Orientation-dependent dielectric properties of Ba(Sn0.15Ti0.85)O3 thin films prepared by sol-gel method

The orientation-dependent dielectric properties of barium stannate titanate (Ba(Sn_0.15Ti_0.85)O₃, BTS) thin films grown on (1 0 0) LaAlO₃ single-crystal substrates through sol-gel process were investigated. The nonlinear dielectric properties of the BTS films were measured using an inter-digital capacitor (IDC). The results show that the in-plane dielectric properties of BTS films exhibited a strong sensitivity to orientation. The upward shift of Curie temperature (T_c) of the highly (1 0 0)-oriented BTS thin films is believed to be attributing to a tensile stress along the in-plane direction inside the film. A high tunability of 47.03% was obtained for the highly (1 0 0)-oriented BTS films, which is about three times larger than that of the BTS films with random orientation, measured at a frequency of 1 MHz and an applied electric field of 80 kV/cm. This work clearly reveals the highly promising potential of BTS films for application in tunable microwave devices.     

Improved dielectric properties of (Pb,Ca)TiO3 thin films prepared by metal-organic decomposition method

(Pb,Ca)TiO₃ (PCT) thin films have been deposited on Pt/Ti/SiO₂/Si substrate by metal-organic decomposition (MOD) technique. The film processing parameters such as drying and annealing temperatures have been optimized to obtain good-quality PCT films. Compositional analysis of the film has been studied by X-ray photoelectron spectroscopy (XPS). The effect of the annealing temperature on the crystalline structure, microstructure and electrical properties have been investigated by X-ray diffraction, atomic force microscopy (AFM) and impedance analyzer, respectively. Amorphous PCT films form at 350 °C and crystallize in the perovskite phase following the isothermal annealing at ?650 °C for 3 h in oxygen ambient. Typical tetragonal structure of the PCT film is evidenced from X-ray diffraction pattern. The grain size in the PCT films increases with an increase in annealing temperature. Significant improvement in the dielectric constant value is observed as compared to other reported work on PCT films. The observed dielectric constant and dissipation factor at 100 kHz for 650 °C annealed PCT films are 308 and 0.015, respectively. The correlation of the film microstructural features and electrical behaviors is described.     

Preparation of porous (Ba,Sr)TiO3 by adding corn-starch

A new method of preparing porous (Ba,Sr)TiO₃ ceramics has been introduced, using an ordinary ceramics processing technique. The effect of corn-starch on the positive temperature coefficient of resistivity characteristics and microstructure of the porous (Ba,Sr)TiO₃ ceramics has been investigated. When the corn-starch addition was 1-20 wt%, the PTCR jump was over 10⁶ and 1-2 orders higher than that of samples without corn-starch. Also, it was found that the (Ba,Sr)TiO₃ ceramics had porous microstructure by the addition of corn-starch. The porosity of the ceramics with 20 wt% corn-starch was 44%. The electrical properties of the (Ba,Sr)TiO₃ ceramics have been discussed, based on the microstructure, resistivity of grain boundaries, donor concentration of grains and the electrical potential barrier of grain boundaries.     

Improvement of electrical properties of Sr-modified (Pb,Ca)TiO3 thin films grown by soft chemistry route

Strontium and calcium-modified lead titanate (Pb_0.70Ca_0.15Sr_0.15)TiO₃ soft chemistry-derived thin films were prepared on platinum-coated silicon substrate by spin-coating method. Investigations were made on the structure, surface morphology and electrical properties of the film. The results by XRD and FE-SEM showed that the film exhibits a pure tetragonal perovskite phase and an average grain size of about 50-60 nm, respectively. Electrical measurements of a metal-ferroelectric-metal type capacitor exhibited a stable and switchable electrical polarization in the film. The structure of the Au/PCST/Pt capacitor showed well-saturated hysteresis loops at an applied voltage of 300 kV/cm with remanent polarization and coercive field values of 22 μC/cm² and 100 kV/cm, respectively. At 100 kHz, the dielectric constant and the dielectric loss of the (Pb_0.70Ca_0.15Sr_0.15)TiO₃ thin film with thickness 240 nm were 528 and 0.05, respectively.     

