Phase diagram and dielectric behavior of Ba0.6Sr0.4TiO3 thin films grown on orthorhombic substrates

Using Landau-Devonshire (LD)-type phenomenological model, we investigate the phase diagrams and dielectric behaviors of single-domain single-crystal Ba_0.6Sr_0.4TiO₃ films deposited on orthorhombic substrates. An anisotropic strain factor is introduced to quantitatively calculate the effects of anisotropic in-plane misfit strains. Investigation indicates that anisotropic strains play a crucial role on formation of stable ferroelectric phases and dielectric properties. The anisotropic strains induce tetragonal phases which only contain one in-plane spontaneous polarization component. These phases do not exist in BST films of the same composition under isotropic strains. Moreover, permittivity and tunability of films can reach to maximum when the corresponding spontaneous polarization component disappears at the boundaries of structural phase transition.     

Enhancement of dielectric and ferroelectric properties in ferroelectric superlattices

I studied theoretically the enhancement of remanent polarization and dielectric permittivity of interfacial-coupled ferroelectric superlattices based on the Landau–Ginzburg theory. Our model adopts the Landau–Khalatnikov equation to describe hysteresis behavior and takes the time-dependent space-charge-limited conductivity into account to investigate the ferroelectric and dielectric properties of ferroelectric superlattices. The results are in good agreement with recent experimental observations on the enhancement of remanent polarization and permittivity of BaTiO₃/SrTiO₃ superlattices and heterolayered Pb(Zr,Ti)O₃ thin films.     

In-plane dielectric characterization of sol–gel derived PLZT (9/65/35) thin films using an interdigital electrode configuration

Lead lanthanum zirconate titanate (PLZT 9/65/35) thin films were deposited on MgO (00l) substrates using a sol–gel method. X-ray diffraction measurements reveal that the PLZT film has epitaxially grown on the substrate and has a pure perovskite structure. Using gold interdigital electrodes the in-plane dielectric properties of the films were measured as a function of frequency (1 kHz to 10 GHz), temperature (293–435 K) and dc electric field (0–20 MV/m). The PLZT (9/65/35) thin film exhibits a diffuse phase transition, which indicates a relaxor-like ferroelectric behavior. The temperature dependence of the characteristic relaxation time was analyzed in terms of the Vögel–Fulcher relation. The relative permittivity has a high tunability of 34–42% in the frequency range of 10 MHz to 1 GHz.     

Influence of laser repetition rate on ferroelectric properties of pulsed laser deposited BaTiO3 films on platinized silicon substrate

BaTiO₃ thin films were deposited by pulsed laser deposition on Pt–Si at different laser pulse repetition frequencies. X-ray diffraction spectra show that preferred oriented films can be grown by adjusting the pulse repetition frequency. Enhanced dielectric and ferroelectric properties obtained in films deposited at 1 Hz is attributed to preferred orientation, low strain and homogeneous grain distribution. The films deposited at 1 Hz show an impressive remanent polarization of 21.4 μC/cm² with a coercive field of 70.0 kV/cm. The shift in Curie temperature, which stems from changing the laser pulse repetition frequency, is associated with the strain state in the film.     

Effect of out-of-plane misfit strain on phase diagrams and ferroelectric properties of ferroelectric films in vertical nanocomposite structures

A phenomenological thermodynamic Landau–Devonshire theory is developed to investigate phase diagrams of epitaxial ferroelectric films with out-of-plane misfit strain induced by vertical nanocomposites. The thermodynamic potential of ferroelectric films is obtained based on the boundary conditions of three-dimensional clamping induced by the vertical nanocomposites. Our calculated results indicate that the out-of-plane misfit strain modulates the transition temperature and spontaneous polarization of ferroelectric films in a wide range even the substrate does not provide an effective in-plane misfit strain control. An enhanced critical transition temperature up to 803 °C in BaTiO₃ films under a tensile out-of-plane misfit strain is predicted, which is consistent with the experimental result very well. The polarization properties of BaTiO₃ films can also be effectively modulated by the out-of-plane misfit strain which is controlled by the volume fraction of nanopillars in the vertical nanocomposites. Our method provides a theoretical guide for the out-of-plane strain engineering of ferroelectric films.     

Ferroelectricity in Gly · H3PO3 crystal

A new Gly · H₃PO₃ crystal was grown and its physical properties were investigated. DSC measurements revealed a phase transition at about 224 K. Dielectric investigations showed a large anomaly of dielectric permittivity at 224.7 K along the b-axis. The appearance of spontaneous polarization (along the b-axis) observed by means of a Sawyer-Tower circuit gives evidence for a para-ferroelectric phase transition in this material.     

