两种不同(Ba,Sr)TiO3薄膜介电-温度特性的研究

研究并比较了两种不同(Ba0.5,Sr0.5)TiO3(BSTO)薄膜介电-温度特性.采用脉冲激光沉积技术在Pt/Ti/SiO2/Si(100)衬底上制备BSTO薄膜,发现制备条件的不同,可以得到介电性质完全不同的BSTO薄膜.在550℃和氮气氛下制备的BSTO薄膜在常温下具有很高的介电常数,在10kHz下,超过2500,并在200K温度以上介电常数基本不变.它的一些电学性质不同于在正常条件(650℃和氧气氛下)制得的BSTO薄膜,而类似于目前广泛报道的巨介电常数材料如CaCu3Ti4O12.两种薄膜介电性质测试结果表明: 氧气氛下制备的BSTO薄膜呈现铁电-顺电相变,符合居里-外斯定律;低温氮气氛下制备的BSTO薄膜,介电弛豫时间和温度的关系符合德拜模型,是热激发弛豫.文中给出了产生这种介电特性的初步解释.     

The dependence of dielectric properties on the thickness of (Ba,Sr)TiO3 thin films

In the dielectric (Ba,Sr)TiO₃ thin films, the correlation between the film thickness and the dielectric properties was investigated. The dielectric properties such as the dielectric constant (ε) and dielectric loss (tan δ) were measured using the capacitor geometry. As the film thickness increased, the dielectric constant also increased due to the reduction of the interfacial dead-layer effect. However, the dielectric loss did not show a monotonous variation with the increasing film thickness. It was found that the dielectric loss correlated well with the non-uniform distribution of local strain, as analyzed by X-ray diffraction, according to the Curie–von Schweidler relaxation law.     

Material constants of (Ba,Sr)TiO3 solid solutions

The phenomenological theory of solid solution is used to calculate the material constants (elastic compliances, susceptibilities, piezoelectric moduli, pyroelectric constants) of Ba _x Sr_{1 ? x} TiO₃ solid solutions over the entire range of concentrations x at room temperature. The phenomenological potential constants and the numerical values of the material constants are given for specific concentrations.     

Scaling effect of flexoelectric (Ba,Sr)TiO3 microcantilevers

The flexoelectric microcantilever offers an alternative approach for the development of micro/nano‐sensors. The transverse flexoelectric coefficients µ₁₂ of barium strontium titanate microcantilevers were measured at room temperature, and found to keep the same value of 8.5 µC/m for microcantilevers with thickness ranging from 30 µm to 1.4 mm. The calculated effective piezoelectric coefficient and electrical energy density of flexoelectric cantilevers are superior to those of their piezoelectric counterparts, suggesting that the flexoelectricity‐induced polarization can be significantly increased as structures are scaled down due to the scaling effect of strain gradient, holding promise for flexoelectric micro/nano cantilever sensing applications. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Ba1-xSrxTiO3及Ba0.6-xPbxSr0.4TiO3陶瓷的制备和介温特性研究

用固相反应法制备了Ba_1-xSr_xTiO₃(BST)及Ba_0.6-xPb_xSr_0.4TiO₃(BPST)陶瓷,通过XRD,FESEM和拉曼谱分析了Pb掺杂对Ba_0.6Sr_0.4TiO₃样品的晶格、相变及表面形貌的影响.测试了BST及B 关键词： BST BPST 弥散相 介温特性     

Structural and crystallization behavior of (Ba,Sr)TiO3 borosilicate glasses

Various glass samples were prepared by melt quench technique in the glass system [(Ba_{1? x} Sr _x ) TiO₃]–[2SiO₂–B₂O₃]–[K₂O] doped with 1?mole% of La₂O₃. Infrared spectra show the number of absorption peaks with different spliting in the wave number range from 450 to 4000?cm^?1. Absorption peaks occurs due to asymetric vibrational streching of borate by relaxation of the bond B–O of trigonal BO₃. Raman spectra show the Raman bands due to ring-type metaborate anions, symmetric breathing vibrations BO₃ triangles replaced by BO₄ tetrahedra, and symmetric breathing vibrations of six-member rings. The differential thermal analysis of a glass sample corresponding to composition x?=?0.0 shows crystallization temperature at 847°C and glass transition temperature at 688°C. X-ray diffraction (XRD) pattern of glass ceramic samples shows the major crystalline phase of BaTiO₃ whereas pyrochlore phases of barium titanium silicate. Scanning electron micrographs confirm the results of XRD as barium titanate is major crystalline phase along with pyrochlore phase of barium titanium silicate.     