Effect of Bi substitution on the magnetic and dielectric properties of epitaxially grown BaFe0.3Zr0.7O3−δ thin films on SrTiO3 substrates

The structural, dielectric and magnetic properties of single crystalline Ba_1−xBi_xFe_0.3Zr_0.7O_3−δ (x=0.0-0.29) thin films have been studied. The pseudotetragonal epitaxial thin films were obtained by pulsed laser-beam deposition (PLD) on (0 0 1) SrTiO₃ (STO) single-crystal substrates. The Bi substitution for the Ba ions up to an extent of x=0.18 caused a slight improvement in the leakage current properties, as well as an enhancement of the apparent dielectric constant. The saturation magnetization of the films was significantly decreased following Bi substitution. These changes were thought to be related to the increase in oxygen deficiencies in the films. The effect of the Bi substitution on the dielectric and magnetic properties was analyzed in conjunction with the change in valence value of the Fe ions.     

The effect of (00l) crystal plane orientation on the thermoelectric properties of Bi2Te3 thin film

Highly (00l)-oriented pure Bi₂Te₃ films with in-plane layered grown columnar nanostructure have been fabricated by a simple magnetron co-sputtering method. Compared with ordinary Bi₂Te₃ film and bulk materials, the electrical conductivity and Seebeck coefficient of such films have been greatly increased simultaneously due to raised carrier mobility and electron scattering parameter, while the thermal conductivity has been decreased due to phonon scattering by grain boundaries between columnar grains and interfaces between each layers. The power factor has reached as large as 33.7 μW cm⁻¹ K⁻², and the out-of-plane thermal conductivity is reduced to 0.86 W m⁻¹ K⁻¹. Our results confirm that tailoring nanoscale structures inside thermoelectric films effectively enhances their performances.     

Preparation and characterization of Cd2Nb2O7 thin films on Si substrates

Thin Cd₂Nb₂O₇ films were grown on single-crystal p-type SiO₂/Si substrates by the metallo-organic decomposition (MOD) technique. The films were investigated by X-ray diffraction, X-ray energy-dispersive spectroscopy, and field emission scanning electron microscopy, and showed a single phase (cubic pyrochlore), a crack-free spherical grain structure, and nanoparticles with a mean size of about 68 nm. A Cauchy model was also used in order to obtain the thickness and index of refraction of the stack layers (transparent layer/SiO₂/Si) by spectroscopic ellipsometry (SE). The dielectric constant (K) of the films was calculated to be about 25 from the capacitance-voltage (C-V) measurements.     

Structure-related infrared optical properties of BaTiO3 thin films grown on Pt/Ti/SiO2/Si substrates

BaTiO₃ thin films with different thickness have been grown on Pt/Ti/SiO₂/Si substrates by a modified sol-gel method. X-ray diffraction analyses show that the BaTiO₃ thin films are polycrystalline. The crystalline quality of the films is improved with increasing thickness. The infrared optical properties of the BaTiO₃ thin films have been investigated using an infrared spectroscopic ellipsometry in the wave number range of 800-4000 cm⁻¹ (2.5-12.5 μm). By fitting the measured pseudodielectric functions with a three-phase model (Air/BaTiO₃/Pt), and a derived classical dispersion relation for the thin films, the optical constants and thicknesses of the thin films have been simultaneously obtained. The refractive index of the BaTiO₃ thin films increases and on the other hand, the extinction coefficient does not change with increasing thickness in the entirely measured wave number range. The dependence of the refractive index on the film thickness has been discussed in detail and was mainly due to both the crystalline quality of the films and packing density. Finally, the absorption coefficient was calculated in the infrared region for applications in the pyroelectric IR detectors.     

