Effect of LaNiO3 buffer layers on the structure and electrical properties of sol–gel-derived Pb(Mg1/3Nb2/3)O3PbTiO3 thin films

Pb(Mg_1/3Nb_2/3)O₃PbTiO₃ (PMNT) thin films on Pt/TiO₂/SiO₂/Si substrates with and without a LaNiO₃ (LNO) buffer layer have been prepared using a sol–gel method. Structures and electrical properties of these two films have been investigated and compared. Highly (111)-oriented PMNT thin films with a certain amount of pyrochlore phase are obtained on bare Pt electrodes. On the contrary, (100)-oriented PMNT thin films with pure perovskite phase are formed on Pt electrodes with a LNO buffer layer. Cracks are found in the former but not in the latter. The dielectric constant of PMNT thin films on LNO-buffer Pt electrodes is larger than that on bare Pt electrodes. A great lowering of the leakage current is observed in the films with a LNO buffer layer. The improvement in the electrical properties is attributed to both the elimination of cracks and the suppression of pyrochlore phase in the films. PACS 77.84.Dy; 77.80.-e; 77.22.Gm     

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.     

Effects of LaNiO<Subscript>3</Subscript> on the structures and properties of SrBi<Subscript>2</Subscript>Ta<Subscript>2</Subscript>O<Subscript>9</Subscript> thin films

SrBi₂Ta₂O₉(SBT)/LaNiO₃(LNO)/Si and SBT/Pt/TiO₂/SiO₂/Si multilayers were fabricated by pulsed laser deposition. With Pt top electrodes, the measured remanent polarization (2P_r) of Pt/SBT/LNO/Si and Pt/SBT/Pt/TiO₂/SiO₂/Si capacitors was 6.5 C/cm² and 5.2 C/cm², respectively. Using LNO as both bottom electrodes and buffer layers, enhanced non-c-axis crystalline SBT films were induced, which resulted in a 2P_r greater than that of the Pt/SBT/Pt/TiO₂/SiO₂/Si capacitor. The hysteresis loop of the Pt/SBT/LNO/Si capacitor showed a great external-field-dependent horizontal shift. Using an electron-injection model, this dependence was addressed. The fatigue-free property of the Pt/SBT/LNO/Si capacitor was experimentally established, in that the non-volatile polarization decreased by less than 5% of the initial value after 1.44×10⁹ switching cycles . PACS 77.84.Dy; 68.65.+g     

La0.3Sr0.7TiO3模板层对Pb(Zr0.5Ti0.5)O3薄膜的铁电性能增强效应的研究

通过sol-gel法在Si (111) 基片上分别制备了LaNiO₃(LNO)底电极和LaNiO₃/La_0.3Sr_0.7TiO₃ (LNO/LSTO)底电极.然后采用sol-gel 方法，在两种衬底上分别制备了Pb (Zr_0.5Ti_0.5)O₃ (PZT)铁电薄膜.XRD分析表明，两种PZT薄膜均具有钙钛矿结构，且在LNO底电极上的PZT薄膜呈(100) 择优取向，而在LNO/LSTO底电极上的PZT薄膜呈随机取向.铁电性能测试表明，相对LNO衬底上制备的PZT薄膜，在LNO/LSTO底电极上制备的PZT薄膜的剩余极化强度得到了有效的增强，同时矫顽场也增大.介电常数和漏电流的测试表明，LNO/LSTO底电极上制备的PZT薄膜具有大的介电常数和漏电流. 关键词： PZT薄膜 铁电性 漏电流 0.3Sr_0.7TiO₃')" href="#">La_0.3Sr_0.7TiO₃     

High pyroelectric Ba0.65Sr0.35TiO3 thin films with Ba0.65Sr0.35RuO3 seeding-layer for monolithic ferroelectric bolometer

Ba_0.65Sr_0.35TiO₃ (BST) thin films were deposited by RF sputtering with a very thin Ba_0.65Sr_0.35RuO₃ (BSR) seeding-layer on Pt/Ti/SiO₂/Si substrate. The crystallization of BST thin films and the surface morphology of BSR seeding-layer were characterized by X-ray diffraction (XRD) and atomic force microscopy (AFM), respectively. XRD patterns show that the BSR seeding-layer affected the orientation of BST thin film, which is highly a-axis textured. It was also found that the BSR seeding-layer had a marked influence on the dielectric properties of BST thin films. Comparing with BST thin films directly deposited on Pt electrode, the dielectric relaxation can be suppressed and dielectric constant increased due to a possible reduction of interface oxygen vacancies at BST/BSR interface. Moreover, J–V measurement indicates that the leakage current density of BST thin films on BSR seeding-layer were greatly reduced compared with that of BST thin films directly on Pt electrodes. The pyroelectric coefficient of BST thin films with BSR seeding-layer is 7.57 × 10⁻⁷ C cm⁻² K⁻¹ at 6 V/μm at room temperature (RT). Our results reveal that high pyroelectric property of BST thin film could be achievable using BSR seeding-layer as a special buffer.     