Raman spectroscopy of BaTiO3/(Ba,Sr)TiO3 superlattices

A series of BaTiO₃/Ba_{1 ? x} Sr _x TiO₃ (BT/BST) superlattices were prepared by pulsed laser deposition on MgO substrates with a constant period of 80 Å (40 Å BT and 40 Å BST) and varying compositions of the BST layer so that the Ba/Sr concentration ratios were 0/100, 30/70, 40/60, 50/50, 60/40, 70/30, 100/0. The soft mode E(1TO) of the polarized Raman spectra transformed depending on the Ba/Sr ratio in the BST layer. As the Sr concentration in the BST layers increased from 0 to 100%, the E(1TO) soft mode half-width varied from 171 to 103 cm^?1 and its frequency increased from 31 to 109 cm^?1 due to the interaction between the epitaxial layers forming the superlattices.     

Dielectric response of (Ba,Sr)TiO3 thin films in a terahertz and IR ranges

Dependences of the dielectric response spectra on the thickness of the films based on the (Ba,Sr)TiO₃ (BST) solid solutions, which were deposited on single-crystal MgO substrates, have been analyzed. Using the Lorentz and Lyddane-Sachs-Teller models, the mutual correspondence of longitudinal optical (LO) and transverse optical (TO) phonon frequencies has established. The giant LO-TO splitting of the lowest-frequency vibration and inversion of LO and TO frequencies of other phonons in the IR spectrum of BST films has been found for the first time.     

X-ray diffraction investigation of BaTiO3/(Ba,Sr)TiO3 superlattices

Samples of BaTiO₃/(Ba_{1 ? x} Sr _x )TiO₃ (BT/BST-x) superlattices have been studied using X-ray diffraction analysis. A complete parallel orientation of all the studied films and the substrate has been revealed, and the modulation periods ?? of the superlattices, the parameters of the unit cell averaged over the ?? period, and the parameters of individual components of the superlattices have been determined.     

Relaxor properties of Nb-modified (Ba0.8Sr0.2)TiO3 ceramics

Nb-doped (Ba_0.8Sr_0.2)TiO₃ ceramics were prepared using conventional mixed-oxide processing technique. Permittivity and loss factor were investigated as a function of temperature for various frequencies of the measuring field. The obtained results confirmed the relaxor ferroelectric behaviour of the studied ceramics, i.e. a strong frequency dispersion of the permittivity maximum and a visible shift of its temperature with frequency. Analysis of real part of permittivity allowed us to determine the value of the freezing temperature characterising the relaxor ferroelectrics. The physical processes, responsible for the relaxor behaviour of the studied ceramics are discussed.     

Improved dielectric and electrical properties of (Ba,Sr)TiO3 thin films using Pt/LaNiO3 as the top-electrode material

(Ba,Sr)TiO₃ (BST) capacitors grown on a LaNiO₃ (LNO) bottom electrode, with Pt (80 nm), LNO (100 nm), and double-layer Pt/LNO (80/10 nm) top electrodes have been investigated. It was found that the dielectric behavior is improved by a decrease of the electrical properties for the BST capacitor using double-layer Pt/LNO top electrodes. The dielectric constant of 100 nm-thick BST films with a Pt electrode was only 165 at 100 kHz, while that with a double-layer electrode was about 242. Correspondingly, the tunability was greatly improved from 26% to 41% with an electric field of 600 kV/cm. These have been attributed to increased interfacial capacitance density, which resulted from an improved interface, between the films and the top electrode. The dielectric loss was also reduced by using a double-layer electrode. Furthermore, the leakage current of a capacitor with a double-layer Pt/LNO electrode was one order of magnitude lower than that with a single LNO electrode. It can be explained by the fact that the weak chemical interaction between LNO (10 nm) and BST causes a high potential barrier at the interface. PACS 81.15.-z; 81.15.Cd; 77.55.+f; 77.84.Dy; 77.22.-d     

