Enhanced ferroelectric properties of (Pb0.90La0.10)Ti0.975O3 multilayered thin films prepared by RF magnetron sputtering

The (Pb_0.90La_0.10)Ti_0.975O₃/PbTiO₃ (PLT/PT), PbTiO₃/(Pb_0.90La_0.10)Ti_0.975O₃/PbTiO₃ (PT/PLT/PT) multilayered thin films with a PbO_x buffer layer were in situ deposited by RF magnetron sputtering at the substrate temperature of 600 °C. With this method, highly (1 0 0)-oriented PLT/PT and PT/PLT/PT multilayered thin films were obtained. The PbO_x buffer layer leads to the (1 0 0) orientation of the films. The dielectric, ferroelectric and pyroelectric properties of the PLT multilayered thin films were investigated. It is found that highly (1 0 0)-oriented PT/PLT/PT multilayered thin films possess higher remnant polarization 2P_r (44.1 μC/cm²) and better pyroelectric coefficient at room temperature p (p = 2.425 × 10⁻⁸ C/cm² K) than these of PLT and PLT/PT thin films. These results indicate that the design of the PT/PLT/PT multilayered thin films with a PbO_x buffer layer should be an effective way to enhance the dielectric, ferroelectric and pyroelectric properties. The mechanism of the enhanced ferroelectric properties was also discussed.     

Effect of buffer layers on the property of Pb(Zr,Ti)O3-Pb(Mn,W,Sb,Nb)O3 thin films grown by pulsed laser deposition

New ferroelectric Pb(Zr,Ti)O₃-Pb(Mn,W,Sb,Nb)O₃ (PZT-PMWSN) thin film has been deposited on a Pt/Ti/SiO₂/Si substrate by pulsed laser deposition. Buffer layer was adopted between film and substrate to improve the ferroelectric properties of PZT-PMWSN films. Effect of a Pb(Zr_0.52Ti_0.48)O₃ (PZT) and (Pb_0.72La_0.28)Ti_0.93O₃ (PLT) buffer layers on the stabilization of perovskite phase and the suppression of pyrochlore phase has been examined. Role of buffer layers was investigated depending on different types of buffer layer and thickness. The PZT-PMWSN thin films with buffer layer have higher remnant polarization and switching polarization values by suppressing pyrochlore phase formation. The remnant polarization, saturation polarization, coercive field and relative dielectric constant of 10-nm-thick PLT buffered PZT-PMWSN thin film with no pyrochlore phase were observed to be about 18.523 μC/cm², 47.538 μC/cm², 63.901 kV/cm and 854, respectively.     

Comparison of the effect of PLT and PZT buffer layers on PZT thin films for ferroelectric materials applications

In order to study the effect of different buffer layers on the Pb(Zr_0.52Ti_0.48)O₃ (PZT) thin films, 10-nm thick (Pb_0.72La_0.28)Ti_0.93O₃ (PLT) and Pb(Zr_0.52Ti_0.48)O₃ buffer layers have been deposited on the Pt(1 1 1)/Ti/SiO₂/Si substrates by pulsed laser deposition, respectively. The top buffer layers were also deposited on PZT thin films with the same thickness of the seed layers in order to enhance the fatigue characteristics of PZT thin films. We compared the results of dielectric constant, hysteresis loops and fatigue resistance characteristics. It was found that the dielectric properties of PZT thin films with PLT buffer layers were improved by comparing with PZT thin films with PZT buffer layers. The polarization characteristics of PZT thin films with PLT buffer layers were observed to be superior to those of PZT thin films using PZT buffer layers. The remanent polarization of PZT thin films showed 36.3 μC/cm² and 2.6 μC/cm² each in the case of use PLT and PZT buffer layers. For the switching polarization endurance analysis, PZT thin films with PLT buffer layers showed more excellent result than that of PZT thin films with PZT buffer layers.     