Dielectric properties of ultrathin films of molecular crystals

Dielectric properties of thin films (TF) of molecular crystals, including the effect of size and the boundary surfaces were analysed using Green's function method. Polarisability of molecules in various film layers and dielectric susceptibility of TF were calculated. A comparison with crystal bulk has shown that dielectric properties of TF are strongly influenced both by the sample dimensions and by the boundary conditions.The frequency dependence of the dielectric susceptibility has also been derived. One obtains the monotonous variation for the frequencies above and below exciton band. However, for the frequencies within the exciton band there appears to be complicated, non-monotonous dependence. The relationship between the dielectric susceptibility and the film width for the same frequency shows a complex, oscillatory behaviour. Furthermore, the amplitude of these oscillations increases with increasing film width, demanding the introduction of a damping factor. Finally, the thickness dependence of dielectric susceptibility was analysed in the Cole-Cole plot.     

Preparation and study of silver added La0.67Ca0.33MnO3 film

La_0.67Ca_0.33MnO₃ (LCMO) and Ag admixed La_0.67Ca_0.33MnO₃ (Ag-LCMO) polycrystalline films have been prepared on SrTiO₃ single crystal (100) substrates by ultrasonic spray pyrolysis technique. These films are characterized using XRD, SEM, and temperature dependence of resistivity (ρ-T) and ac susceptibility (χ-T). The films are having cubic structure with lattice parameters as 3.890 and 3.885 Å for LCMO and Ag-LCMO films, respectively. The peek in ρ-T curve (T_p) and the ferromagnetic transition temperature (T_C) for the Ag-LCMO film is higher than that of LCMO film. The stability of both the films was tested by repeated measurements of its characteristics over a period of one week after several thermal cycling from room temperature to 77 K. In the LCMO film, the peak in the ρ-T curve (T_p) is found to shift towards lower value and conduction noise of the film increases in the subsequent measurements. In the case of Ag-LCMO the value of T_p, T_C and conduction noise of the film did not change even after several measurements. Silver segregating at the grain boundaries in Ag-LCMO polycrystalline film seems to be responsible for improving the characteristics of Ag-LCMO films.     

Dielectric relaxation and a.c. conduction phenomena of PbO-PbF2-B2O3 glasses doped with FeO

PbO-PbF₂-B₂O₃ glasses containing different concentrations of FeO have been prepared. The glasses are characterized by X-ray diffraction and differential thermal analysis. The dielectric properties viz., dielectric constant, loss, conductivity, over a moderately wide range of frequency and temperature and dielectric breakdown strength have been investigated. The results of these studies have been analyzed in the light of different oxidation states of iron with the aid of the data on IR, ESR, optical absorption and magnetic susceptibility measurements. The analysis shows that iron ions exist mainly in Fe³⁺ state, occupy tetrahedral positions and increase the insulating strength of the glass if FeO is present in smaller concentrations. However, if FeO is present in higher concentrations in the glass matrix, (i) the dielectric relaxation intensity has been observed to increase, (ii) the intensity and the half width of the ESR signal has been observed to decrease and (iii) the value of magnetic moment (evaluated from magnetic susceptibility) has been observed to drop to a value of 4.6 μ_B from 5.7 μ_B. From these results it has been concluded that in this concentration range, iron ions exist mainly in divalent state.     

Crystal orientation dependence of the in-plane dielectric properties for Ba(Sn0.15Ti0.85)O3 thin films

Barium tin titanate Ba(Sn_0.15Ti_0.85)O₃ (BTS) thin films with (1 0 0), (1 1 0) and (1 1 1) orientation were grown on (1 0 0), (1 1 0) and (1 1 1) LaAlO₃ (LAO) single-crystal substrates through sol–gel process, respectively. The in-plane dielectric properties of the films were measured on interdigital capacitor (IDC). Films with the (1 1 1) orientation had larger relative dielectric constant and larger tunability against the dc bias electric field than (1 0 0)- and (1 1 0)-oriented films. This difference in dielectric properties in these three kinds of oriented BTS films may be attributed due to change in the direction and magnitude of electric polarization in orientation engineered BTS films. This work clearly reveals the dielectric properties of BTS films exhibited a strong sensitivity to crystal orientation.     

