Enhancement of ferroelectricity in gadolinium (Gd) and transition metal (Ni, Co, Cr) Co-doped BiFeO3 thin films via a chemical solution deposition technique

The BiFeO₃ (BFO) and the gadolinium and transition metal ions co-doped (Bi_0.9Gd_0.1)(Fe_0.975 TM _0.025)O_3-δ (TM?=?Ni, Co and Cr, BGFNi, BGFCo and BGFCr) thin films were prepared on Pt(111)/Ti/SiO₂/Si(100) substrates by using a chemical solution deposition method. Compared to the pure BFO, improved electrical and ferroelectric properties were observed in the co-doped (Bi_0.9Gd_0.1)(Fe_0.975 TM _0.025)O_3-δ thin films. Among the thin films, the BGFCr thin film exhibited large remnant polarization (2P _r ), low coercive field (2E _c ), and reduced leakage current density, which are 136 μC/cm², 1360 kV/cm at 1470 kV/cm, and 5.14?×?10^-6 A/cm² at 100 kV/cm, respectively.     

Structural and improved electrical properties of rare earth (Sm, Tb and Ho) doped BiFe0.975Mn0.025O3 thin films

Pure BiFeO₃ (BFO) and rare earth (RE) ion co-doped (Bi_0.9RE_0.1)(Fe_0.975Mn_0.025)O₃ (RE?=?Sm, Tb and Ho, denoted by BSFM, BTFM and BHFM) thin films were prepared on Pt(111)/Ti/SiO₂/Si(100) substrates by using a chemical solution deposition method. Formations of distorted rhombohedral perovskite structure for the thin films were confirmed by using an X-ray diffraction and a Raman scattering analysis. Microstructural features for the thin films were examined by using a scanning electron microscopic analysis. Among the thin films, the lowest leakage current density of 1.22?×?10^?6 A/cm² (at 100 kV/cm), large remnant polarization (2Pr) of 72.4 μC/cm² and low coercive field (2E _c ) of 689 kV/cm (at 980 kV/cm) were measured for the BTFM thin film.     

DC conduction behavior of Bi3.15Nd0.85Ti3O12 thin films grown by RF-magnetron sputtering

The Bi_3.15Nd_0.85Ti₃O₁₂ (BNT) thin films were deposited on Pt(111)/Ti/SiO₂/Si substrates by using RF-magnetron sputtering method and studied the ferroelectric and leakage current charateristics. The polarization – electric field (P-E) hysteresis loops of BNT film was well saturated with the remnant polarization (2P _r ) of 29.8 μC/cm² and a coercive field (2E _c ) of 121 kV/cm. The leakage current density – electric field (J-E) characteristics of the Pt/BNT/Pt capacitor reveals the presence of two conduction region, having Ohmic behavior at low electric field (below 50 kV/cm) and Schottky-emission or Poole-Frenkel emission at high electric field (above 60 kV/cm). The barrier height and trapped level of BNT films are estimated to be 1.11 eV and 0.90 eV, respectively.     

Fabrication and characteristics of PZT thick films on Pt/Ti foil substrates for piezoelectric vibrators

Crack free perovskite PbZr_0.53Ti_0.47O₃ (PZT (53/47)) thick films up to 30 μm were prepared on flexible platinum-coated titanium foil substrates (Pt/Ti) by a metal organic decomposition (MOD) process. The dielectric, ferroelectric and piezoelectric properties of the films were examined and discussed. A well-saturated hysteresis loop of the thick film was present in almost rectangular shape (Pr?=?35 μC/cm²; Ec?=?32 kV/cm). The efficient piezoelectric coefficient d _{33, f} of the thick film is about 448 (1 kHz). PZT piezoelectric vibrators were made in bimorph mode. The displacements of the vibrators were investigated as the functions of the applied electric field and the substrate thickness. Under the same condition, the vibrator made from the thinnest Pt/Ti substrate gives the largest displacement.     

Characterization of PT ferroelectric thin films on porous silica for pyroelectric IR detectors

Ferroelectric PbTiO₃ thin films were deposited on Pt/DS/PS/SiO₂/Si substrates by sol–gel technique. Porous silica (PS) thin film was used as thermal-insulation layer and dense silica (DS) thin film was a buffer layer to reduce surface roughness of PS layer. Root mean square surface roughness can be effectively reduced from 9.7 to 3.5 nm after PS buffer layer was prepared. The average grain size of PT thin films decreased slightly with increasing thickness of porous silica. Dielectric constant of PT increased from 107 to 171 at 1 KHz as thickness of PS layer increased from 0 to 2,000 nm. PT thin film prepared on 2,000 nm porous silica exhibited good dielectric property. The leakage current density was less than 1.6?×?10^-6 A/cm² when the applied electrical field was 200 kV/cm. The composite film is suitable for preparing pyroelectric IR detectors.     