Experimental evidence of breakdown strength and its effect on energy-storage performance in normal and relaxor ferroelectric films

Normal-ferroelectric Pb(Zr_0.52Ti_0.48)O₃ (PZT) and relaxor-ferroelectric Pb_0.9La_0.1(Zr_0.52Ti_0.48)O₃ (PLZT) thin-films are deposited on SrRuO₃-covered SrTiO₃/Si substrates. An ultrahigh recoverable energy-storage density (U_reco) of 68.2 J/cm³ and energy efficiency (η) of 80.4% are achieved in the PLZT thin-films under a large breakdown strength (E_BD) of 3600 kV/cm. These values are much lower in the PZT thin-films (U_reco of 10.3 J/cm³ and η of 62.4% at E_BD of 1000 kV/cm). In addition, the remanent polarization (P_r) and dielectric-constant are also investigated to evaluate the breakdown strength in thin-films. Polar nano-regions (PNRs) are created in the PLZT thin-films to enable relaxor behavior and lead to slim polarization loops along with very small P_r. The excellent operating temperature of energy-storage performance and also the breakdown strength obtained in the PLZT thin-films are mainly ascribed to the presence of PNRs. Moreover, both PZT and PLZT thin-films exhibit superior performance up to 10¹⁰ times of charge-discharge cycling.     

Periodicity and orientation dependence of electrical properties of [(Pb0.90La0.10)Ti0.975O3/PbTiO3]n (n = 1-6) multilayer thin films

The [(Pb_0.90La_0.10)Ti_0.975O₃/PbTiO₃]_n (PLT/PT)_n (n = 1-6) multilayer thin films were deposited on the PbO_x(1 0 0)/Pt/Ti/SiO₂/Si substrates by RF magnetron sputtering method. The layer thickness of PbTiO₃ in one periodicity kept unchanged, and the layer thickness of (Pb_0.90La_0.10)Ti_0.975O₃ is varied. The electrical properties of the (PLT/PT)_n multilayer thin films were investigated as a function of the periodicity (n) and the orientation. The studied results show that the PbO_x buffer layer results in the (PLT/PT)_n films’ (1 0 0) orientation, and the (1 0 0)-oriented (PLT/PT)_n multilayer thin films with n = 2 exhibit better pyroelectric properties and ferroelectric behavior than those of (PLT/PT)_n films with other periodicities and orientations. The underlying physical mechanism for the enhanced electrical properties of (PLT/PT)_n multilayer thin films was carefully discussed in terms of the periodicities and orientations.     

Light-induced intrinsic defects in PLZT ceramics

This paper reports on an EPR study of a ferroelectric, 1.8/65/35, and an antiferroelectric, 2/95/5, of optically transparent Pb_1?y La_yZr_1?x Ti_xO₃ (PLZT) ceramics within a broad temperature range (20–300 K) after illumination at a wavelength of 365–725 nm. Illumination with ultraviolet light, whose photon energy corresponds to the band gap of these materials, at T<50 K creates a number of photoinduced centers: Ti³⁺, Pb⁺, and Pb³⁺. It is shown that these centers are generated near a lanthanum impurity, which substitutes for both the Pb²⁺ and, partially, Ti⁴⁺ ions through carrier trapping from the conduction or valence band into lattice sites. The temperature ranges of the stability of these centers are measured, and the position of their local energy levels in the band gap is determined. The most shallow center is Ti³⁺, with its energy level lying 47 meV below the conduction band bottom. The Pb³⁺ and Pb⁺ centers produce deeper local levels and remain stable in the 2/95/5 PLZT ceramics up to room temperature. The migration of localized carriers is studied for both ceramic compositions. It is demonstrated that, under exposure to increased temperature or red light, the electrons ionized into the conduction band from Ti³⁺ are retrapped by the deeper Pb⁺ centers, thus hampering the carrier drift in the band and the onset of photoconduction. The part played by localized charges in the electrooptic phenomena occurring in the PLZT ceramics is discussed.     

Index of refraction in ‘dirty’ displacive ferroelectrics

We report measurements of the optic index of reflection as a function of temperature, n(T), for several highly disordered ferroelectrics: PLZT ceramic [Pb_1?xLa_x(Zr_0.65Ti_0.35)_1?x/4O₃ where x = 0.08] and single crystals of Pb₃(MNb₂)O₉ where M = Zn and Mg. The results are qualitatively different from the unusual displacive ferroelectric behavior and the difference is clearly due to local disorder.     