Electrical conduction and optical properties of amorphous (Sb2Se3)100−xSnx thin films

The variation of DC electrical conductivity and the optical properties of thermally evaporated a- (Sb₂Se₃)_100−xSn_x thin films with temperature have been studied. It is found that the thermal activation energy decreases, while the optical gap first increases (up to x=1) and then decreases, with the increase in Sn content. These results have been explained by taking into consideration the structural modifications induced by the incorporation of Sn into the parent alloy. The variation in the conductivity prefactor (σ_o) with Sn addition indicates a change in the dominant conduction transport mechanism from extended states to localized states. An experimental correlation between the activation energy and the pre-exponential factor has been observed, indicating the validity of Meyer–Neldel rule in the studied samples.     

Piezoelectric non-linearity in PbSc0.5Ta0.5O3 thin films

Epitaxial (001)-oriented PbSc_0.5Ta_0.5O₃ (PST) thin films were deposited by pulsed laser deposition. Local piezoelectric investigations performed by piezoelectric force microscopy show a dual slope for the piezoelectric coefficient. A piezoelectric coefficient of 3 pm/V was observed at voltages up to 0.8 V. However, at voltages above 0.8 V, there is a steep increase in piezoelectric coefficient mounting to 23.2 pm/V. This nonlinear piezoelectric response was observed to be irreversible in nature. In order to better understand this nonlinear behavior, voltage dependent dielectric constant measurements were performed. These confirmed that the piezoelectric non-linearity is indeed a manifestation of a dielectric non-linearity. In contrast to classical ferroelectric systems, the observed dielectric non-linearity in this relaxor material cannot be explained by the Rayleigh model. Thus the dielectric non-linearity in the PST films is tentatively explained as a manifestation of a percolation of the polar nano regions.     

Annealing temperature influence on electrical properties of ion beam sputtered Bi2Te3 thin films

Ion beam sputtering process was used to deposit n-type fine-grained Bi₂Te₃ thin films on BK7 glass substrates at room temperature. In order to enhance the thermoelectric properties, thin films are annealed at the temperatures ranging from 100 to 400 °C. X-ray diffraction (XRD) shows that the films have preferred orientations in the c-axis direction. It is confirmed that grain growth and crystallization along the c-axis are enhanced as the annealing temperature increased. However, broad impurity peaks related to some oxygen traces increase when the annealing temperature reached 400 °C. Thermoelectric properties of Bi₂Te₃ thin films were investigated at room temperature. The Bi₂Te₃ thin films, including as-deposited, exhibit the Seebeck coefficients of −90 to −168 μV K⁻¹ and the electrical conductivities of 3.92×10²-7.20×10² S cm⁻¹ after annealing. The Bi₂Te₃ film with a maximum power factor of 1.10×10⁻³ Wm⁻¹ K⁻² is achieved when annealed at 300 °C. As a result, both structural and transport properties have been found to be strongly affected by annealing treatment. It was considered that the annealing conditions reduce the number of potential scattering sites at grain boundaries and defects, thus improving the thermoelectric properties.     

Charge transport and discharge mechanism in (PVC+KClO3) polymer electrolyte films

This paper presents results of the studies on ionic conductivity and transference number measurements on potassium chlorate (KClO₃) complexed polyvinyl chloride (PVC) films prepared by solution-cast technique. Temperature dependence of ionic conductivity and transference number data indicated the dominance of ion-type charge transport in these specimens. The magnitude of conductivity increased with increase in the concentration of the salt and temperature. Using this (PVC+KClO₃) electrolyte, solid-state electrochemical cells were fabricated and their discharge profiles were studied under a constant load of 100 kΩ. Several cell profiles associated with these cells were evaluated and are reported.     

On the power-law behavior of the AC conductivity of the mixed crystal (NH4)3H(SO4)1.42(SeO4)0.58

A power law used to describe the AC conductivity from 299 to 393 K of the mixed crystal (NH₄)₃H(SO₄)_1.42(SeO₄)_0.58 led to fractional exponent values ranging from 1.08 to 0.91, depending on structural changes induced on temperature variation [B. Louati, M. Gargouri, K. Guidara and T. Mhiri, J. Phys. Chem. Solids 66 (2005) 762]. In the present note, we suggest that the fractional law exhibits features of lattice relaxation. Despite the structural changes, the parameters of the power law are mutually interconnected to yield a temperature independent phenomenon. Such behavior is probably of general validity and characterizes the universal fractional dispersion of the AC conductivity, as it was also observed in glasses of different composition.     

