溶胶-凝胶法制备的Ba0.8Sr0.2TiO3薄膜的结构及铁电性质研究

采用0.05mol/L的前驱体溶液,利用溶胶-凝胶法成功制备了室温下具有优良铁电性质的Ba_0.8Sr_0.2TiO₃ (BST)薄膜.X射线衍射分析表明,制得的BST薄膜室温下呈四方相,场发射扫描电子显微观测显示BST薄膜表面平整、致密、无裂纹出现,薄膜晶粒呈柱状结构、尺寸在150nm左右.电学测量表明制备的BST薄膜室温下具有优良的铁电性能.薄膜的剩余极化P_r约为35μC/cm²,矫顽电场E关键词：     

The influence of Co doping on the dielectric, ferroelectric and ferromagnetic properties of Ba0.70Sr0.30TiO3 thin films

Ba_0.70Sr_0.30TiO₃ (BST) thin films doped by Co (BSTC) are fabricated by sol-gel method on a Pt/Ti/SiO₂/Si substrate. A strong correlation is observed among the microstructure, dielectric, ferroelectric, ferromagnetic properties and Co concentration. The dielectric constant of BST thin films can be tailored from 343 to 119 by manipulating the Co concentration. The dielectric loss of BSTC thin films are still kept below 0.020 and the tunability is above 30% at a dc-applied electric field of 500 kV/cm. With increasing Co doping up to 10 mol%, the coexistence of ferromagnetism and ferroelectrics is found. Suitable dielectric constant, low-dielectric loss, and high tunability of this kind of thin films can be useful for potential tunable applications.     

Influence of substrate temperature on structures and dielectric properties of pyrochlore Bi1.5Zn1.0Nb1.5O7 thin films prepared by pulsed laser deposition

The influence of substrate temperature on structural and dielectric properties of cubic pyrochlore Bi_1.5Zn_1.0Nb_1.5O₇ (BZN) thin films prepared by pulsed laser deposition process has been investigated. BZN thin films were deposited on Pt/Ti/SiO₂/Si(1 0 0) substrate and in situ annealed at 700 °C. The results indicate that the substrate temperature has a significant effect on the structural and dielectric properties of BZN thin films. The films exhibit a cubic pyrochlore structure in the substrate temperature range from 550 °C to 700 °C and at the annealing temperature of 700 °C. With further increase of substrate temperature to 750 °C, the phases of Bi₂O₃, BiNbO₄ and Bi₅Nb₃O₁₅ can be detected in the XRD pattern due to the Zn loss. The dielectric constant and loss tangent of the films deposited at 650 °C are 192 and 6 × 10⁻⁴ at 10 kHz, respectively. The tunability is 10% at a dc bias field of 0.9 MV/cm.     

Microstructure and electrical properties of Ba0.5Sr0.5TiO3 thin films prepared on copper foils with La2O3 buffer layers

Ba_0.5Sr_0.5TiO₃ (BST) thin films were deposited on copper foils via sol-gel method with La₂O₃ as a buffer layer. The films were processed in almost inert atmosphere so that the substrate oxidation was avoided while allowing the perovskite film phase to crystallize. The existence of a La₂O₃ buffer layer between the BST thin film and Cu foil improved the dielectric constant and reduced the leakage current density of the BST thin film. Meanwhile, the BST thin film exhibited ferroelectric character at room temperature, which was contrast to the para-electric behavior of the film without the buffer layer. Effects of La₂O₃ buffer layer on the crystallizability and microstructure of BST thin films were also investigated.     

Microstructure and interfacial properties of HfO2-Al2O3 nanolaminate films

High-k HfO₂-Al₂O₃ composite gate dielectric thin films on Si(1 0 0) have been deposited by means of magnetron sputtering. The microstructure and interfacial characteristics of the HfO₂-Al₂O₃ films have been investigated by using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and spectroscopic ellipsometry (SE). Analysis by XRD has confirmed that an amorphous structure of the HfO₂-Al₂O₃ composite films is maintained up to an annealing temperature of 800 °C, which is much higher than that of pure HfO₂ thin films. FTIR characterization indicates that the growth of the interfacial SiO₂ layer is effectively suppressed when the annealing temperature is as low as 800 °C, which is also confirmed by spectroscopy ellipsometry measurement. These results clearly show that the crystallization temperature of the nanolaminate HfO₂-Al₂O₃ composite films has been increased compared to pure HfO₂ films. Al₂O₃ as a passivation barrier for HfO₂ high-k dielectrics prevents oxygen diffusion and the interfacial layer growth effectively.     