Fabrication of the hydrogen resistive ferroelectric film of the (Pb0.72La0.28)Ti0.93O3/Pb(Zr0.52Ti0.48)O3/(Pb0.72La0.28)Ti0.93O3 heterostructure by a pulsed laser deposition method

(Pb_0.72La_0.28)Ti_0.93O₃ (PLT)/Pb(Zr_0.52Ti_0.48)O₃ (PZT)/PLT heterostructure was fabricated by using a pulsed laser deposition method. After depositing this structure, the hydrogen annealing process was performed in the forming gas (95% N₂ + 5% H₂) at a substrate temperature of 400 °C for 30 min to study the effects of hydrogen passivation.The heterostructure was not degraded by the hydrogen annealing in contrast with the case of PZT film without buffer layers. This heterostructure showed almost no degradation in terms of the remanent polarization even after the H₂ annealing, while the PZT film exhibited 64% reduction, which is from 20.1 to 7.3 μC/cm² after the annealing. The leakage current was decreased by an order in the case of the heterostructure, while the leakage current of the PZT film increased by an order.These can be explained that the PLT bottom buffer layer works as a seeing layer to help the PZT growth and the top PLT buffer layer acts as a barrier for penetrating hydrogen atoms.     

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     

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.     

Dynamics of birefringence properties in 17/30/70 PLZT ceramics

Birefringent properties of PLZT ceramics (Pb₈₃La₁₇)(Zr₃₀Ti₇₀)O₃ were investigated by measuring the transverse electrooptic effect in a 0.2 mm-thick wafer at various speeds of external voltage changes. At least two types of internal polarized microregions of different physical nature in charge of the electrooptical properties are observed.     

Measurement of optical and surface properties of PLZT thin films

Lanthanum-modified lead zirconate titanate (Pb_0.93La_0.07(Zr_0.3Ti_0.7)_0.93O₃, PLZT7/30/70) thin films with and without a seeding layer of PbTiO₃ (PT) were successfully deposited on indium-doped tin oxide (ITO) coated glass substrate via spin coating in conjunction with a sol–gel process, and a top transparent conducting thin film of SnO₂ was also prepared in the same way. The thicknesses of PLZT and PT layers are 0.5 μm and 24 nm, respectively. The retardance of PLZT film was measured by a new heterodyne interferometer and enhanced by application of a seeding layer of PT. The Pockels linear electro-optical coefficient of PLZT film with a PT layer was determined to be 3.17 × 10^?9 m/V when the refractive index is considered as 2.505, which is one order larger than 1.4 × 10^?10 m/V for PLZT12/40/60 doped with Dy reported in the literature. The root-mean-square (rms) roughness of PLZT thin film with a PT layer (R_rms = 6.867 nm) was larger than that of PLZT film (R_rms = 0.799 nm). From the comparisons, the average transmittance of PLZT film with a PT seeding layer was 77.01%, which was a little smaller than that of PLZT film (around 80.75%). Experimental results imply that the PT seeding layer plays a key role in the increase of retardance value, leading to a higher Pockels coefficient.     

Ferroelectric properties of highly c-axis oriented Bi4−xLaxTi3O12 film-based capacitors

Highly c-axis oriented lanthanum-modified bismuth titanate (Bi_4−xLa_xTi₃O₁₂) films having a variety of lanthanum (La) contents were grown on Pt/TiO₂/SiO₂/Si(100) substrates using metal-organic sol deposition and subsequent annealing at 650 °C for 1 h. After systematically examining the ferroelectric properties of Bi_4−xLa_xTi₃O₁₂ films as a function of the La-content, it was concluded that the film with x=0.85 had the largest remanent polarization in the direction parallel to the c-axis. The Pt/Bi_3.15La_0.85Ti₃O₁₂/Pt capacitor showed a well-saturated polarization-electric field (P-E) switching curve with the switching remanent polarization (2P_r) value of 33 μC/cm² and the coercive field (E_c) of 68 kV/cm at an applied voltage of 10 V. More importantly, the capacitor exhibited fatigue-free behavior up to 6.5×10¹⁰ read/write switching cycles at a frequency of 1 MHz. The capacitor also demonstrated an excellent charge-retaining ability and a strong resistance against the imprinting failure.     