1-3型纳米多铁复合薄膜中电场诱导的磁化研究

运用Landau-Devonshire热力学唯像理论,考虑铁电相和铁磁相的电致伸缩、磁致伸缩效应以及产生于铁电/铁磁和薄膜/基底界面的弹性应力作用,两次重整介电和磁作用系数得到了这种多铁系统在Landau自由能函数下的本征二次方磁电耦合形式,从而研究了外延1-3型纳米多铁复合薄膜中极化、磁化随薄膜厚度、温度的变化以及该薄膜中外加电场诱导的磁化变化.结果表明薄膜平面内的应压力的弛豫使得磁化强度和极化强度随薄膜厚度的增加而减少,外加电场不仅能诱导铁电相极化场翻转,而且由于铁电和铁磁相界面竖直方向的弹性耦合导致 关键词： 多铁 磁电效应 磁致伸缩 薄膜     

The size effect of Ba0.6Sr0.4TiO3 thin films on the ferroelectric properties

Barium strontium titanate (BST) thin films were prepared by RF magnetron sputtering. The dielectric constant-voltage curves and the hysteresis loops of BST thin films with different grain sizes and film thicknesses were investigated. When the grain size increases from 12 nm to 35 nm, remarkable increases in dielectric constant and tunability were observed. Above 12 nm, the BST films exhibited size effects, i.e. a decrease in maximal polarization (P_m) and an increase in coercive electric field (E_c) with reduction in grain size. In our investigation, the dielectric constant, tunability and maximal polarization increased as the film thickness increased. Furthermore, the size dependence of the dielectric constant and tunability of Ba_0.6Sr_0.4TiO₃ thin films is determined by that of the maximal polarization and the coercive electric field.     

Ferroelectric properties of niobium-doped strontium bismuth tantalate films

The characteristics of ferroelectric thin films of strontium bismuth tantalate (SBT) and niobium-doped strontium bismuth tantalate (SBTN) deposited by radio-frequency (RF) magnetron sputtering on Pt/TiO₂/SiO₂/Si substrates were investigated. For the formation of the structure of the ferroelectric material, the deposited films were subjected to a subsequent annealing at temperatures of 970–1070 K in an O₂ atmosphere. The results of the X-ray diffraction analysis demonstrated that, in contrast to SBT films, in which the Aurivillius phase is formed only at annealing temperatures of 1050–1070 K, the formation of this phase in SBTN films is observed already at a temperature of 970 K. The dependences of the dielectric permittivity, remanent polarization, and coercive force of the SBT and SBTN films on the subsequent annealing conditions were determined. It was found that, upon doping of the SBT films with niobium, the remanent polarization increases by a factor of approximately three, the Curie temperature increases by 50 K, and the dielectric permittivity also increases. It was revealed that, in contrast to the SBT films, the polarization of the SBTN films is observed already at an annealing temperature of approximately 970 K. It was shown that the replacement of SBT films by SBTN films in the manufacture of high-density nonvolatile ferroelectric randomaccess memory (FeRAM) capacitor modules makes it possible to decrease the synthesis temperature from 1070 to 990–1000 K, which improves the compatibility with the planar technology of semiconductor devices. However, it turned out that an increase in the coercive field makes niobium-doped SBT films less attractive for the use in FeRAM.     

Phase transitions in barium–strontium titanate films on MgO substrates with various orientations

A comparative study of the lattice dynamic upon phase transitions in a polycrystalline Ba_0.8Sr_0.2TiO₃ (BST) film on a Pt substrate and in epitaxial BST films grown on various sections of an MgO substrate has been performed by Raman spectroscopy. It has been found that different sequences of phase transitions take place in these films. The BST/Pt films demonstrate the same sequence of phase transitions that is observed in the bulk ceramics. The hardening of a soft mode in BST/(001)MgO and BST/Pt films shows that the transition from the tetragonal ferroelectric phase to the paraelectric phase has features of the displacement-type phase transition and also the order–disorder phase transition. When approaching the ferroelectric transition temperature, the soft mode in the BST/(111)MgO film is softened, following the Cockran law, which indicates the displacement-type phase transition.     

Mechanism of the polarization response in the relaxor state of lead scandotantalate single crystals with different levels of ion ordering

The dielectric properties and optical transmission of stoichiometric lead scandotantalate (PST) single crystals in strong electric fields was studied above the temperature of the spontaneous ferroelectric phase transition (T_sp). It is shown that the mechanism of polarization response directly above T_sp is related to induced polarization effects and macrohysteretic behavior only in ac fields above 5 kV/cm. Ananalysis of reciprocal dielectric permittivity carried out over a broad temperature range far above the temperature at which the dielectric permittivity passes through a maximum revealed that specific features of the relaxor behavior manifest themselves up to 400°C even in highly ordered PST crystals.     