PATTERNED HIGH FREQUENCY THICK FILM MEMS TRANSDUCER

ABSTRACT

Ferroelectric properties of BiFeO₃ (BFO) thin films epitaxially grown on SrRuO₃ (SRO)/(001)SrTiO₃ (STO) structure were investigated. First, bottom SRO electrodes were deposited on STO substrates by metalorganic chemical vapor deposition (MOCVD) or by sputtering. Then, BFO thin films were deposited on SRO/STO structures by chemical solution deposition. X-ray diffraction analysis showed that the SRO films deposited by both methods grew epitaxially on STO substrates as a single phase perovskite structure, but the out-of-plane lattice parameters of SRO were different, that is, they were 0.396 nm in MOCVD and 0.399 nm in sputtering. The leakage current densities were higher than 1 A/cm² at room temperature in BFO films on both MOCVD-and sputtered-SRO, but the current density in the film on sputtered SRO decreased to 2 × 10^?4 A/cm² at 80 K. The remanent polarization of approximately 50 μC/cm² was observed at 80 K in the BFO thin film on sputtered-SRO/STO.     

Preparation of TiO<Subscript>2</Subscript> thin films deposited from highly dense targets with multi-oxide glass doping

Glass doped TiO₂ (GTO) thin films were deposited by radio frequency (RF) magnetron sputter at room temperature and annealed in a reductive atmosphere containing 90 % N₂ and 10 % H₂. Highly dense TiO₂ ceramic mixed with glass consisting of multi-metal oxides (as a sintering aid) was used as the sputtering target. This sintering aid allows low temperature densification of TiO₂ target through a liquid phase wetting mechanism, and also works as a doping resource. XRD and FESEM were carried out to characterize the microstructure of the GTO films and the results reveal that the doping of multi-metal ions enhances the crystallization and increases the grain size of TiO₂ films. TEM analysis also showed that these metal ions were dissolved into TiO₂ lattices. The electrical and optical properties of TiO₂ thin films at different glass concentrations were evaluated and compared to the films merely doped with MoO₃. The electrical resistivity of the GTO films reaches 9.1 × 10^–4 Ω·cm at 2 wt% glass doping, corresponding to a carrier density of 8.9 x 10²⁰ cm^-3 and a mobility of 7.1 cm²/Vs. Meanwhile, the electrical resistivity of the TiO₂ film doped with glass was found to be lower than that of MoO₃-doped film. This was mainly attributed to the increase in carrier concentration by double doping effect of glass. The optical band gap of the GTO films ranged from 3.34 to 3.42 eV, which is greater than that of the un-doped TiO₂ film. This blue shift of approximately 0.18 eV was due to the Burstein-Moss effect.     

Enhanced ferroelectric properties of multilayer SBT-BTN thin films for NVRAM applications

Ferroelectric SrBi₂Ta₂O₉ – (Bi₄Ti₃)_1-xNb_xO₁₂ (SBT-BTN) multilayer thin films with various stacking periodicity have been synthesized on Ir/Ti/SiO₂/Si substrates by metal organic chemical vapor deposition technique (MOCVD). Tributylbismuth [Bi(C₄H₉)₃], strontium-bis[tantal(pentane-ethoxy)(2-methoxyethoxide)] [Sr[Ta(OEt)₅(OC₂H₄OMe)]₂], titanium bis(isopropoxy)bis(1-methoxy-2-methyl-2-propoxide) [Ti(OiPr)₂(mmp)₂] and niobium-ethoxide [Nb(OC₂H₅)₅] were selected as precursors. X-ray diffraction patterns show that the multilayer films annealed at 800°C consisted of a fully formed perovskite phase with polycrystalline structure. The remanent polarization (2·P_r) and coercive field strength (E_c) were 16.2 μC/cm² and 230 kV/cm, respectively, values which are much higher compared to pure SBT film (2·P_r = 6.4 μC/cm², E_c = 154 kV/cm).     

The Study of Ferroelectric La-Doped PbTiO3 Thin Films Prepared by RF Magnetron Sputtering

Ferroelectric La-modified lead titanate (PLT) thin film were grown on Pt/Ti/SiO2/Si by sputtering the Pb_0.93La_0.07TiO₃ targets containing an amounts of excess 8% PbO. The effects of sputtering and annealing conditions on the crystalline structures and the surface morphologies of the PLT thin films have been investigated. The remanent polarization (Pr) and the coercive field of the PLT film through rapid thermal annealing (RTA) was 10.2 μC/cm² and 45 kV/cm respectively. The maximum pyroelectric coefficient reached 19 nC/cm².K at 20°C.     

