Film thickness dependence of electro-optic effect in epitaxial BaTiO3 thin films

Based on the phenomenological Landau-Devonshire theory, we investigate the film thickness dependence of ferroelectric and electro-optic properties of epitaxial BaTiO₃ thin films grown on SrTiO₃ and MgO substrates. By using the effective substrate lattice parameter concept, the film thickness dependence of misfit strain is incorporated into the theory. Therefore, the film thickness dependence of ferroelectric and electro-optic properties in epitaxial BaTiO₃ thin films can be explained. Moreover, a large quadratic electro-optic effect was obtained in the BaTiO₃ thin films, which is in good agreement with the experimental result of BaTiO₃ thin films on the MgO substrate.     

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.     

Structural and electrical properties of 0.7Pb(Mg<Subscript>1/3</Subscript>Nb<Subscript>2/3</Subscript>)O<Subscript>3</Subscript>–0.3PbTiO<Subscript>3</Subscript> thin films grown on Ir/MgO buffered Si(100) substrates

Thin films of 0.7Pb(Mg_1/3Nb_2/3)O₃–0.3PbTiO₃ (PMN-PT) have been grown on Ir/MgO buffered Si(100) substrates at different substrate temperatures by pulsed laser deposition. Crystalline phases as well as preferred orientations in the PMN-PT films were investigated by X-ray diffraction analysis (XRD). The microstructure, dielectric and ferroelectric properties of PMN-PT film prepared at 650 °C were studied. The results show that the film prepared at 650 °C exhibits pure perovskite phase and single c-axis orientation. The dielectric constant and dissipation factor of the single c-axis oriented film are 1000 and 0.04 at a frequency of 1 kHz, while the remnant polarization and coercive field are about 13.0 μC/cm² and 100 kV/cm under an electric field of 480 kV/cm, respectively. PACS 81.15.Fg; 77.80.-e; 77. 22.Ej; 77.55.+f; 85.50.Gk     

Ferroelectricity and structure of BaTiO3 grown on YBa 2Cu3O_{7 - \delta } thin films

We have investigated the crystal structure and the ferroelectric properties of BaTiO₃ thin films with YBa₂Cu₃O as the bottom and Au as the top electrode. Epitaxial heterostructures of YBa₂Cu₃O and BaTiO₃ were prepared by dc and rf sputtering, respectively. The crystal structure of the films was characterised by X-ray diffraction. The ferroelectric behaviour of the BaTiO₃ films was confirmed by hysteresis loop measurements using a Sawyer Tower circuit. We obtain a coercive field of 30 kV/cm and a remanent polarisation of 1.25 μC/cm². At sub-switching fields the capacitance of the films obeys a relation analogous to the Rayleigh law. This behaviour indicates an interaction of domain walls with randomly distributed pinning centres. At a field of 5 MV/m we calculate a 3% contribution of the irreversible domain wall motion to the total dielectric constant. Received 24 June 1999 and Received in final form 27 August 1999     

(111)取向(Pb,La)TiO3铁电薄膜中90°纳米带状畴与热释电性能的研究

采用射频磁控溅射技术在Pt/Ti/SiO₂/Si(100)衬底上生长了掺镧钛酸铅(PLT)铁电薄膜.用X射线衍射技术(XRD)研究了PLT薄膜结晶性能，结果表明PLT薄膜为 (111)择优取向钙钛矿相织构.使用原子力显微镜(AFM)和压电响应力显微镜(PFM) 分别观察了PLT薄膜的表面形貌和对应区域的电畴结构.PFM观察显示PLT薄膜中存在90°纳米带状畴，电畴的极化为首尾相接的低能量的排列方式，带状畴的宽度为20—60nm.研究了PLT10铁电薄膜的制备条件与性能之间的关系.发现在优化条件下制备的PLT10铁电薄膜的介电常数ε_r为365、介电损耗tgδ为0.02，热释电系数γ为2.18×10^-8C·(cm²·K)^-1，可以满足制备非制冷红外探测器的需要. 关键词： PLT薄膜 电畴 PFM 极化     