Effect of deposition temperature on orientation and electrical properties of (K0.5Na0.5)NbO3 thin films by pulsed laser deposition

Lead-free ferroelectric K_0.5Na_0.5NbO₃ (KNN) thin films have been prepared on Pt/TiO₂/SiO₂/Si substrates by pulsed laser deposition process. The structures, crystal orientations and electrical properties of thin films have been investigated as a function of deposition temperature from 680 °C to 760 °C. It is found that the deposition temperature plays an important role in the structures, crystal orientations and electrical properties of thin films. The crystallization of thin films improves with increasing deposition temperature. The thin film deposited at 760 °C exhibits strong (0 0 1) preferential orientation, large dielectric constant of 930 and the remnant polarization of 8.54 μC/cm².     

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.     

Dielectric properties of continuous composition spreaded MgO-Ta2O5 thin films

The dielectric properties of MgO-Ta₂O₅ continuous composition spread (CCS) thin films were investigated. The MgO-Ta₂O₅ CCS thin films were deposited on Pt/Ti/SiO₂/Si substrates by off-Axis RF magnetron sputtering system, and then the films were annealed at 350 °C with rapid thermal annealing system in vacuum. The dielectric constant and loss of MgO-Ta₂O₅ CCS thin films were plotted via 1500 micron-step measuring. The specific point of Ta₂O₅-MgO CCS thin film (post annealed at 350 °C) showing superior dielectric properties of high dielectric constant (k ∼ 28) and low dielectric loss (tan δ < 0⋅004) at 1 MHz were found in the area of 3-5 mm apart from Ta₂O₅ side on the substrate. The cation's composition of thin film was Mg:Ta = 0.4:2 at%.     

Synthesis of fine-crystalline Ba0.6Sr0.4TiO3-MgO ceramics by novel hybrid processing route

We report the use of a novel powder-in-sol precursor hybrid processing route to synthesize dense, homogeneous, and fine-crystalline Ba_0.6Sr_0.4TiO₃-MgO (BST-MgO) ceramics as well as the study of the sintering behavior, microstructures, and dielectric properties of the ceramics. Nanosized BST powders are dispersed into BST sol-gel precursor and uniformly distributed BST slurry is obtained after ball-milling mixing. Mg(NO₃)·6H₂O solution is added to the BST slurry to give homogeneous BST-MgO slurry upon ball-milling mixing. The BST-MgO slurry is dried and calcined prior to pressing and sintering at low temperatures of 1200-1300 °C to form the ceramics. The ceramics possess very low dielectric loss tangent below 0.005 for frequency above 1 kHz and for temperature in the range −190-80 °C. The dielectric constant and dielectric tunability increase, while the ferroelectric transition broadening decreases, with increasing average grain size.     

The interfacial structures of (Ba, Sr)TiO3 films deposited by radio frequency magnetron sputtering

Ba_0.6Sr_0.4TiO₃ (BST) films were deposited on Pt/SiO₂/Si substrates by radio frequency magnetron sputtering. The deposited films were crystallized by conventional thermal annealing (CTA) and rapid thermal annealing (RTA). The interfacial structures of BST/Pt were studied. High-resolution transmission electron microscopy (HRTEM) observation shows that there is a transition layer at BST/Pt interface, and the layer is 4-5 nm thick for CTA and 2-3 nm for RTA. X-ray photoelectron spectroscopy (XPS) investigations show that the layer is composed of perovskited BST phase and non-perovskited BST phase. The content of the non-perovskited BST phase is most for CTA, whereas that of the perovskited BST phase is most for RTA. It is found that the transition layer thickens with the increase of annealing temperature, and CTA corresponds to faster thickening rate. XPS shows that the non-perovskited BST phase does not come from the absorbed CO₂ or CO contaminations, but from other interfacial elements. Also, it is indicated that the RTA-annealed BST film capacitor shows much better dielectric properties, with an average value of 150 higher dielectric constant and almost two orders of magnitude lower leakage current density than the CTA-annealed film capacitor. Grazing X-ray diffraction (GXRD) patterns exhibit that the RTA-annealed BST films present more compact structure. It is such a compact structure that can effectively prevent the absorbed elements further diffusing toward two sides, and cause thinner transition layer, thus result in higher dielectric constant and lower leakage current density.     

Correlation between microstructure and optical properties of nano-crystalline TiO2 thin films prepared by sol-gel dip coating

Titanium dioxide thin films have been prepared from tetrabutyl-orthotitanate solution and methanol as a solvent by sol-gel dip coating technique. TiO₂ thin films prepared using a sol-gel process have been analyzed for different annealing temperatures. Structural properties in terms of crystal structure were investigated by Raman spectroscopy. The surface morphology and composition of the films were investigated by atomic force microscopy (AFM). The optical transmittance and reflectance spectra of TiO₂ thin films deposited on silicon substrate were also determined. Spectroscopic ellipsometry study was used to determine the annealing temperature effect on the optical properties and the optical gap of the TiO₂ thin films. The results show that the TiO₂ thin films crystallize in anatase phase between 400 and 800 °C, and into the anatase-rutile phase at 1000 °C, and further into the rutile phase at 1200 °C. We have found that the films consist of titanium dioxide nano-crystals. The AFM surface morphology results indicate that the particle size increases from 5 to 41 nm by increasing the annealing temperature. The TiO₂ thin films have high transparency in the visible range. For annealing temperatures between 1000 and 1400 °C, the transmittance of the films was reduced significantly in the wavelength range of 300-800 nm due to the change of crystallite phase and composition in the films. We have demonstrated as well the decrease of the optical band gap with the increase of the annealing temperature.     