溶胶-凝胶法制备(Ba0.7Sr0.3)TiO3/LaNiO3异质薄膜及其结构和介电性质研究

采用改进的溶胶-凝胶方法在单晶Si(100)衬底上制备了介电性能优异的(Ba0.7Sr0.3)TiO3/LaNiO3 异质薄膜.实验发现,在750 ℃下、O2气氛中晶化的LaNiO3薄膜的电阻率最小.C-V与I-V特性测量表明(Ba0.7Sr0.3)TiO3薄膜具有优异的介电性能,在频率为50 kHz、零偏压下的相对介电常数εr>300,偏压为6 V时漏电流密度JL<1.2×10-6 A/cm2.     

Structural,photoluminescent, and dielectric properties of Eu3+-doped Ba0.7Sr0.3TiO3 thin films

Eu³⁺-doped Ba_0.7Sr_0.3TiO₃ thin films were prepared by a chemical solution deposition method and characterized by X-ray diffraction, field emission scanning electron microscopy, photoluminescence and dielectric measurements. The thin films were well crystallized with a pure perovskite structure. A contraction of the unit cell was observed upon incorporation of Eu³⁺ ions below 2 mol%, while an expansion occurred as the Eu³⁺ concentration was further increased above 2 mol%, indicating that Eu³⁺ ions with different concentrations occupied different lattice sites. Photoluminescence spectra showed two prominent transitions of Eu³⁺ ions at 594 nm (⁵D₀ → ⁷F₁) and 618 nm (⁵D₀ → ⁷F₂) upon excitation at 395 nm (⁷F₀ → ⁵L₆). There existed two quenching concentrations at 2 mol% and 4 mol% due to different lattice sites of the Eu³⁺ ions. We also investigated the dielectric properties of the thin films. Our study suggests that Eu³⁺-doped Ba_0.7Sr_0.3TiO₃ thin films have potential applications in multifunctional optoelectronic devices.     

Temperature effect on the trapped-charge relaxation in (Ba,Sr)TiO3 films on silicon

The trapped-charge relaxation has been calculated for a two-layer insulator with negligible conductivity in one of the layers the conductivity of the other layer obeying the Pool-Frenkel mechanism. The calculated values are compared with the experimental data on the trapped-charge relaxation in (Ba,Sr)TiO₃ films on silicon substrates. On the basis of this comparison, the depth of location and concentration of Frenkel emission centers are estimated. The results obtained can be used in the analysis of relaxation processes in ferroelectrics, which have strong electric fields in surface layers.     

Investigation of the low-and infralow-frequency dielectric response of Ba0.7Sr0.3TiO3 thin films

The low-and infralow-frequency dielectric properties of Ba_0.7Sr_0.3TiO₃ thin films annealed at temperatures of 750 and 900°C are investigated over wide ranges of temperatures (from ?180 to +100°C), frequencies (from 0.1 Hz to 10.0 kHz), and amplitudes of the measuring electric field (from 15 to 255 kV/cm). The samples are found to undergo giant relaxation characteristic of layered heterogeneous structures. It is noted that, at a higher annealing temperature (900°C), the relaxation region is shifted toward lower temperatures (higher frequencies).     

(Sr,Mn)TiO3: a magnetoelectric multiglass

By close analogy with multiferroic materials with coexisting long-range electric and magnetic orders a "multiglass" scenario of two different glassy states is observed in Sr(0.98)Mn(0.02)TiO(3) ceramics. Sr-site substituted Mn2+ ions are at the origin of both a polar and a spin glass with glass temperatures T(g) approximately equal to 38 K and < or =34 K, respectively. The structural freezing triggers that of the spins, and both glassy systems show individual memory effects. Thanks to strong spin-phonon interaction within the incipient ferroelectric host crystal SrTiO3, large higher order magnetoelectric coupling occurs between both glass systems.     

