The Dielectric Properties for Yttrium Doped SBT Thin Films Prepared by Sol-Gel Method

In this work, Sr_0.5Ba_0.5Ti_1-zY_zO₃ (SBT) thin films were prepared on a Pt/SiO₂/Si substrate by sol-gel process. The microstructures of SBT thin films were examined by IR, XRD and TEM. The influences of Y on the microstructure and dielectric properties of Sr_0.5Ba_0.5Ti_1-zY_zO₃ thin films were studied. It is found that tetragonal perovskite crystal grains existed in SBT thin films. Increasing Y doping has a clear effect on the grain size of SBT. It is found that the proper Y doping content decreases dielectric loss for SBT thin films.     

Fabrication and characterization of Au/SBT/LZO/Si MFIS structure

Ferroelectric SrBi₂Ta₂O₉ (SBT) films on a p-type Si (100) wafer with a LaZrO _x (LZO) buffer layer have been fabricated to form a metal-ferroelectric-insulator–semiconductor (MFIS) structure. The LZO thin film and SBT films were deposited by using a sol–gel method. The equivalent oxide thickness (EOT) value of the LZO thin film was about 8.83 nm. Also, the leakage current density of the LZO thin film is about 3.3?×?10^?5 A/cm² at bias sweeping voltage of ±5 V. SBT films were crystallized in polycrystalline phase with highly preferred (115) orientation. Also, the intensity of each pick slightly increased as thickness of SBT films increased. The C–V characteristics of Au/SBT/LZO/Si structure showed clockwise hysteresis loop. The memory window width increased as the thickness of SBT films increased. The leakage current density of Au/SBT/LZO/Si structure decreased as thickness of SBT films increased.     

Preparation of SrBi2Ta2O9 ferroelectric thin film by rf magnetron sputtering

Abstract

SrBi₂Ta₂O₉ (SBT) thin films were deposited on 6-inch Pt/Ti/SiO₂/Si substrates by rf magnetron sputtering using a 12-inch ceramic SBT single target. It is found that several sputtering parameters such as argon (Ar) pressure and rf power were very effective to control the Bi content of SBT thin films which is essential for obtaining good ferroelectric properties.     

Characterization of the CeO2 thin films for insulation layer and Pt/SrBi2Ta2O9/CeO2/Si MFISFET structure

Abstract

CeO₂ and SrBi₂Ta₂O₉ (SBT) thin films for MFISFET (metal-fcrroelectrics-insulator-semiconductor field effect transistor) were deposited by rf sputtering and pulsed laser deposition method, respectively. The effects of oxygen partial pressure during deposition for CeO₂ films were investigated. The oxygen partial pressure significantly affected the preferred orientation, grain size and electrical properties of CeO₂ films. The CeO₂ thin films with a (200) preferred orientation were deposited on Si(100) substrates at 600°C. The films deposited under the oxygen partial pressure of 50 % showed the best C-V characteristics among those under various conditions. The leakage current density of films showed order of the 10^?7～10^?8 A/cm² at 100 kV/cm. The SBT thin films on CeO₂/Si substrate showed dense microstructure of polycrystalline phase. From the C-V characteristics of MFIS structure composed of the SBT film annealed at 800°C, the memory window width was 0.9 V at ±5 V. The leakage current density of Pt/SBT/CeO₂/Si structure annealed at 800°C was 4×10^?7 A/cm² at 5 V.     

Effects of Substrate and Annealing Temperatures on the Characteristics of SrBi4Ti4O15 Thin Films

In this study, radio frequency (RF) sputtering was used as the method and the layer-structured bismuth compound of SrBi₄Ti₄O₁₅ + 4 wt% Bi₂O₃ ferroelectric ceramic was used as the target to deposit the SrBi₄Ti₄O₁₅ (SBT) thin films. The addition of excess Bi₂O₃ content in the target ceramic was used to compensate the vaporization of Bi₂O₃ during the sintering and deposition processes. SBT ferroelectric thin films were deposited on Pt/Ti/SiO₂/Si under optimal RF magnetron sputtering parameters with different substrate temperatures for 2 h. After that the SBT thin films were post-heated using rapid temperature annealing (RTA) method. The dielectric and electrical characteristics of the SBT thin films were measured using metal-ferroelectric-metal (MFM) structure. From the physical and electrical measurements of X-ray diffraction pattern, scanning electronic microscope (SEM), I-V curve, and C-V curve, we had found that the substrate temperature and RTA-treated temperature had large influences on the morphology, the crystalline structure, the leakage current density, and the dielectric constant of the SBT thin films.     