Highly frequency-, temperature-, and bias-stable dielectric properties of 500 °C processed Bi2SiO5 thin films with low dielectric loss

Excellent dielectric frequency, bias, and temperature stability of bismuth silicate (Bi₂SiO₅, BSO) thin films with a low dielectric loss has been obtained in this study. The thin films were prepared on Pt/Ti/SiO₂/Si substrates by a chemical solution deposition method at a relatively low annealing temperature of 500 °C. The BSO films have a preferred growth along (200) orientation with dense fine-grained surface morphology. The dielectric constant and dielectric loss of the thin film annealed at 500 °C are 57 and 0.01, respectively, at 100 kHz, with little change between 1 kHz and 100 kHz and in the bias electric field range between −250 kV/cm and 250 kV/cm, indicating that the thin film exhibits a low dielectric loss as well as excellent frequency and bias field stability. The dielectric-temperature measurements confirmed that the BSO thin film annealed at 500 °C also has good temperature stability between 150 K and 450 K. Our results suggest that the BSO thin films have potential applications in the next-generation integrated capacitors.     

(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     

Low dielectric loss Ba0.6Sr0.4TiO3/MgTiO3 composite thin films prepared by a sol–gel process

The dielectric properties of Ba_0.6Sr_0.4TiO₃ (BST)/MgTiO₃ (MT) composite thin films deposited on Pt(1 1 1)/Ti/SiO₂/Si(1 0 0) substrates by the sol–gel method were investigated. The X-ray pattern analysis indicates that the thin films exhibit good crystalline quality with perovskite phase and that insertion of MT layer does not obviously affect the phase structure of BST thin films. The characterization of dielectric properties demonstrates that configuration of BST/MT/BST thin films is an effective approach to obtain low dielectric loss and dielectric tunability of BST thin films. At room temperature, the tunability of pure BST60 films and BST/MT (15 nm)/BST composite thin films is 47% and 36%, respectively, at the frequency of 1 MHz with an applied electric field of 400 kV/cm. For BST/MT/BST composite thin films, considerable reduction in the dielectric loss values is observed, which renders them attractive for tunable microwave device applications.     

Effect of annealing temperature on microstructure, optical and electrical properties of sputtered Ba0.9Sr0.1TiO3 thin films

Ba_0.9Sr_0.1TiO₃ (BST) thin films were deposited on fused quartz and Pt/TiN/Si₃N₄/Si substrates by radio frequency magnetron sputtering technique. Microstructure and chemical bonding states of the BST films annealed at 700 °C were characterized by field emission scanning electron microscopy, X-ray photoelectron spectroscopy, glancing angle X-ray diffraction and Raman spectrum. Optical constants including refractive indices, extinction coefficients and bandgap energies of the as-deposited BST film and the BST films annealed at 650, 700 and 750 °C, respectively, were determined from transmittance spectra by envelope method and Tauc relation. Dielectric constant and remnant polarization for the BST films increase with increasing annealing temperature. Leakage current density-applied voltage (J–V) data indicate that the dominant conduction mechanism for all the BST capacitors is the interface-controlled Schottky emission under the conditions of 14 V < V < 30 V and −30 V < V < −14 V. Furthermore, the inequipotential J–V characteristics for the BST films annealed at various temperatures are mainly attributed to the combined effects of the different thermal histories, relaxed stresses and strains, and varied Schottky barrier heights in the BST/Pt and Pt/BST interfaces.     

The effect of Si surface nitridation on the interfacial structure and electrical properties of (La2O3)0.5(SiO2)0.5 high-k gate dielectric films

Thermal stability, interfacial structures and electrical properties of amorphous (La₂O₃)_0.5(SiO₂)_0.5 (LSO) films deposited by using pulsed laser deposition (PLD) on Si (1 0 0) and NH₃ nitrided Si (1 0 0) substrates were comparatively investigated. The LSO films keep the amorphous state up to a high annealing temperature of 900 °C. HRTEM observations and XPS analyses showed that the surface nitridation of silicon wafer using NH₃ can result in the formation of the passivation layer, which effectively suppresses the excessive growth of the interfacial layer between LSO film and silicon wafer after high-temperature annealing process. The Pt/LSO/nitrided Si capacitors annealed at high temperature exhibit smaller CET and EOT, a less flatband voltage shift, a negligible hysteresis loop, a smaller equivalent dielectric charge density, and a much lower gate leakage current density as compared with that of the Pt/LSO/Si capacitors without Si surface nitridation.     