Nonlinear dielectric response of epitaxial Ba<Subscript>0.6</Subscript>Sr<Subscript>0.4</Subscript> TiO<Subscript> 3</Subscript> thin films

Based on Landau-Devonshire (LD)-type phenomenological thermodynamic theory, the electric field dependence of the dielectric properties of tetragonal single-domain barium strontium titanate(Ba_1-xSr_xTiO₃) films on cubic substrates is theoretically investigated by taking into account the high order terms of the polarization. At room temperature, the nonlinear dielectric responses of epitaxial Ba_0.6Sr_0.4TiO₃ films are provided by adjusting the film thickness and growth temperature. The strong nonlinearity of relative dielectric constant and pyroelectric coefficient are attained around critical film thickness on MgO (69 nm) and LaAlO₃ (132 nm) substrates or critical growth temperature on MgO (337 °C) substrate with respect to epitaxy-induced lattice misfit and thermal stresses during deposition. This can be explained that small compressive stresses are effective to support high nonlinearity of dielectric constant and pyroelectric coefficient for Ba_0.6Sr_0.4TiO₃ films irrespective of whether they are on compressive substrate or tensile substrate. It is also predicted that a large tunability may be achieved by altering processing conditions, such as the film thickness and growth temperature for different substrates. Our theoretical results are in good agreement with the experimental data reported in literature.     

脉冲激光淀积BaTiO3薄膜的介电与铁电特性

用脉冲激光淀积方法在SrTiO₃衬底上制备了BaTiO₃/YBa₂Cu₃O_7-δ（铁电/超导）双层膜，X射线分析表明BaTiO₃薄膜是高度c取向的．对BaTiO₃薄膜的介电和铁电性能进行了实验研究．观察到铁电薄膜特有的电滞线和蝶型C-V曲线，薄膜呈现出较好的铁电性，在铁电随机存储等领域有重要的应用前景 关键词：     

Si基Bi3.25La0.75Ti3O12铁电薄膜的制备与特性研究

采用Sol-Gel工艺低温制备了Si基Bi_3.25La_0.75Ti₃O₁₂铁电薄膜.研究了退火温度对薄膜微观结构、介电特性与铁电性能的影响.500℃退火处理的Bi_3.25La_0.75Ti₃O₁₂薄膜未能充分晶化，晶粒细小且有非晶团聚，介电与铁电性能均较差.高于550℃退火处理的Bi_3.25La_{0.75 关键词： 铁电薄膜 3.25}La_0.75Ti₃O₁₂')" href="#">Bi_3.25La_0.75Ti₃O₁₂ Sol-Gel工艺     

Structure and electrical properties of trilayered BaTiO3/(Na0.5Bi0.5)TiO3–BaTiO3/BaTiO3 thin films deposited on Si substrate

Highly (110)-oriented trilayered BaTiO₃ (25 nm) /(Na_0.5Bi_0.5)_0.94Ba_0.06TiO₃ (300 nm) / BaTiO₃ (25 nm) thin films were deposited on Pt/Ti/SiO₂/Si substrates via chemical solution deposition. It was found that the inserted bottom BaTiO₃ layer between Pt and (Na_0.5Bi_0.5)_0.94Ba_0.06TiO₃ is very effective for promoting the crystallinity and (110)-oriented growth of NBT-BT films. Meanwhile, the BaTiO₃ layers also provide better interfaces between the ferroelectric thin film and the electrodes in terms of reducing leakage current. The trilayered films showed enhanced dielectric and ferroelectric properties compared with the pure NBT-BT films. Well saturated hysteresis loops were obtained due to good electrical insulating properties in the high electric field region.     