不同衬底上Pb(Zr0.52Ti0.48)O3择优取向铁电薄膜的制备和研究

通过MOD法在Si(100)和Pt(111)/Ti/SiO₂/Si基片上制备出LaNiO₃ ( LNO)薄膜.再通过修 正的Sol-gel法，在Pt(111)/Ti/SiO₂/Si,LNO/Si(100)和LNO/Pt/Ti/SiO_{2< /sub>/Si三种衬底上 制备出具有择优取向的Pb(Zr0.52Ti0.48)O3铁电薄膜. 经XRD分析表明，L NO薄膜具有(100)择优取向的类钙钛矿结构；PZT薄膜均具有钙钛矿结构，且在Pt(111)/Ti/S iO2/Si衬底上的薄膜以(110)择优取向，在LNO/Pt/Ti/SiO2/Si和LN O/Si(100)衬底上的 薄膜以(100)择优取向.经场发射SEM分析和介电、铁电性能测试表明，在LNO/Si和LNO/Pt/Ti /SiO2/Si衬底上的PZT薄膜的平均粒径、介电常数以及剩余极化强度均比以Pt/T i/SiO2/Si为衬底的薄膜大. 关键词： 3}薄膜')" href="#">LaNiO₃薄膜 PZT铁电薄膜 择优取向 剩余极化强度     

Microstructure and dielectric properties of pulsed-laser-deposited CaCu 3 Ti 4 O 12 thin films on LaNiO 3 buffered Pt/Ti/SiO 2 /Si substrates

CaCu₃Ti₄O₁₂ (CCTO) thin films have been prepared by a pulsed-laser-deposition method on LaNiO₃ buffered Pt/Ti/SiO₂/Si substrates, and their microstructure and dielectric properties have been compared with those of the films deposited directly on Pt/Ti/SiO₂/Si substrates. The crystalline structure and the surface morphology of the CCTO thin films were markedly affected by the bottom electrodes. Both the films show temperature-independent dielectric properties in a wide temperature range, which is similar to those properties obtained in single-crystal or epitaxial thin films, while the room-temperature dielectric constant of the 350-nm-thick CCTO films on LaNiO₃/Pt/Ti/SiO₂/Si substrates at 100 kHz was found to be 2300, which was increased significantly compared with that obtained in the films on Pt/Ti/SiO₂/Si substrates. Using the impedance spectroscopy technique, it has been suggested that the high dielectric constant response of the CCTO thin films originates from the grain boundary layer mechanism as found in internal barrier layer capacitors. PACS 77.55.+f; 81.15.Fg; 68.55.-a     

Influence of ambient oxygen pressure on the preferred orientation, microstructures, and dielectric properties of (Ba1-xSrx)TiO3 thin films with compositionally graded structures

Compositionally graded (Ba_1-xSr_x)TiO₃ (BST) thin films, with x decreasing from 0.25 to 0.0, were deposited on Pt(111)/Ti/SiO₂/Si(100) substrates by pulsed-laser ablation at 600 °C and under ambient oxygen pressures ranging from 50 to 400 mTorr. The influence of the ambient gas pressure on the preferred orientation, microstructures, and dielectric properties of compositionally graded BST films was investigated by X-ray diffraction, scanning electron microscopy, and dielectric frequency spectra, respectively. As the ambient oxygen pressure was increased, the preferred orientation evolved in the order: (100)+(110)(110)+(111) random orientation, and the surface roughness of the graded BST films also increased. The graded BST films deposited at high ambient oxygen pressures (300400 mTorr) exhibited a grainy structure with polycrystalline grains throughout the film thickness, whereas the graded films deposited at low ambient oxygen pressures (50200 mTorr) possessed a columnar structure. The evolution of the microstructure was ascribed to the different physical and chemical properties of the species that were incident onto the substrates at the various oxygen pressures. The dielectric properties of the graded BST films were dependent upon the ambient oxygen pressures. The graded BST films deposited at 200 mTorr exhibited the highest dielectric constant. PACS 77.55.+f; 77.22.Ch; 81.15.Fg     