Characteristics of sandwich-structured Al2O3/HfO2/Al2O3 gate dielectric films on ultra-thin silicon-on-insulator substrates

Sandwich-structure Al₂O₃/HfO₂/Al₂O₃ gate dielectric films were grown on ultra-thin silicon-on-insulator (SOI) substrates by vacuum electron beam evaporation (EB-PVD) method. AFM and TEM observations showed that the films remained amorphous even after post-annealing treatment at 950 °C with smooth surface and clean silicon interface. EDX- and XPS-analysis results revealed no silicate or silicide at the silicon interface. The equivalent oxide thickness was 3 nm and the dielectric constant was around 7.2, as determined by electrical measurements. A fixed charge density of 3 × 10¹⁰ cm⁻² and a leakage current of 5 × 10⁻⁷A/cm² at 2 V gate bias were achieved for Au/gate stack /Si/SiO₂/Si/Au MIS capacitors. Post-annealing treatment was found to effectively reduce trap density, but increase in annealing temperature did not made any significant difference in the electrical performance.     

Influence of temperature annealing on optical properties of SrTiO3/BaTiO3 multilayered films on indium tin oxide

We have prepared SrTiO₃/BaTiO₃ thin films with multilayered structures deposited on indium tin oxide (ITO) coated glass by a sol-gel deposition and heating at 300-650 °C. The optical properties were obtained by UV-vis spectroscopy. The films show a high transmittance (approximately 85%) in the visible region. The optical band gap of the films is tunable in the 3.64-4.19 eV range by varying the annealing temperature. An abrupt decrease towards the bulk band gap value is observed at annealing temperatures above 600 °C. The multilayered film annealed at 650 ° C exhibited the maximum refractive index of 2.09-1.91 in the 450-750 nm wavelength range. The XRD and AFM results indicate that the films annealed above 600 ° C are substantially more crystalline than the films prepared at lower temperatures which were used to change their optical band gap and complex refractive index to an extent that depended on the annealing temperature.     

Annealing effects on microstructural and optical properties of Nanostructured-TiO2 thin films prepared by sol-gel technique

In this paper we report on the effect of annealing on the microsctructural and optoelectronic properties of titanium dioxide (TiO₂) thin films prepared using sol-gel method onto silicon (Si) (100) and quartz substrates. The annealing temperatures range from 200 to 1000 °C. The Microstructural properties of annealed thin films were investigated by Thermal gravimetric analyses (TGA), X-ray diffraction (XRD) and Raman Spectroscopy. The surface morphology of the film was examined using Atomic Force Microscopy (AFM) method. The optical properties of TiO₂ thin films were characterized using UV-VIS and Spectroscopic ellipsometry. The results have shown that the TiO₂ thin films persist in the anatase phase even after annealing at 800 °C. The phase transformation from anatase to rutile occurred only when the films were annealed at 1000 °C. AFM studies revealed nanocrystalline structure where their shape and density depend strongly on the annealing temperatures. The elaborated nanostructured-TiO₂ thin films present a high transparency in the visible range. Spectroscopic ellipsometry (SE) study was used to determine the effect of annealing temperature on the thickness and on the optical constant of TiO₂ thin films. Spectroscopic ellipsometry and UV-VIS shows that the band gap of TiO₂ thin films was found to decrease when the annealing temperature increases. The Anatase phase was find to show higher photocatalytic activity than the rutile one.     

The preparation and refractive index of BST thin films

Radio-frequency magnetron sputtering technique is used to deposit Ba_0.65Sr_0.35TiO₃ (BST) thin films on fused quartz substrates. In order to prepare the high-quality BST thin films, the crystallization and microstructure of the films were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM) and atomic force microscopy (AFM). More intense characteristic diffraction peaks and better crystallization can be observed in BST thin films deposited at 600 °C and subsequently annealed at 700 °C. The refractive index of the films is determined from the measured transmission spectra. The dependences of the refractive index on the deposition parameters of BST thin films are different. The refractive index of the films increases with the substrate temperature. At lower sputtering pressure, the refractive index increases from 1.797 to 2.197 with pressure increase. However, when the pressure increases up to 3.9 Pa, the refractive index reduces to 1.86. The oxygen to argon ratio also plays an important effect on the refractive index of the films. It has been found that the refractive index increases with increase in the ratio of oxygen to argon. The refractive index of BST thin films is strongly dependent on the annealing temperature, which also increases as the annealing temperature ascends. In a word, the refractive index of BST thin films is finally affected by the films’ microstructure and texture.