Fabrication of MFIS diodes using sol-gel derived SBT films and LaAlO3 buffer layers

Abstract

We demonstrate the ferroelectric behavior of Sr_0.8Bi_2.2Ta₂O₉ (SBT) films grown on Si(100) substrates by using lanthanum aluminate (LaAlO₃) buffer layers. LaAlO₃ films were prepared by vacuum evaporation method. Then, they were subjected to ex situ dry N₂ annealing in a rapid thermal annealing (RTA) furnace. From the capacitance-voltage (C-V) measurement, the dielectric constant of LaAlO₃ was estimated to be 20～25. On these substrates, SBT films (210nm) were deposited by sol-gel method and they were characterized by XRD analysis after annealing under various conditions. It was found from C-V characteristics that the memory window of an SBT film annealed at 750°C for 30min in O₂ atmosphere was about 3.0V for the voltage sweep of ±10V. It was also found from the retention measurement that the capacitance values of the SBT film annealed at 750°C did not change over 12hours. It is concluded from these results that the SBT/LaAlO₃/Si(100) structure is one of the most promising structures for realizing MFISFETs (metal-ferroelectric-insulator-semiconductor field-effect-transistors).     

Preparation of Si-Added SrBi2Ta2O9 Ferroelectric Thin Films by RF Magnetron Sputtering

Si-added SrBi₂Ta₂O₉ (SBT) ferroelectric films were prepared by RF magnetron sputtering on a Pt/Ti/SiO₂/Si (100) structure. The films were deposited at temperatures below 100°C for surpressing Bi evaporation, and crystallized at 800°C in air. A typical composition was Sr_0.79Bi_2.37Ta_2.00Si_0.2O_x. The remanent polarization value (2Pr) of the Si-added SBT film was 16 μC/cm². The Si atom addition was found to be effective in improvement of the fatigue and leakage current of SBT ferroelectric films. The leakage current density was further improved by annealing in the high-pressure oxygen ambient at 7 atms.     

Degradation mechanisms of SrBi2Ta2O9 ferroelectric thin film capacitors during forming gas annealing

Abstract

The effects of annealing in forming gas (5% hydrogen, 95% nitrogen; FGA) are studied on spin coated SrBi₂Ta₂O₉ (SBT) thin films. SBT films on platinum bottom electrode are characterized with and without platinum top electrode by Scanning Electron Microscopy (SEM), Auger Electron Spectroscopy (AES), High Temperature X-Ray Diffraction (HT-XRD) and Secondary Ion Mass Spectrometry (SIMS).

High Temperature X-Ray Diffraction (HT-XRD) of blanket Ti/Pt/SBT films in forming gas revealed that the bismuth layered perovskite structure of the SBT is stable up to approx. 500°C. SIMS analysis of Pt/SBT/Pt samples annealed in deuterated forming gas (5% D₂, 95% N₂) showed that the hydrogen accumulates in the SBT layer and at the platinum interfaces next to the SBT. After FGA of blanket SBT films, tall platinum-bismuth whiskers are seen on the SBT surface.

Performing the FGA of the whole Pt/SBT/Pt/Ti stack, two different results are found. For the samples with a high temperature annealing (HTA) step in oxygen after top electrode patterning, top electrode peeling is observed after FGA. For the samples without a HTA step after top electrode patterning, no peeling is observed after FGA.     