Sol–gel derived ferroelectric Bi3.15Nd0.85Ti3O12 thin films of predominant 100/010/119 orientation deposited both on Nb-doped (011)SrTiO3 and on (011)SrRuO3/(011)SrTiO3

Ferroelectric Bi_3.15Nd_0.85Ti₃O₁₂ (BNdT) thin films of predominant 100/010/119 orientation were grown through a cheap and simple sol–gel process both on Nb-doped (011)SrTiO₃ and on (011)SrRuO₃/(011)SrTiO₃. Using rapid heating rates during crystallization, films containing 28% (100)/(010)-oriented grains plus 19% (119)-oriented grains were obtained on SrRuO₃/SrTiO₃, while 30% (100)/(010)- and 18% (119)-oriented grains were obtained on Nb:SrTiO₃. The films consist of columnar grains and 90° a–b domains exist in large BNdT grains. The BNdT thin films exhibit excellent ferroelectric and dielectric properties with a remanent polarization 2P_r=39.2 μC/cm² and a dielectric constant ε_r=184.5. PACS 77.80.Fm; 77.80.Dj; 68.60.Wm; 68.55.Jk; 68.37.Lp     

Ferroelectric SrxBa1-xNb2O6 optical waveguiding thin films on SiO2-coated Si(100) substrates

x Ba_1-xNb₂O₆ (x=0.5) films (abbreviated as SBN:0.5) on SiO₂-coated Si substrates are potential components for the application of integrated electro-optics devices. SBN:0.5 optical waveguiding thin films on SiO₂-coated Si substrates with a very thin MgO diffusion buffer have been successfully prepared by pulsed laser deposition. The as-grown films have a refractive index of 2.28, which is close to that of bulk SBN. X-ray analysis showed that the as-grown films have a single-phase tetragonal tungsten bronze structure. The SBN:0.5 thin films prepared by PLD exhibit favorable ferroelectric and optical waveguiding properties. The composition and the morphology of the films were also examined by XPS and by SEM, respectively. Ferroelectric SBN:0.5 optical waveguiding thin films on SiO₂-coated Si substrates are expected to be used in integrated electro-optic devices. Received: 27 February 1997/Accepted: 17 October 1997     

Effects of strontium and calcium simultaneous substitution on electrical and structural properties of Pb1?x?yCaxSryTiO3 thin films

Ferroelectric Pb_1−x−y Ca _x Sr _y TiO₃ thin films (denoted by PCST90, PCST70, and PCST30) were deposited on the Pt/Ti/SiO₂/Si substrates by a chemical solution deposition method. Their properties were investigated from the viewpoint of crystal structure, microstructure, dielectric, and ferroelectric properties. X-ray diffraction patterns revealed the formation of PCST90, PCST70, and PCST30 thin films without any secondary phases. Infrared and Raman spectroscopy results show that a gradual phase transition from tetragonal to pseudocubic or cubic perovskite structure may occur in PCST thin films with the simultaneous increase of Ca²⁺ and Sr²⁺ contents. Both substitution of isovalent Ca²⁺ and Sr²⁺ at Pb²⁺-site enhanced the dielectric constant and reduced the remnant polarization. In addition, ferroelectric test analyses show that the PCST thin films undergo a ferroelectric-to-paraelectric phase transformation with an amount of Pb²⁺, Ca²⁺, and Sr²⁺ at 30%, 35%, and 35% mol, respectively. Hence, the absence of ferroelectric property may be attributed to a decreasing of the octahedron distortion in the perovskite structure accompanied by a weakening of long-range ferroelectric order.     

Effect of microstructure of MgO buffer layer on BaTiO3 grown on silicon substrates

MgO ultrathin films were grown on Si(1 0 0) substrates as buffer layers for the growth of ferroelectric BaTiO₃ thin films by laser molecular beam epitaxy (L-MBE). The deposition process of MgO buffer layers grown on silicon was in situ monitored by reflection high-energy electron diffraction (RHEED). The structure of BaTiO₃ films fabricated on MgO buffers was investigated by X-ray diffraction. Biaxially textured MgO was obtained at high laser energy density, but when the laser energy was lowered, MgO buffer was transformed to the form of texture with angular dispersion with the increase of the film thickness. BaTiO₃ films grown on the former buffer were completely (0 0 1) textured, while those on the latter were (0 0 1) preferred orientated. Furthermore, the fabricated MgO buffers and BaTiO₃ films had atomically smooth surface and interface. All these can reveal that the quality of textured MgO buffer is a key factor for the growth of BaTiO₃ films on silicon.     