Capacitance of the La0.67Sr0.33MnO3/(Ba,Sr)TiO3 interface induced by electric field penetration into the manganite electrode

(001)La_0.67Sr_0.33MnO₃/(001)(Ba_xSr_{1 ? x} TiO₃/(001)La_0.67Sr_0.33MnO₃(x= 0–0.25) three-layer heterostructures are grown by laser evaporation on (001)La_0.3Sr_0.7Al_0.65Ta_0.35O₃ single-crystalline substrates. In a wide temperature range (≈150 K), effective permittivity ? of (1000 nm)Ba_0.25Sr_0.75TiO₃ and (1000 nm)SrTiO₃ films grown obeys the relationship ? ～ (T ? T _CW)^?1, where T _CW is the Curie-Weiss temperature for related bulk crystals. Using experimental dependences ?(T), the capacitance of the (001)La_0.67Sr_0.33MnO₃/(001)Ba_xSr_1?x TiO₃ and (001)La_0.67Sr_0.33MnO₃/(001)SrTiO₃ interfaces, which is due to electric field penetration into the manganite electrode, is estimated (C _int≈4μF/cm²). At bias voltages of ± 2.5 V, the change in the permittivity of the STO and BSTO films in the heterostructures studied reaches 25 and 45%, respectively.     

两种不同(Ba,Sr)TiO3薄膜介电-温度特性的研究

研究并比较了两种不同(Ba_0.5,Sr_0.5)TiO₃(BSTO)薄膜介电-温度特性.采用脉冲激光沉积技术在Pt/Ti/SiO₂/Si(100)衬底上制备BSTO薄膜，发现制备条件的不同，可以得到介电性质完全不同的BSTO薄膜.在550℃和氮气氛下制备的BSTO薄膜在常温下具有很高的介电常数，在10kHz下，超过2500，并在200K温度以上介电常数基本不变.它的一些电学性质不同于在正常条件(650℃和氧气氛下)制得的BSTO薄膜，而类似于目前广泛报道的巨介电常数材料如CaCu_３Ti_４O₁₂.两种薄膜介电性质测试结果表明: 氧气氛下制备的BSTO薄膜呈现铁电-顺电相变，符合居里-外斯定律；低温氮气氛下制备的BSTO薄膜，介电弛豫时间和温度的关系符合德拜模型，是热激发弛豫.文中给出了产生这种介电特性的初步解释. 关键词： 薄膜 脉冲激光沉积 介电弛豫     

Effect of low-angle boundaries on the dielectric properties of epitaxial Ba0.8Sr0.2TiO3 films

The effect of low-angle boundaries on the dielectric properties of epitaxial Ba_0.8Sr_0.2TiO₃ films is studied by comparing films differing in crystalline-block size. It is found that the permittivity diminishes considerably when the block sizes are reduced. The maximum of the temperature-dependent permittivity is shifted towards lower temperatures, and the sensitivity of the permittivity to an electric field is reduced. Moreover, it is found that the maximum in the permittivity temperature dependence is displaced towards lower temperatures when the applied measured voltage is increased and becomes higher than the coercive voltage. The width of a hysteresis loop decreases significantly when the frequency of the controlling field is reduced. The reasons for the observed behavior are analyzed.     

Structural and microwave properties of (Ba,Sr)TiO3 films grown by pulsed laser deposition

The relationship between the structure and the microwave dielectric properties of epitaxial Ba_0.5Sr_0.5TiO₃ (BST) films has been investigated. Single-phase BST films (40-160 nm) have been deposited onto (100) MgO substrates by pulsed laser deposition. As-deposited films show a significant tetragonal distortion. The in-plane lattice parameters (a) are always larger than the surface normal lattice parameters (c). The tetragonal distortion depends on the thickness of the films and the post-deposition annealing conditions. Films annealed at 900 °C show less tetragonal distortion than the as-deposited film and the films annealed at higher temperatures. The distortion in the film is due to stress caused by the lattice mismatch and thermal expansion coefficient differences between the film and the substrate. The dielectric constant and its change with dc bias voltage of BST films on MgO at microwave frequencies increase with increasing annealing temperature from 900 °C to 1200 °C, which corresponds to an increase in the tetragonal distortion.