Low temperature preparation of ferroelectric SrBi2Ta2O9 thin films by a modified RF magnetron sputtering technique

Abstract

Bi–layered ferroelectric SrBi₂Ta₂O₉ (SBT) films were successfully prepared on Pt/Ti/SiO₂/Si substrates at 650°C by a modified rf magnetron sputtering technique. The SBT films annealed for 1 h in O₂ (760 torr) and again for 30 min in O₂ (5 torr) at 650°C show a average grain size of about 49 nm. The SBT films annealed at 65 0°C have a remanent polarization (P_r) of 6.0 μC/cm² and coercive field (E_c) of 36 kV/cm at an excitation voltage of 5 V. The films showed fatigue–free characteristics up to 4.0 × 10¹⁰ switching cycles under 5 V bipolar pulse. The retention characteristics of SBT films looked very promosing up to 1.0 × 10⁵ s.     

Atomic-scale microstructures of SrBi2Ta2O9 (SBT) ferroelectric thin films prepared by MOD and PLD for ferams applications

Abstract

In this work, the microstructural defects in SrBi₂Ta₂O₉ (SBT) ferroelectric thin films were investigated at the atomic-scale by high-resolution transmission electron microscopy (HRTEM). A stacking fault with an extra inserted Bi-O plane normal to the c-axis was observed in SBT film with 10mol% excess bismuth prepared by metalorganic deposition. Edge dislocations with an average space about 3nm were observed at the small misorientation angle (8.2°) tilt grain boundary of SBT film with (001)-orientation prepared by pulsed laser deposition. The Burgers vector b for the edge dislocation was determined to be 1/2[110]α₀, where α₀ is the parameter of SBT unit cell. Chemical compositions of grains and grain boundaries in SBT films annealed in forming gas at 450°C and 500°C for 60 minutes were analyzed by using energy dispersive spectra at the nano-scale. Effects of the microstructural defects and microchemistry of the grain boundaries on the leakage current of SBT films are briefly discussed.     

Electrical and memory window properties of Sr0.8-xBaxBi2.2Ta2-yZryO9 ferroelectric gate in metal-ferroelectric-insulator-semiconductor structure

Electrical characteristics of Sr_0.8-xBa_xBi_2.2Ta_2-yZr_yO₉ ferroelectric films grown on HfO₂/Si wafers by sol–gel spin coating technique were investigated from the viewpoint of application as ferroelectric gates in metal-ferroelectric-insulator-semiconductor (MFIS) stacks. It was observed that the leakage current density level was 10^-8 A/cm² under 14?V for moderate doping ratio. Determined memory windows from C-V characteristics of Sr_0.8Bi_2.2Ta₂O₉ (SBT) and Sr_0.8-xBa_xBi_2.2Ta_2-yZr_yO₉ (x?=?0.04, 0.08, 0.12 and y?=?0.1, 0.2, 0.3) are 0.59, 0.65, 0.75, and 0.86?V at gate sweeping bias of 5?V, respectively. Some part of electronic properties of Sr_0.8-xBa_xBi_2.2Ta_2-yZr_yO₉ with the objective to enhance memory window up to 45?% were discussed. It was interpreted that defects which are formed in Ba and Zr modified SBT affected the electronic processes like leakage current, memory window and charge trapping.     

In situ formation of sol-gel derived PbTiO3/NiFe2O4 biphase thin film

In this article, magnetoelectric (ME) biphase composite thin films consisted of PbTiO₃ as ferroelectric phase and NiFe₂O₄ as ferromagnetic phase which were successfully formed in situ by sol-gel process. The phase structure, morphology and dielectric properties of the films were measured by X-ray diffraction (XRD), scanning electron microscope (SEM) and LCR precision impedance analyzer. It is concluded that the thin films were capable of being controlled to form the biphase composite of PbTiO₃ and NiFe₂O₄ at the heat-treatment temperature between 600 and 850 °C. The phases coexisting in the composite thin film are in forms of solid solutions doped with Ni²⁺ and Fe³⁺ and with Ti⁴⁺, respectively. Their lattice constants vary with their doping contents. The capacitance of the composite thin film depends on the content of perovskite phase and the doping addition of Ni²⁺ and Fe³⁺ in crystalline phase of PbTiO₃.     