Lead-free ferroelectric BaTiO3 doped-(Na0.5Bi0.5)TiO3 thin films processed by pulsed laser deposition technique

The difficulties in synthesizing phase pure BaTiO₃ doped-(Na_0.5Bi_0.5)TiO₃ are known. In this work, we reporting the optimized pulsed laser deposition (PLD) conditions for obtaining pure phase 0.92(Na_0.5Bi_0.5)TiO₃-0.08BaTiO₃, (BNT-BT_0.08), thin films. Dielectric, ferroelectric and piezoelectric properties of BNT-BT_0.08, thin films deposited by PLD on Pt/TiO₂/SiO₂/Si substrates are investigated in this paper. Perovskite structure of BNT-BT_0.08 thin films with random orientation of nanocrystallites has been obtained by deposition at 600 °C. The relative dielectric constant and loss tangent at 100 kHz, of BNT-BT_0.08 thin film with 530 nm thickness, were 820 and 0.13, respectively. Ferroelectric hysteresis measurements indicated a remnant polarization value of 22 μC/cm² and a coercive field of 120 kV/cm. The piezoresponse force microscopy (PFM) data showed that most of the grains seem to be constituted of single ferroelectric domain. The as-deposited BNT-BT_0.08 thin film is ferroelectric at the nanoscale level and piezoelectric.     

Dielectric dispersion in PbO-Sb2O3-As2O3:V2O5 glasses

Dielectric properties, viz. dielectric constant ε′, loss tan δ and a.c conductivity σ_ac (over a wide range of frequency and temperature) and dielectric breakdown strength of PbO-Sb₂O₃-As₂O₃ glasses doped with V₂O₅ (ranging from 0 to 0.5 mol%) are studied. Analysis of these results, based on optical absorption and ESR spectra, indicates that the insulating strength of the glasses is comparatively high when the concentration of V₂O₅ is about 0.3 mol% in the glass matrix.     

Synthesis and characterisation of Gd-doped BaTiO3 thin films prepared by laser ablation for optoelectronic applications

The results of gadolinium (Gd)-doped barium titanate (BaTiO₃) thin films prepared by laser ablation on glass and silicon substrates are reported. Rutherford backscattering (RBS) analyses carried out on glass samples indicated the substitution of barium (Ba) by gadolinium (Gd) after annealing, leading to a film with composition Ba_0.76TiGd_0.01O_2.5. There is a reduction in the thickness from 2.21 to 2.02 microns for as-deposited and annealed films. The films on silicon showed a higher degree of crystallinity compared to that of glass substrates due to increased annealing temperature. The average grain size calculated using the X-ray diffraction (XRD) pattern from silicon substrates was 30 nm. The film has a tetragonal structure with a “c/a” ratio of 1.03 signifying that the incorporation of Gd in BaTiO₃ led to the elongation of the c-axis. The percentage transmittance reduced from 80 to 50% due to annealing and this is probably due to structural changes in the film. Swanepoel envelope method employed on the interference fringes of the transmittance pattern led to the determination of the variation of the refractive index with wavelength. Sellmier single oscillator model was applied to determine the optical constants of the films on glass substrates. Bandgap analyses carried out showed the reduction in bandgap with annealing and also the possibility that Gd incorporation has modified the film chemistry leading to the existence of direct (4.35 eV) and indirect (3.88 eV) allowed transitions in the annealed films. Dielectric property measurement carried out under ambient conditions gave a relaxation time τ of 1.6×10⁻⁴ s and conduction by small polaron with the onset of polaron conduction set at about 7 kHz. It is conjectured that these properties, especially the high refractive index and the high bandgaps, can make Gd-doped BaTiO₃ a good candidate for optoelectronic applications.