Dielectric and Ferroelectric Properties of Ba(Zr0.35Ti0.65)O3 Thin Films Grown by a Sol-Gel Process

The Ba(Zr_0.35Ti_0.65)O₃ (BZT) thin films were deposited via sol-gel process on LaNiO₃-coated silicon substrates. XRD showed that the crystallinity of BZT film grown on LaNiO₃ coated silicon substrates is better than that of BZT film grown on Pt. Both films showed perovskite phase and polycrystalline structure. The temperature dependent dielectric measurements revealed that the thin films had the relaxor behavior and diffuse phase transition characteristics. The capacitor tuning was about 44% for each BZT film grown on LaNiO₃/Pt and Pt electrodes at 1 MHz. Especially, the values of dielectric loss at 1 MHz ranged from 0.02 to 0.009 in the bias range of 0 to 514 kV/cm, respectively. The leakage currents density of thin films grown on LaNiO₃/Pt and Pt electrodes at 300 kV/cm was about 8.5 × 10^–7 and 1.1 × 10^–5 A/cm², respectively. This work demonstrates a potential use of BZT films for application in tunable microwave devices.     

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.     

Micro-structure and ferroelectric properties of BiFeO3 thin films formed on Pt-coated r-plane sapphire substrates

Magnetoelectric BiFeO₃ (BFO) materials exhibit ferroelectric and ferromagnetic properties simultaneously, therefore they have a potential to be applied in magnetic as well as ferroelectric devices. BFO thin films were formed by depositing sol-gel solutions on Pt-coated r-plane sapphire dielectric substrates. We did not observe any secondary phase such as Bi₂Fe₄O₉ on the r-plane sapphire substrates, which is generally observed on Si substrates. We observed small ferroelectric grains of about 0.1 μm on Pt/sapphire structures. The leakage current density in BFO films was found to be decreased dramatically after optimizing process conditions of stoichiometric BFO chemical solution. The leakage current densities were in the range of 10^{− 7} A/cm² at room temperature and 10^{− 9} A/cm² at 80 K under 0.4 MV/cm applied electric field. The main reason for low leakage current is considered to be reduction of oxygen vacancies due to the presence of exclusive Fe^{3 +} valance state in the films. An applied electric field higher than 0.5 MV/cm was required to pole the BFO films, which made it difficult to obtain the saturated polarization at room temperature. We could measure the saturated remanent polarization in the BFO films at 80 K and the obtained remanent polarization was 100 μC/cm².     

Design and implementation of combline bandpass tunable filter using barium-strontium-titanate thin-film capacitors

The design, fabrication and microwave properties of tunable fifth-order combline bandpass filter using etched barium-strontium-titanate (BST) thin films on sapphire (0001) substrates were investigated. At 1 MHz and 1000 kV/cm electric field, the dielectric tunability, the remanent polarization (2P_r) and the coercive electric field (2E_C) of BST films were 45.96%, 2.26 µC/cm² and 81.83 kV/cm, respectively. The loss tangent was 1.36% at zero electric field. After the BST parallel plate capacitors characterization, BST capacitors were loaded at the end of parallel coupled resonators in the design of the tunable filter. With the application of 20 V DC voltage, the center frequency of the filter varied from 1.17 GHz to 1.34 GHz which corresponds to a relative shift of 13.5%.     

Structure and Properties of Preferential (110) Orientation BiFeO3 Thin Films by Sol-Gel Method

Abstract

Multiferroic materials, coexisting of ferroelectric, ferromagnetic and ferroelastic properties, possess potential applications in functional devices. BiFeO₃ (BFO) is a unique room temperature multiferroic material with high ferroelectric Curie temperature and Neel temperature. The BFO thin films were prepared on Si (111) substrate by sol-gel method in this paper. XRD analyses show that the thin films exhibit pure phase and preferred (100) orientation when annealing temperature is 500?°C. Field emission scanning electron microscopy shows that the crystallization degree of the films is getting better with the increase of annealing temperature. The thickness of the sample is about 400?nm. The hysteresis loop of BFO films annealing at 500?°C show 1.93?µC/cm² remnant polarizations. However, the hysteresis loop is not perfect, which may be caused by a large leakage current. The magnetic hysteresis loop of BFO films is tested as well, indicating that the BFO film is antiferromagnetic and the residual magnetization (Mr) and coercive field (Hc) of the BFO films were 0.054?emu/g and 1026.4?Oe, respectively.     