The Enhanced Dielectric and Insulating Properties of Al2O3 Modified Ta2O5 Thin Films

Future-generation memory devices will require materials with higher dielectric constants compared to conventional dielectric materials such as silicon oxide and silicon nitride. Tantalum oxide (Ta₂O₅) is one of the most promising high dielectric constant materials because of its ease of integration into conventional VLSI processes compared to other complex oxide dielectrics. The dielectric constant and thermal stability characteristics of bulk Ta₂O₅ samples were previously reported to enhance significantly through small substitutions of Al₂O₃. However, this improvement in the dielectric constant of (1 – x)Ta₂O₅-xAl₂O₃ was not clearly understood. The present research attempts to explain the higher dielectric constant of (1 – x)Ta₂O₅-xAl₂O₃ by fabricating thin films with enhanced dielectric properties. A higher dielectric constant of 42.8 was obtained for 0.9Ta₂O₅-0.1Al₂O₃ thin films compared to that reported for pure Ta₂O₅ (25–30). This increase was shown to be closely related to a-axis orientation. Pure Ta₂O₅ thin films with similar a-axis orientation also exhibited a high dielectric constant of 51.7, thus confirming the orientation effect. Systematic study of dielectric and insulating properties of (1 – x)Ta₂O₅-xAl₂O₃ thin films indicate improved leakage current properties and reliability characteristics such as temperature coefficient of capacitance and bias stability with increase in Al₂O₃ concentrations.     

Phase transition and electrical studies of wolframium doped SrBi2Ta2O9 ferroelectric ceramics

In this study, crystalline structure, dielectric and impedance properties of SrBi₂Ta₂O₉ (SBT) - based ferroelectric ceramics have been investigated with the substitution of wolframium/tungsten (W) onto the tantalum site. Wolframium doped SrBi₂(W _x Ta_{1 − x} )₂O₉ (0.0 ≤ x ≤ 0.20) ceramics were synthesized by solid state reaction method. The X-ray diffractogram analysis revealed that the substitution formed a single phase layered perovskite structure for the doping content up to x ≤ 0.05. The dielectric measurements as a function of temperature show an increase in Curie temperature (T _c ) over the composition range of x = 0.05 to 0.20. The W^{6 +} substitution in perovskite-like units results in a sharp dielectric anomaly at the ferroelectric phase transition. Furthermore, the dielectric constant at their respective Curie temperature increases with wolframium doping. Both enhanced Curie temperatures and dielectric constants at the Curie points indicate an increase in polarizability, which could be attributed to the increased “rattling space” due to the incorporation of the smaller tungsten cations. The dielectric loss reduces significantly with tungsten addition. AC impedance properties vis-à-vis wolframium content has also been studied.     

Forming gas annealing effects on the microstructure and ferroelectricity of SrBi2Ta2O9 thin films prepared by metalorganic decomposition

Abstract

Ferroelectric SrBi₂Ta₂O₉(SBT) thin films prepared by metalorganic decomposition (MOD) method were annealed in forming gas (5% hydrogen + 95% nitrogen) at different temperatures for 60 min. SEM analysis results showed that an amount of columnar structures appeared on SBT surface when the annealing temperature was up to 450°C. When the annealing temperature raised up to 500°C, these columnar structures grew along one dimension and changed into wire structures. The EDX micro-area mapping analysis result showed that Bi was concentrated in the columnar or wire structures on SBT surface. The ferroelectric property analysis results showed that the hysteresis loops still existed after 5 min forming gas processing (350°C or 400°C), but when the annealing time was longer than 10 min, the resistance of the SBT samples became too low to measure the hysteresis loops.     

Preparation and Ferroelectric Properties of K0.5Na0.5NbO3 Thin Films Derived from Non-alcohol Niobium Salt Sol-gel Process

Lead-free K_0.5Na_0.5NbO₃ (KNN) thin films were prepared on Pt (111) /Ti/SiO₂/Si (100) substrates by a polyvinylpyrrolidone (PVP)-modified sol-gel method without any metal alkoxides. The effects of PVP on the crystallization, surface morphology and electrical properties were investigated. It was found that the introduction of PVP into the sol could reduce the annealing temperature, enhance the surface quality and improve the KNN film of (100) oriented growth. Compared with the pure non-PVP-modified KNN thin films, the dielectric and ferroelectric properties of the KNN films were significantly enhanced by adding PVP into the sol. In particular, the PVP-modified KNN films which were annealed at 550°C exhibited relatively saturated polarization-electric field (P-E) hysteresis loops with high remnant polarization P_r of 22 μC/cm², dielectric constant of 280 and dielectric loss of 0.09, respectively, indicating promising lead-free piezoelectric film candidate for future applications.     