Dielectric response of Ba0.75Sr0.25TiO3 epitaxial films to electric field and temperature

The structure and dielectric parameters of the intermediate ferroelectric layer in the (001)SrRuO₃ ∥ (100)Ba_0.75Sr_0.25TiO₃ ∥ (001)SrRO₃ heterostructure grown by laser ablation on (001)La_0.294Sr_0.706Al_0.647Ta_0.353O₃ were studied. Tensile mechanical stresses accounted for the polar axis in the ferroelectric, being oriented predominantly parallel to the substrate plane. The remanent polarization in the Ba_0.75Sr_0.25TiO₃ layer increased approximately linearly with decreasing temperature in the interval 320–200 K. The real part of the dielectric permittivity of the intermediate ferroelectric layer reached a maximum ?′/?₀=4400 at T _M≈285 K (f=100 kHz). The narrow peak in the temperature dependence of the dielectric loss tangent for the Ba_0.75Sr_0.25TiO₃ ferroelectric layer, observed for T<T _M, shifted toward lower temperatures with decreasing frequency and increasing bias voltage applied to the electrodes.     

Bismuth ferrite composite thin films

0.60Bi_0.90La_0.10FeO₃–0.40Pb(Zr_0.52Ti_0.48)O₃ composite thin films were deposited on Pt/TiO₂/SiO₂/Si(100) substrates by radio-frequency sputtering and their ferroelectric and fatigue properties were mainly investigated. The composite thin films have a low dielectric loss, a high dielectric constant, and enhanced ferroelectric properties of 2P _r～122.6 μC/cm² and 2E _c～479.3 kV/cm, together with a fatigue-free behavior at 200 kHz. Their fatigue behavior is strongly dependent on measurement frequencies, and the concentration of oxygen vacancies plays an important role in their fatigue behavior.     

Pyroelectric properties of some compounds based on protein aminoacids

Protein aminoacid-based compounds were synthesized, and their single crystals were grown. The dielectric and pyroelectric properties of the crystals were studied in the temperature ranges 80–340 and 140–340 K, respectively. It was established that three of the compounds studied (L-His(H₃PO₄)₂, L-TyrHCl, L-Ala₂H₃PO₃ · H₂O) are linear pyroelectrics, with their room-temperature pyroelectric figures of merit being close to those of ferroelectric triglycine sulfate crystals.     

Influence of the substrate on ferroelectric properties of 〈1 1 1〉 oriented rhombohedral Pb(Zr0.6Ti0.4)O3 thin films

〈1 1 1〉-oriented Pb(Zr_0.6Ti_0.4)O₃ thin films were elaborated in the same run by RF multitarget sputtering on Si/SiO₂/TiO₂/Pt(1 1 1) and LaAlO₃/Pt(1 1 1) substrates. PZT thin films were textured, exhibiting 〈1 1 1〉 fibre texture on silicon substrates whereas epitaxial relationships were found when grown on LaAlO₃/Pt(1 1 1). On the latter substrate, values of spontaneous polarization and of dielectric permittivity were measured close to that calculated previously along the 〈1 1 1〉 direction of PZT rhombohedral single crystal. On the contrary, spontaneous polarization and dielectric permittivity measured on PZT thin films deposited on platinized silicon were found deviating from calculated values. These different electrical results are attributed to different ferroelectric domain configurations.     

Structure and dielectric behavior of TlSbS2

A comparison of structure and dielectric properties of TlSbS₂ thin films, deposited in different thicknesses (400–4100 Å) by thermal evaporation of TlSbS₂ crystals that were grown by the Stockbarger–Bridgman technique and the bulk material properties of TlSbS₂ are presented. Dielectric constant ε ₁ and dielectric loss ε ₂ have been calculated by measuring capacitance and dielectric loss factor in the frequency range 20 Hz–10 KHz and in the temperature range 273–433 K. It is observed that at 1 kHz frequency and 293 K temperature the dielectric constant of TlSbS₂ thin films is ε ₁=1.8–6 and the dielectric loss of TlSbS₂ thin films is ε ₂=0.5–3 depending on film thickness. In the given intervals, both of dielectric constant and dielectric loss decrease with frequency, but increase with temperature. The maximum barrier height W _m is calculated from the dielectric measurements. The values of W _m for TlSbS₂ films and bulk are obtained as 0.56 eV and 0.62 eV at room temperature, respectively. The obtained values agree with those proposed by the theory of hopping over the potential barrier. The temperature variation of ac conductivity can be reasonably interpreted in terms of the correlated barrier hopping model since it obeys the ω ^s law with a temperature dependent s (s<1) and going down as the temperature is increased. The temperature coefficient of capacitance (TCC) and permittivity (TCP) are evaluated for both thin films and bulk material of TlSbS₂.     

