluminum garnet (YAG, Y₃Al₅O₁₂) and yttrium iron garnet (YIG, Y₃Fe₅O₁₂) were synthesized on single-crystal Al₂O₃ substrates by a modification of spray pyrolysis using a high-temperature inductively coupled plasma at atmospheric pressure (spray–ICP technique). Using this technique, films could be grown at faster rates (0.12 μm/min for YAG and 0.10 μm/min for YIG) than using chemical vapor deposition (0.005–0.008 μm/min for YAG) or sputtering (0.003–0.005 μm/min for YIG). The films were dense and revealed a preferred orientation of (211). The growth of YIG was accompanied by coprecipitation of α-Fe₂O₃. The coprecipitation, however, could be largely suppressed by preliminary formation of a Y₂O₃ layer on the substrate.     

A Novel Method for Fabrication of Y2O3-Stabilized ZrO2 Electrolyte Films

Gas-tight Y₂O₃-stabilized ZrO₂ (YSZ) films were prepared on NiO–YSZ and NiO–SDC (Sm_0.2Ce_0.8O_1.9) anode substrates by a novel method. A cell, Ni–YSZ/YSZ(10 μm)/LSM–YSZ, was tested with humidified hydrogen as fuel and ambient air as oxidant. The maximum power densities of 1.64, 1.40, 1.06, and 0.60 W/cm² were obtained at 850°, 800°, 750°, and 700°C, respectively. With methane as fuel, a cell of Ni–SDC/YSZ (12 μm)/LSM–YSZ exhibited the maximum power densities of 1.14, 0.82, 0.49, and 0.28 W/cm² at 850°, 800°, 750°, and 700°C, respectively. The impedance results showed that the performance of the cell was controlled by the electrode polarization rather than the resistance of YSZ electrolyte film.     

Electrophoretic Deposition of Y2O3-Stabilized ZrO2 Electrolyte Films in Solid Oxide Fuel Cells

An electrophoretic deposition (EPD) method was applied for the preparation of yttria-stabilized zirconia (YSZ) films for solid oxide fuel cell (SOFC) applications. Dense YSZ films with uniform thickness can be readily prepared with the EPD method by using acetylacetone or acetone as a solvent. The open-circuit voltages of SOFC, for which the YSZ films were prepared by the EPD method, increased with increasing repetitions of deposition and sintering. It was found that the open-circuit voltage exceeded 1.0 V after five repetitions. When the planar SOFC was fabricated using La_0.6Sr_0.4MnO₃ as a cathode, and electroless plating Pt as an anode, the open-circuit voltage and the maximum power density attained were 1.03 V and 1.84 W·cm⁻², respectively. Consequently, it became evident that the electrophoretic deposition was a suitable processing route for the formation of gas-tight YSZ films with thickness less than 10 μm.     

Effects of Excess Bi2O3 on the Ferroelectric Behavior of Nd-Doped Bi4Ti3O12 Thin Films

Effects of excess Bi₂O₃ content on formation of (Bi_3.15Nd_0.85)Ti₃O₁₂ (BNT) films deposited by RF sputtering were investigated. The microstructures and electrical properties of BNT thin films are strongly dependent on the excess Bi₂O₃ content and post-sputtering annealing temperature, as examined by XRD, SEM, and P – E hysteresis loops. A small amount of excess bismuth improves the crystallinity and therefore polarization of BNT films, while too much excess bismuth leads to a reduction in polarization and an increase in coercive field. P – E loops of well-established squareness were observed for the BNT films derived from a moderate amount of Bi₂O₃ excess (5 mol%), where a remanent polarization 2P _r of 25.2 μC/cm² and 2E _c of 161.5 kV/cm were shown. A similar change in dielectric constant with increasing excess Bi₂O₃ content was also observed, with the highest dielectric constant of 304.1 being measured for the BNT film derived from 5 mol% excess Bi₂O₃.     

High Critical Current YBa2Cu3O7−δ Thick Films on Improved Rolling-Assisted Biaxially Textured Substrates (RABiTS™)

YBa₂Cu₃O_7−δ (YBCO) films with thicknesses ranging from 1.0 to 6.4 μm were deposited by pulsed laser deposition on rolling-assisted biaxially textured substrates (RABiTS). The RABiTS were of the configuration CeO₂/YSZ/Y₂O₃/Ni–3 at.% W. As the YBCO film thickness increased, I _c continued to increase and reached ∼300 A/cm width for a 4.3 μm-thick YBCO film. Commonly observed mechanisms for J _c decrease with increasing YBCO film thickness were not observed. Homogeneous microstructures obtained in even the thickest YBCO films, suggest that the I _c/width can still be enhanced considerably.     

Effects of TiO2 Seeding Layer on Crystalline Orientation and Ferroelectric Properties of Bi3.15Nd0.85Ti3O12 Thin Films Fabricated by a Sol–Gel Method

The effect of a 20-nm thick TiO₂ seeding layer on the growth of a Bi_3.15Nd_0.85Ti₃O₁₂ (BNT) thin film on Pt(111) thin-film substrates has been studied. Under otherwise identical deposition process conditions, the BNT film could be turned from a highly random orientation to a (200) preference orientation by adding the seeding layer. Field-emission scanning electron microscope result reveals that the BNT thin film with the TiO₂ seeding layer is composed of fine grains with smaller sizes about 80–150 nm in diameter. The P _r and E _c values of the BNT thin film and BNT film with the TiO₂ seeding layer were 36 and 16 μC/cm², and 96.9 and 92 kV/cm at a voltage of 12 V, respectively. The fatigue test exhibited a very strong fatigue endurance up to 10⁹ cycles for both films. The leakage current densities were generally in the order of 10⁻⁶–10⁻⁵ A/cm² for both samples.     

Ferroelectric Phase Stability Studies in Spray Deposited KNO3:PVA Composite Films

The composite films of potassium nitrate (KNO₃):poly(vinyl alcohol) (PVA) have been prepared at different temperatures by spray-deposition technique. Ferroelectric hysteresis loops were traced at room temperature for the composite films using modified Sawyer and Tower circuit. The X-ray diffraction studies confirm the existence of ferroelectric phase III of KNO₃ in the composite films at the room temperature, where this phase in pure KNO₃ films is known to exist in the temperature range 110°–124°C. The composite films deposited at 200°C shows the optimum remanent polarization, P _r∼17 μC/cm². The P _r was studied in the frequency range 10 Hz–1 kHz. The stability of the P _r in the composite films exhibits improved fatigue compared with that of quenched KNO₃ films. The capacitance–voltage ( C – V ) characteristics exhibits butterfly features which supports the presence of ferroelectric phase in the composite films. The atomic force microscopy images show that the composite films have uniform dispersion of KNO₃ particles in the PVA matrix.