Enhanced ferroelectric property of (Pb0.95Ca0.05)(Nb0.02Zr0.80Ti0.20)O3 thin films prepared by RF magnetron sputtering

(Pb_0.95Ca_0.05)(Nb_0.02Zr_0.80Ti_0.20)O₃ [PCNZT] thin films were deposited on the Pt(1 1 1)/Ti/SiO₂/Si(1 0 0) substrates by RF magnetron sputtering with and without a LaNiO₃ [LNO] buffer layer. Ca and Nb elements in PZT films enhance the ferroelectric property, LaNiO₃ buffer layer improves the crystal quality of the PCNZT thin films. PCNZT thin films possess better ferroelectric property than that of PZT films for Ca and Nb ion substitution, moreover, PCNZT thin films with a LNO buffer layer possess (1 0 0) orientation and good ferroelectric properties with high remnant polarization (P_r = 38.1 μC/cm²), and low coercive field (E_c = 65 kV/cm), which is also better than that of PCNZT thin films without a LNO buffer layer (P_r = 27.9 μC/cm², E_c = 74 kV/cm). The result shows that enhanced ferroelectric property of PZT films can be obtained by ion substitution and buffer layer.     

溶胶-凝胶法制备Sr2Bi4Ti5O18薄膜及其铁电性能研究

采用溶胶-凝胶法,在氧气氛中和层层晶化的工艺条件下,成功地制备了沉积在Pt/Ti/SiO₂/Si(100)衬底上的铁电性能优良的Sr₂Bi₄Ti₅O₁₈ (SBTi)薄膜,并研究了SBTi薄膜的微结构、表面形貌、铁电性能和疲劳特性.研究表明：薄膜具有单一的层状钙钛矿结构，且为随机取向；薄膜表面光滑，无裂纹，厚度约为725nm；铁电性能测试显示较饱和、方形的电滞回线，当外电场强度为275kV/cm时 关键词： 溶胶-凝胶法 铁电薄膜 2Bi₄Ti₅O₁₈')" href="#">Sr₂Bi₄Ti₅O₁₈     

Spectroscopic ellipsometry investigations of PLT ferroelectric thin films with various La concentrations in the mid-infrared spectral region

(Pb_1-xLa_x)Ti_1-x/4O₃ (PLT) ferroelectric thin films with various La concentrations have been grown on LaNiO₃/Si(100) substrates by a modified sol-gel technique. X-ray-diffraction analyses show that the PLT and LaNiO₃ thin films are polycrystalline and entirely perovskite phase. The infrared optical properties of the PLT thin films have been investigated using infrared spectroscopic ellipsometry in the wavelength range of 2.5–12.5 m. By fitting the measured ellipsometric parameter (cos and cos) data with a four-phase model (air/PLT/LaNiO₃/Si), and a derived dispersion relation for the PLT thin films, the optical constants and thicknesses of the thin films have been determined. The refractive index of the PLT thin films decreases with increasing wavelength; however, by a Kramers–Kronig analysis the extinction coefficient increases with increasing wavelength. Moreover, the refractive index and extinction coefficient of the PLT thin films increase with increasing La concentration. This indicates that the infrared optical constants of the PLT thin films are a function of the La concentration. It is believed that the increase in the infrared optical constants of the PLT thin films with increasing La concentration is mainly due to the crystallinity and the electronic band structure of the PLT thin films. PACS 77.55.+f; 78.66.-w; 78.30.Am; 81.70.Fy     

Raman spectroscopic studies of PbxLa1−xTi1−x/4O3 thin films grown on Si substrates by RF magnetron sputtering

A systematic spectroscopic investigation of Pb_xLa_1−xTi_1−x/4O₃ (PLT) thin films grown on PbO_x/Pt/Ti/SiO₂/Si substrate by RF magnetron sputtering was performed by using confocal Raman spectroscopy. Influence of the growth condition modification including different growth temperatures, with various buffer layer thickness, and post-annealing treatments were analyzed with taking advantages of the corresponding Raman spectral band variation in the respective process. Significant change in the spectral bands occurred with the alteration of the growth condition, and the related mechanisms were discussed after spectral deconvolution, providing reliable information about the direction for film growth.     