Structural and electrical properties of (Na0.85K0.15)0.5Bi0.5TiO3 thin films deposited on LaNiO3 and Pt bottom electrodes

(Na_0.85K_0.15)_0.5Bi_0.5TiO₃ thin films were deposited on LaNiO₃(LNO)/SiO₂/Si(1 0 0) and Pt/Ti/SiO₂/Si(1 0 0) substrates by metal-organic decomposition, and the effects of bottom electrodes LNO and Pt on the ferroelectric, dielectric and piezoelectric properties were investigated by ferroelectric tester, impedance analyzer and scanning probe microscopy, respectively. For the thin films deposited on LNO and Pt electrodes, the remnant polarization 2P_r are about 22.6 and 8.8 μC/cm² under 375 kV/cm, the dielectric constants 238 and 579 at 10 kHz, the dielectric losses 0.06 and 0.30 at 10 kHz, the statistic d_33eff values 95 and 81 pm/V. The improved piezoelectric properties could make (Na_1−xK_x)_0.5Bi_0.5TiO₃ thin film as a promising candidate for piezoelectric thin film devices.     

Thermo-Sensitive Ba0.64Sr0.36TiO3 Thin Film Capacitors for Dielectric Type Uncooled Infrared Sensors

Ba_0.64Sr_0.36TiO₃ (BST) thin films are prepared on Pt/Ti/SiO₂/Si₃N₄/SiO₂/Si substrates by a sol-gel method. Thermo-sensitive BST thin film capacitors with a Metal-Ferroelectrics-Metal (M-F(BST)-M) structure are fabricated as the active elements of dielectric type uncooled infrared sensors. XRD are employed to analyze the crystallographic structures of the films. AFM observations reveal a smooth and dense surface of the films with an average grain size of about 35 nm. Rapid temperature annealing (RTA) process is a very efficient way to improve crystallization quality. The preferable annealing temperature is 800°C for 1 min. The butterfly shaped C-V curves of the capacitors indicate the films have a ferroelectric nature. The dielectric constant and dielectric loss of the films at 100 kHz are 450 and 0.038, respectively. At 25°C, where the thermo-sensitive capacitors work, the temperature coefficient of dielectric constant (TCD) is about 5.9 %/°C. These results indicate that the capacitors with sol-gel derived BST thin films are promising to develop dielectric type uncooled infrared sensors.     

Preparation of epitaxial compositionally graded (Ba1-xSrx)TiO3 thin films with enhanced dielectric properties

Epitaxial compositionally graded (Ba_1-xSr_x)TiO₃ (BST) (0.0x0.25) thin films were deposited on (100) LaAlO₃ substrates by pulsed laser ablation, the substrates having bottom electrodes made of 100-nm-thick conductive La_0.5Sr_0.5CoO₃ (LSCO). Extensive X-ray diffraction, rocking-curve, and -scan studies indicate that the graded films are (100)-oriented and exhibit good in-plane relationships of [010]_BST//[010]_LAO and [001]_BST//[001]_LAO. For the up-graded films with barium concentration (1-x) increasing across the film thickness in the direction from the film/substrate interface to the film surface, the full width at half maximum of the BST film (200) rocking curve and the surface roughness, examined by atomic force microscopy, were larger than those of the down-graded films with barium concentration decreasing from the film/substrate interface to the film surface. The dielectric properties of the graded films, measured using vertical structures, show that at room temperature, the dielectric constant (_r) and dissipation factor (cos) at 100 kHz were 380 and 0.013 for the up-graded films, and 650 and 0.010 for the down-graded films, respectively. The dielectric behavior was enhanced in the down-graded films, which was attributed to the fact that the pure BaTiO₃ layer in the down-graded BST films not only serves as a bottom layer but also acts as an excellent seeding layer for enhancing subsequent film growth, leading to better film crystallinity and larger grain sizes in the down-graded films. The graded BST films undergo a diffuse phase transition, giving a broad, flat capacitance-versus-temperature profile. With such a graded structure, it is possible to build a dielectric thin-film capacitor having a capacitance which has a low temperature dependence over a broad temperature regime. PACS 77.55.+f; 68.55.Jk; 81.15.Fg     