Strong thickness dependence of aurivillius phase formation in SrBi2Ta2O9 thin films

Sr_0.7Bi_2.4Ta₂O₉ (SBT) thin films were studied for the dependence of Aurivillius phase formation kinetics on their film thickness. SBT thin films were fabricated using a sol-gel process and spin coating, and their thickness was varied controlling the number of spin coating. The films were first heated at a low temperature for the complete crystallization of amorphous film to fluorite phase and then further heated at different elevated temperatures for the phase transformation to Aurivillius for 40 min. It was found that the phase transformation kinetics apparently increased with thickness up to ∼390 nm, and then it sharply decreased at higher values. The Aurivillius crystal size decreased and the density of crystals increased with the increase of film thickness up to ∼390 nm, implying increasing number of nuclei due to the reduced energy barrier for nucleation. Above the critical value both the size and density of crystals decreased. It is suggested that up to ∼390 nm the tensile strain energy in the films, which was stored by the shrinkage of thin films during the removal of remaining organic components from sol-gel chemistry, plays a major role for determining the phase transformation kinetics and above the critical value SBT films act as a free bulk material without substrate constraints.     

Growth and characterization of epitaxial SrBi2Ta2O9 films on (110) SrTiO3 substrates

Abstract

SrBi₂Ta₂O₉ (SBT) is an attractive material for nonvolatile ferroelectric memory applications. In this paper we report on the deposition of highly epitaxial and smooth SrBi₂Ta₂O₉ films on (110) SrTiO₃substrates. The films were grown by pulsed laser deposition at temperatures ranging from 600 to 800°C and at various laser fluences from a Bi-excess SBT target. The background oxygen pressure was maintained at 28 Pa during the film deposition. Structural characterization of the films was performed by x-ray diffraction. Atomic force microscopy was used to investigate morphology and growth of the films. The films grew with preferred (115) or (116) orientation. The roughness was of the order of unit cell height. The films display a growth pattern resulting in corrugated film morphology.     

Effects of bi2o3 buffer layer on ferroelectric properties of srbi2ta2o9 thin films by liquid-delivery mocvd

Abstract

Ferroelectric SrBi₂Ta₂O₉ thin films were deposited on the Bi₂O₃ buffered Pt/Ti/SiO₂/Si substrates using liquid-delivery metalorganic chemical vapor deposition. SBT films with 5nm thick-Bi₂O₃ buffer layer on Pt bottom electrode showed stronger (115) orientation than those without Bi₂O₃ buffer layer after annealing at 750°C. The value of the remanent polarization of SBT films with Bi₂O₃ buffer layer were improved significantly in comparison with those for the films without Bi₂O₃ buffer layer. The remanent polarization(2Pr) and coercive field(Ec) of SBT films without and with Bi₂O₃buffer layer annealed at 750°C were 11.9, 20.8 μ C/cm2 and 57, 37.8kV/cm at an applied voltage of 5 V, respectively.     

Improvement in the electrical properties of ferroelectric SrBi2Ta2O9 capacitors by electron beam irradiation on precursor films

Abstract

Ferroelectric SrBi₂Ta₂O₉ (SBT) capacitors were fabricated by the Electron-Beam-Induced Patterning process and their electrical properties were evaluated in detail. In this process, the dose of an electron beam irradiated on precursor films had a great influence on the electrical properties of the SBT capacitors. The appropriate electron dose significantly improved the electrical properties of the SBT capacitors although the excess electron dose made severe deterioration in the properties. The SBT capacitors fabricated with the optimum electron dose, 1.5 mC/cm² for Sr:Bi:Ta = 0.8:2.2:2.0 solutions, exhibited excellent ferroelectric properties: a remanent polarization of 11.5 μC/cm², a coercive field of 40 kV/cm, a leakage current of 8×10^?8 A/cm²@ 1V and fatigue-free up to 1010 cycles. It seems that such improvements were caused by the adjustment of Bi contents in the films and the modification or the decompositon of precursors before heat treatment by electron beam irradiation.