Dielectric characterization of semiconducting ZnPc films sandwiched between Gold or Aluminum electrodes

The dependencies of complex dielectric functions (the dielectric constant, ε ₁, and the dielectric loss, ε ₂), on frequency and temperature of zinc phthalocyanine (ZnPc) thin films sandwiched between either gold or aluminum Ohmic-electrode contacts have been investigated in the temperature range of 93–470 K and frequency range 0.1–20 kHz. It is found that both values of ε ₁ and ε ₂ decrease with increasing frequency and increase with decreasing temperature. The rate of change depends greatly on the temperature and frequency ranges under consideration. Around room temperature, neither ε ₁ nor ε ₂ show any appreciable change through the whole range of frequencies. Thus, the dielectric dispersion is found to include of both dipolar and interfacial polarizations. The dependencies of both dielectric functions on frequency at different temperatures were found to follow a universal power law of the form ω ⁿ , where the index 0<n≤?1. This indicates that the correlated barrier hopping (CBH) model is a suitable mechanism to describe the dielectric behavior in ZnPc films. Furthermore, the results of the dielectric response indicate that polarization in these films could be in the form of non-Debye polarization. However, the Debye polarization can be traced below room temperature. The obtained results of the relaxation-time, τ, dependency on temperature have shown that a thermally-activated process may be dominated in ZnPc thin films conduction at high temperatures. Partial phase transition (from α- to β-phase) has been observed around 400 K in molecular relaxation-time, τ, and optical dielectric constant, ε _∞. Arrhenius behavior has been observed for all the dielectric loss and conductivity relaxation-times above room temperature and their activation energies are explained and reported. The optical dielectric constant ε _∞ was found to increase with temperature.     

The DC bias function of electrical characterization of PVA inducted nickel chloride composite film

The synthesis of nickel chloride (NiCl₂)-mixed with polyvinyl alcohol films of 15–20 μm in thickness has been carried by solution blending technique. The dielectric properties of the films have been measured in the frequency range of 20 Hz to 1 MHz under a positive bias potential in the range from 0 to 40 V. Improved electric characterization was demonstrated due to ionic incorporation of NiCl₂. The low-frequency polarization was based on the Maxwell–Wagner interfacial model. Hence, this composite film may suggest as suitable electronic polar medium for versatile low-frequency applications.     

Effect of electric field on the dielectric permittivity of betaine phosphite crystals in the paraelectric phase

Temperature dependences of the dielectric permittivity of betaine phosphite crystals are studied both without and under application of an electric bias. It is shown that, in view of the fact that the high-temperature improper ferroelastic (antiferrodistorsive) phase transition at T _c1=355 K is nearly tricritical, the nonlinear temperature dependence of inverse dielectric permittivity in the paraelectric phase and the effect of the field on the dielectric permittivity can be described within a phenomenological model containing two coupled (polar and nonpolar) order parameters with a negative coupling coefficient. An analysis of the model revealed that, in the case where two phase transitions, a nonpolar and a ferroelectric one, can occur in the crystal, all of its dielectric properties, including the polarization response in a field, can be described by one dimensionless parameter a. For the crystal under study, we have a=?2.5. This value of the parameter corresponds to a second-order ferroelectric transition far from the tricritical point, at which a=?1. It is shown that the polarization response in the paraelectric phase in an electric field calculated within this model differs radically from that in the ferroelectric phase-transition model for which the Curie-Weiss law holds in the paraelectric phase.     

Barium silicate modified strontium bismuth tantalate ferroelectric thin films

Novel strontium bismuth tantalate (Sr_0.8Bi_2.2Ta₂O₉ (SBT)) modified with 3 and 5 mol% ratio barium silicate (Ba₂SiO₄) thin films were grown on Pt(100?nm)/Ti(50?nm)/SiO₂/Si(100) substrates by spin coating technique. The influence of barium silicate doping in SBT was studied from the view point of changing dielectric and ferroelectric properties like dielectric constant (ε_r) and remnant polarization (P_r). Well crystallized thin films showed convenient ferroelectric properties with comparatively lower P_r in the range between 1.52 and 0.44 µC/cm² and smaller ε_r value of 163. Thus, with such reduced values of P_r and ε_r barium silicate modified SBT offers a useful potential to be used in Ferroelectric Field Effect Transistor (FeFET) type (1T-type) Ferroelectric Random Access Memories (FeRAMs) upon improving insulation properties.