La掺杂对Bi4Ti3O12薄膜铁电性能的影响

利用Sol-Gel法在Pt/Ti/SiO₂/Si衬底上制备出Bi₄Ti₃O₁₂和Bi_3.25La_0.75Ti₃O₁₂薄膜，研究了La掺杂对Bi₄Ti₃O₁₂薄膜的晶体结构、铁电性能和疲劳特性的影响，发现La掺杂没有改变Bi₄Ti₃O₁₂薄膜的基本晶体结构，并且提高了Bi₄Ti₃O₁₂铁电薄膜的剩余极化值和抗疲劳性能，对La掺杂改善Bi₄Ti₃O₁₂铁电薄膜性能的机理进行了讨论. 关键词： 铁电性能 4Ti₃O₁₂薄膜')" href="#">Bi₄Ti₃O₁₂薄膜 3.25La_0.75Ti₃O₁₂薄膜')" href="#">Bi_3.25La_0.75Ti₃O₁₂薄膜 sol-gel法 La掺杂     

Effects of vanadium doping on structure and electrical properties of SrBi4Ti4O15 thin films

The effects of vanadium(V) doping into SrBi₄Ti₄O₁₅ (SBTi) thin films on the structure, ferroelectric, leakage current, dielectric, and fatigue properties have been studied. X-ray diffraction result showed that the crystal structure of the SBTi thin films with and without vanadium is the same. Enhanced ferroelectricity was observed in the V-doped SrBi₄Ti₄O₁₅ (SrBi_4−x/3Ti_4−xV_xO₁₅, SBTiV-x (x = 0.03, 0.06, and 0.09)) thin films compared to the pure SrBi₄Ti₄O₁₅ thin film. The values of remnant polarization (2P_r) and coercive field (2E_c) of the SBTiV-0.09 thin film capacitor were 40.9 μC/cm² and 105.6 kV/cm at an applied electric field of 187.5 kV/cm, respectively. The 2P_r value is over five times larger than that of the pure SBTi thin film capacitor. At 100 kHz, the values of dielectric constant and dielectric loss were 449 and 0.04, and 214 and 0.06 for the SBTiV-0.09 and the pure SBTi thin film capacitors, respectively. The leakage current density of the SBTiV-0.09 thin film capacitor measured at 100 kV/cm was 6.8 × 10⁻⁹ A/cm², which is more than two and a half orders of magnitude lower than that of the pure SBTi thin film capacitor. Furthermore, the SBTiV-0.09 thin film exhibited good fatigue endurance up to 10¹⁰ switching cycles. The improved electrical properties may be related to the reduction of internal defects such as bismuth and oxygen vacancies with changes in the grain size by doping of vanadium into SBTi.     

Electric field effects on the dielectric and acoustic anomalies of Pb[(Mg1/3Nb2/3)0.83Ti0.17]O3 single crystals studied by dielectric and Brillouin spectroscopies

The effect of the electric field on the dielectric and acoustic properties of Pb[(Mg_1/3Nb_2/3)_0.83Ti_0.17]O₃ single crystals was investigated as functions of temperature and the electric field strength. The dielectric constant and the acoustic mode behaviors exhibited typical relaxor behaviors when there was no bias field. The longitudinal acoustic mode showed splitting under a moderate electric field of 1 kV/cm applied along the [001] direction, indicating coexistence of macroscopic/mesoscopic ferroelectric states and relaxor states. Further increase in the electric field up to 2 kV/cm induced a clear ferroelectric phase transition, which became smeared out due to the proximity of the electric field to the critical point. The electric field-temperature phase diagram of Pb[(Mg_1/3Nb_2/3)_0.83Ti_0.17]O₃ was suggested based on the observed field-induced changes in the dielectric and the acoustic properties.