Low temperature growth of sol-gel SrBi2Ta2O9 thin films by low-pressure annealing

A new low-temperature processing method to prepare SrBi₂Ta₂O₉ thin films is proposed. These thin films were prepared on Pt/Ta/SiO₂/Si substrates by a sol-gel method, and their structural and electrical properties were investigated. Films were annealed before and after the top Pt electrode deposition. The first annealing was performed in a 760-Torr oxygen atmosphere at 600 °C for 30 min, and the second annealing was performed in a 5-Torr oxygen atmosphere at 600 °C for 30 min. The films were well crystallized and fine-grained after the second annealing. The electrical characteristics of the 200-nm-thick film obtained by this new process were as follows: remanent polarization, P_r = 8.5 μC/cm²; coercive field, E_c = 36 kV/cm; and leakage current density, I_L = 1 × 10⁻⁷ A/cm² (at 150 kV/cm). This process is very attractive for highly integrated ferroelectric nonvolatile memory applications. © 1997 Scripta Technica, Inc. Electr Eng Jpn, 120(2): 27–33, 1997     

Effect of crystalline phases on the ferroelectric properties of HoMnO3 thin films

Ferroelectric HoMnO₃ thin films were deposited on the Si (100) substrates at 700°C for 2 h by metal–organic chemical vapor deposition. When the films were post-annealed at 800°C for 1 h in air, the single phase of hexagonal HoMnO₃ was detected, and the remnant polarization (Pr) and coercive field (Ec) were decreased due to the decrease of c-axis orientation. With an increase of annealing time, the crystalline phase of HoMnO₃ was changed from the single hexagonal to the mixtures of the hexagonal and orthorhombic phases of HoMnO₃, and/or HoMn₂O₅. Leakage current density was related with charge valence of Mn ion and surface roughness of thin film. Pr of hexagonal HoMnO₃ thin films with high c-axis orientation was 136 nC/cm² and the leakage current density was 10^?6 A/cm².     

Growth characteristics and film properties of gallium doped zinc oxide prepared by atomic layer deposition

We carried out comprehensive studies on structural, optical, and electrical properties of gallium-doped zinc oxide (Ga:ZnO) films deposited by atomic layer deposition (ALD). The gallium(III) isopropoxide (GTIP) was used as a Ga precursor, which showed pure Ga₂O₃ thin film with high growth rate. Using this precursor, conductive Ga doped ZnO thin film can be successfully deposited. The electrical, structural and optical properties were systematically investigated as functions of the Ga doping contents and deposition temperature. The best carrier concentration and transmittance (7.2?×?10²⁰ cm^?3 and 83.5 %) with low resistivity (≈3.5?×?10^?3?Ωcm) were observed at 5 at.% Ga doping concentration deposited at 250 °C. Also, low correlation of deposition temperature with the carrier concentration and film structure was observed. This can be explained by the almost same atomic radius of Ga and Zn atom.     

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.     

Pulsed excimer laser deposition of ferroelectric thin films

Abstract

Pulsed UV excimer laser ablation was employed to deposit multi-axial, bi-axial and uni-axial ferroelectric compositions of PZT, bismuth titanate and lead germanate respectively. In general, a fluence lower than 2 J/cm² caused a preferential evaporation of volatile components, resulting in stoichiometric imbalance. However, the fluences beyond 2 J/cm² enabled the deposition of stoichiometric thin films of multi-component oxide systems. The intrinsic bombardment due to the energetic ablated species during the thin film deposition seemed to influence the composition, structure, orientation and the electrical properties. The electrical characterization of ferroelectric films indicated a dielectric constant of 800–1000, a P_r of 32μC/cm² and E_c of 130KV/cm for polycrystalline PZT films and the corresponding quantities were measured to be 150, 7 μC/cm² and 20 KV/cm for in-situ crystallized c-axis preferred oriented bismuth titanate films. Lead germanate thin films oriented along c-axis (003) showed a dielectric constant of 30, a P_r of 2.5 μC/cm² and E_c of 55 KV/cm.     

Annealing temperature effect on ferroelectric and magnetic properties in Mn-added polycrystalline BiFeO3 films

We fabricated 5 at.% Mn-added polycrystalline BiFeO₃ films and investigated the annealing temperature effect on structural, ferroelectric and magnetic properties. In the x-ray diffraction patterns, only the diffraction peaks due to the BiFeO₃ structure were observed and no secondary phase could be observed at annealing temperatures between 773 and 923 K. Adding Mn suppressed the leakage current density in the high electric field region when compared to pure BiFeO₃ films. The conduction mechanism of the Mn-added BiFeO₃ films was dominated by Ohmic conduction. Remanent polarization of the Mn-added polycrystalline BiFeO₃ films for an applied electric field of approximately 1.5 mV/cm was 63 μC/cm² for the specimen annealed at 773 K and 46 μC/cm² for the specimen annealed at 923 K, although the remanent polarization still exhibited a tendency to increase with an increase in the electric field. Spontaneous magnetization was obtained at high annealing specimens. This study revealed that the annealing temperature strongly affected the ferroelectric and magnetic properties in Mn-added polycrystalline BiFeO₃ films. In addition, by optimizing the annealing temperature, we realized multiferroics coexistent with spontaneous magnetization and spontaneous polarization at room temperature in the Mn-added polycrystalline BiFeO₃ film.