Effect of lanthanum substitution on the Raman spectra of barium titanate thin films

Thin films of Ba_1−xLa_xTiO₃ on platinum substrates were synthesized using the sol–gel method for x values of 0.0, 0.03, 0.05, and 0.10, and the effect of trivalent La³⁺ substitution on the structural and dielectric properties was studied. Using X‐ray diffraction, structural analysis of these compositions revealed a slight increase in the tetragonal distortion of the unit cell with increase in La content. Accordingly, an increase in the tetragonal to cubic transition temperature T_T/C was detected by temperature‐dependent Raman spectroscopy in the range of 70–500 K. Unlike the results from Raman scattering for the La‐doped BaTiO₃ films, the dielectric measurements showed broad and diffused dielectric maxima, making the estimation of the transition temperature merely qualitative. Copyright © 2006 John Wiley & Sons, Ltd.     

Off-axis pulsed laser deposition system for epitaxial oxide growth on substrates up to 2 inches in diameter

A novel off-axis pulsed-laser deposition (PLD) system for ferroelectric oxide thin films has been developed. The substrates are mounted "upside-down" and are rotating. The maximum substrate size is 2 inches in diameter. The optical and structural properties of the grown BaTiO₃ films are compared to the films produced by an on-axis PLD system. The stoichiometry and thickness were checked with Rutherford backscattering spectrometry (RBS). The crystalline quality and orientation were investigated with X-ray diffraction (XRD) and Rutherford backscattering spectrometry in channeling configuration (RBS/C). Using atomic force microscopy, the rms surface roughness was measured. The BaTiO₃ films grown on MgO form a planar optical waveguide. The optical losses and the refractive indices of these waveguides were determined with a prism coupling setup. Films grown on 10᎒ mm² MgO (100) substrates in on-axis geometry show optical waveguide losses less than 3 dB/cm.     

Laser-deposited thin films for butane detection

Thin films of ZnO and BaTiO₃, prepared by pulsed laser deposition (PLD), were studied as sensors for butane detection. The layers of ZnO, prepared on special substrates, were used as conductive-type sensors. The layers of ZnO and BaTiO₃, deposited on fused silica substrates, were tested by the optical m-line technique. Butane concentrations as low as 100 ppm were detected at room temperature.     

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.     

Room-temperature multiferroic properties of Bi4.15Nd0.85Ti3FeO15 thin films prepared by the metal–organic decomposition method

Aurivillius-structured Bi_4.15Nd_0.85Ti₃FeO₁₅ multiferroic thin films with four perovskite slabs were deposited on Pt/Ti/ SiO₂/Si substrates by the metal–organic decomposition method. The structural, dielectric and multiferroic properties of the films were investigated. Good ferroelectric behavior along with large dielectric constant and small loss factor were observed at room temperature. A weak ferromagnetic rather than an antiferromagnetic property was observed at room temperature by magnetic measurement. Moreover, the ferromagnetic property was enhanced when the temperature was below 13 K and a large saturation magnetization of about 5.4 emu/cm³ was obtained at 4 K. Possible reasons are put forward to discuss the complicated magnetic property.     

Effect of preferred orientation on magnetoelectric properties of multiferroic La0.7Sr0.3MnO3/BaTiO3 heterostructure

The epitaxial La_0.7Sr_0.3MnO₃/BaTiO₃ bilayer heterostructures were deposited on LaAlO₃ (001) and (110) substrates by pulsed laser deposition. The inherent ferromagnetic, ferroelectric properties and strong magnetoelectric (ME) effect at room temperature were approved, which correlated to the preferred orientation of the films. Both heterostructures showed similar frequency-dependent ME behavior in 0.1 kHz-100 kHz, the ME voltage coefficients were around 140 mV/cm Oe and 104.8 mV/cm Oe at 1 kHz for (001) and (110) oriented bilayers, respectively. This was at least one order of magnitude higher than previously reported results of the related heterostructures, which is mainly ascribed to the lower dielectric constant of BTO film.     

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.