Dielectric and piezoelectric properties of the Ba0.92Ca0.08Ti0.95Zr0.05O3 thin films grown on different substrate

Lead free Ba_0.92Ca_0.08Ti_0.95Zr_0.05O₃ (BCZT) thin films were deposited on Pt/Ti/SiO₂/Si and LaNiO₃(LNO)/Pt/Ti/SiO₂/Si substrates by a sol–gel processing technique, respectively. The effects of substrate on structure, dielectric and piezoelectric properties were investigated in detail. The BCZT thin films deposited on LNO/Pt/Ti/SiO₂/Si substrates exhibit (100) orientation, larger grain size and higher dielectric tunability (64%). The BCZT thin films deposited on Pt/Ti/SiO₂/Si exhibit (110) orientation, higher Curie temperature (75 °C), better piezoelectric property (d₃₃ of 50 pm/V) and lower dielectric loss (0.02). The differences in dielectric and piezoelectric properties in the two kinds of oriented BCZT films should be attributed to the difference of structure, in-plane stress and polarization rotation in orientation engineered BCZT films.     

Microstructures and dielectric properties of compositionally graded (Ba1-xSrx) TiO3 thin films prepared by pulsed laser deposition

Compositionally graded (Ba_1-xSr_x)TiO₃ (BST) (x:0.0∼0.25) thin films were grown on Pt (111)/TiO₂/SiO₂/Si (100) substrates using layer-by-layer pulsed laser deposition in the temperature range 550–650 °C. Both downgraded (Ba/Sr ratio varying from 100/0 at the bottom surface to 75/25 at the top surface) and upgraded (Ba/Sr ratio varying from 75/25 at the bottom surface to 100/0 at the top surface) BST films were prepared. Their microstructures were systematically studied by X-ray diffractometry and scanning electron microscopy. A grain morphology transition from large ‘rosettes’ (>0.30 μm) to small compact grains (70–110 nm) was observed in the downgraded BST films as the deposition temperature was increased from 550 to 650 °C. No such grain morphology transition was detected in the upgraded BST films. Dielectric measurements with metal electrodes revealed an enhanced dielectric behavior in the downgraded films. This enhancement is mainly attributed to the large compressive stress field built up near the interface between the downgraded film and substrate. Furthermore, the BaTiO₃ layer in the downgraded BST films not only serves as a bottom layer but also as an excellent seeding layer for enhancing the crystallization of the subsequent film layers in the downgraded films. Received: 10 December 2001 / Accepted: 12 March 2002 / Published online: 19 July 2002 RID="*" ID="*"Corresponding author. Fax: 86-25/359-5535, E-mail: xhzhu@public1.ptt.js.cn     

Characteristics of Ba xSr 1–xTiO 3 thin films grown by pulsed laser ablation of rotating split targets of BaTiO 3 and SrTiO 3

We have grown heterostructures of Ba_xSr_1-xTiO₃(BST)/La_0.7Sr_0.3MnO₃(LSMO) on LaAlO₃(LAO) substrates by the pulsed laser deposition method. BST films with x=0.2,0.5,0.7 and 0.8 have been prepared using a novel rotating split-target arrangement. The lattice constant of the BST films is found to vary linearly with Ba/Sr ratio. An excellent cube-on-cube epitaxial relationship of (100)_BST||(100)_LSMO||(100)_LAO has also been obtained. Scanning electron microscopy studies have revealed smooth and crack-free BST films with a uniform grain size of about 100 nm. Dielectric measurements, made with patterned Au top electrodes and conducting LSMO bottom layers, have shown a maximum permittivity of approximately 280 at 5 kHz in BST films with x=0.7. P–E loop analyses of the Ba_0.7Sr_0.3TiO₃ and Ba_0.8Sr_0.2TiO₃ films have yielded remnant polarization values of 1.66 and 1.81C/cm², respectively. PACS 81.15Fg; 68.55Jk; 77.55+f     

Tailoring resistive switching characteristics in WOx films using different metal electrodes

We have investigated the role of the metal/oxide junction interface on the resistive switching (RS) characteristics in WO_3+x films. The WO_x films are fabricated on Pt substrates by magnetron sputtering at room temperature. Top metal contact (Au or Al) is fabricated by using thermal evaporator. The thicknesses of WO_x films and top electrodes are 1 μm and 200 nm, respectively. It has been found that the bi-polar RS direction is dependent on the choice of top metal electrode, Au or Al. The sample with a Au top electrode shows clockwise (CW) RS mode whilst the sample with a Al top electrode shows counter-clockwise (CCW) RS mode. The on/off ratio is 10 times for Au/WO_x/Pt and 100 times for Al/WO_x/Pt. The bi-polar RS modes are modeled in terms of the difference in the electronegativity of the top and bottom electrodes.     

Controlled growth of rutile TiO2 by atomic layer deposition on oxidized ruthenium

Crystalline rutile TiO₂ films were grown by atomic layer deposition on oxidized Ru electrodes using a titanium methoxide as the metal precursor and O₃ as the oxidant. A protective layer of ～0.3 nm TiO₂ grown with H₂O as the oxidant was first deposited in order to avoid etching of the Ru bottom electrode by the O₃ used for the growth of the TiO₂ (bulk) layer. Electrical evaluation of the capacitor stacks with TiO₂ as dielectric, RuO₂/Ru and Pt as the bottom and top electrodes respectively, resulted in superior characteristics of the rutile phase as compared to the anatase. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Thickness dependent magnetic and ferroelectric properties of LaNiO3 buffered BiFeO3 thin films

BiFeO₃ (BFO) thin films with thickness increasing from 40 to 480 nm were successfully grown on LaNiO₃ (LNO) buffered Pt/Ti/SiO₂/Si(100) substrate and the effects of thickness evolution on magnetic and ferroelectric properties are investigated. The LNO buffer layer promotes the growth and crystallization of BFO thin films. Highly (100) orientation is induced for all BFO films regardless of the film thickness together with the dense microstructure. All BFO films exhibited weak ferromagnetic response at room temperature and saturation magnetization is found to decrease with increase in film thickness. Well saturated ferroelectric hysteresis loops were obtained for thicker films; however, the leakage current dominated the ferroelectric properties in thinner films. The leakage current density decreased by three orders of magnitude for 335 nm film compared to 40 nm film, giving rise to enhanced ferroelectric properties for thicker films. The mechanisms for the evolution of ferromagnetic and ferroelectric characteristics are discussed.     

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.     

Bipolar resistive switching in BiFe_(0.95)Zn_(0.05)O_3 films

Bipolar resistive switching is studied in BiFe0.95Zn0.05O3 films prepared by pulsed laser deposition on （001） SrTiO3 substrate, with LaNiO3 as the bottom electrode, and Pt as the top electrode. Multiple steps of resistance change are ob- served in the resistive switching process with a slow voltage sweep, indicating the formation/rupture of multiple conductive filaments. A resistive ratio of the high resistance state （HRS） to the low resistance state （LRS） of over three orders of mag- nitude is observed. Furthermore, the conduction mechanism is confirmed to be space-charge-limited conduction with the Schottky emission at the interface with the top Pt electrodes in the HRS, and Ohmic in the LRS. Impedance spectroscopy demonstrates a conductive ferroelectric/interfacial dielectric 2-layer structure, and the formation/rupture of the conductive filaments mainly occurs at the interfacial dielectric layer close to the top Pt electrodes.     

Effects of substrates on the structure and dielectric properties of Ba(Sn0.15Ti0.85)O3 thin films

Ba(Sn_0.15Ti_0.85)O₃ (BTS) thin films were grown on Pt(1 1 1)/Ti/SiO₂/Si and LaNiO₃(LNO)/Pt(1 1 1)/Ti/SiO₂/Si substrates by a sol-gel processing technique, respectively. The BTS thin films deposited on annealed Pt(1 1 1)/Ti/SiO₂/Si and annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si substrates exhibited strong (1 1 1) and perfect (1 0 0) orientations, respectively. The BTS thin films grown on un-annealed Pt(1 1 1)/Ti/SiO₂/Si substrates showed random orientation with intense (1 1 0) peak, while the films deposited on un-annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si substrate exhibited random orientation with intense (1 0 0) peak, respectively. The dielectric constant of the BTS films deposited on annealed Pt(1 1 1)/Ti/SiO₂/Si, annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si, un-annealed Pt(1 1 1)/Ti/SiO₂/Si and un-annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si substrates was 512, 565, 386 and 437, respectively, measured at a frequency of 100 kHz. A high tunability of 49.7% was obtained for the films deposited on annealed LNO/Pt(1 1 1)/Ti/SiO₂/Si substrate, measured at the frequency of 100 kHz with an applied electric field of 200 kV/cm. The high tunability has been attributed to the (1 0 0) texture of the films and larger grain sizes.