Na0.5K0.5NbO3 Film Microwave Varactors

Na_0.5K_0.5NbO₃ (NKN) and Pb(Zr_0.53Ti_0.47)O₃ (PZT) films have been grown by rf-magnetron sputtering and pulsed laser deposition techniques, correspondingly, on sapphire (Al₂O₃-0112, r-cut), quartz (Y+36°-cut) and YAlO₃ + 1% Nd (Nd:YAlO₃-001) single crystal substrates with Interdigital Capacitor (IDC) of Coplanar Waveguide (CPW) structure. Photolithography and metal lift-off technique was used for processing of the tunable microwave capacitor. Microwave network analyzer with G-S-G Picoprobe and probe station performed microwave measurement with external DC bias. NKN film interdigital capacitors on Nd:YAlO₃ show superior performance in the microwave range from 1 to 40 GHz. Within this range, the voltage tunability (40 V, 200 kV/cm) was about 29%, loss tangent ～ 0.13, K-factor from 152% @10 GHz to 46% @40 GHz, voltage independent C _p was about 230 fF, tan δ _p changes from 0.14 @10 GHz to 0.36 @40 GHz, real and imaginary part of interconnect impedance increases with frequency from 0.13 Ω @10 GHz to 0.50 Ω @40 GHz and from 1.9 Ω @10 GHz to 5.9 Ω @40 GHz respectively.     

Characterization of dielectric and acoustic properties of CSD PZT thin films at high frequencies

In this study, the microwave dielectric and the acoustic properties of Pb(Zr _x ,Ti_1-x )O₃ (PZT) thin films deposited using chemical solution deposition (CSD) were investigated using the same measurement setup. High dielectric constants in the range of ~280–540 and loss tangents less than 0.1 at 4 GHz were measured, where the value depends on the thickness of the PZT film. The voltage tunability of the 340 nm and 440 nm thick PZT thin films was ~34% and 5% for the 140 nm thick PZT film at 120 kV/cm and 4 GHz. The acoustic parameters of the PZT thin films under DC bias voltages were determined using a one-dimensional acoustic wave resonator model. For the PZT films of thicknesses 340 nm and 440 nm, the acoustic resonance frequency shift was about 15 MHz and the electromechanical coupling coefficient was ~10% at an electric field of 160 kV/cm. The large dielectric constant and high tunability suggest that the characterized PZT thin films may be suitable for radio frequency (RF) applications such as high-density RF MIM capacitors and other tunable devices.     

Low temperature sintering of screen-printed Pb(ZrTi)O3 thick films

Abstract

There has been increasing interest in ferroelectric lead zirconate titanate (PZT) films for the applications in piezoelectric and pyroelectric devices. Many potential applications require a film thickness of above 10 μm for higher force, better sensitivity and stability. But it is very difficult to fabricate the PZT thick film on the silicon substrate because of the volatility of PbO and the interdiffusion of the Pb and Si through the bottom electrode during the sintering at normal temperatures (such as above 1200°C). We speculated densification and reaction mechanism of the PZT thick films fabricated at relatively low temperature (under 1000°C) without sintering aids. The PZT thick films were screen-printed on Pt / Al₂O₃ substrate using a paste of PbO, ZrO₂ and TiO₂ powder mixture. Highly densified PZT thick films could be fabricated on Pt / Al₂O₃ substrate at 1000°C, and we achieved the density, remanent polarization, coercive field, dielectric permittivity, dissipation factor and breakdown field of 98%, 10 μC/cm² and 20 kV/cm, 540, 0.009 and 15 MV/m, respectively. The results show the possibility of densification of the PZT thick film at relatively low temperature without sintering aids, and the results are promising for the use of PZT thick films in various applications.     

Rf Sputtered Na0.5K0.5NbO3 Films on Oxide Substrates as Optical Waveguiding Material

Highly crystalline Na_0.5K_0.5NbO₃ (NKN) thin films of 1–2 μm thickness were deposited by rf-magnetron sputtering of a stoichiometric, ceramic target on single crystal LaAlO₃(001) and Al₂O₃(0112) substrates. X-ray diffraction measurements revealed epitaxial quality of NKN/LaAlO₃ film structures, whereas NKN films on sapphire substrates were found to be preferentially c-axis oriented. A prism-coupling technique was used to characterize optical and waveguiding properties. A bright-line spectrum at λ = 632.8 nm, revealed sharp peaks, corresponding to transverse magnetic (TM) and electric (TE) waveguide propagation modes in NKN/LaAlO₃ and NKN/Al₂O₃ thin films. Using a least mean square fit the refractive index for the films and film thickness were calculated. The extraordinary and ordinary refractive indices were determined to n _e = 2.207 ± 0.002 and n _o = 2.261 ± 0.002, and n _e = 2.216 ± 0.002 and n _o = 2.247 ± 0.002 at λ = 632.8 nm for 2.0 μm thick NKN films on LaAlO₃ and Al₂O₃, respectively. This corresponds to a birefringence Δn = n _e ? n _o = ?0.054 ± 0.003 and Δn = ?0.031 ± 0.003 in the films, where the larger Δn for the NKN/LaAlO₃ structure can be explained by the superior crystalline quality compared to NKN/Al₂O₃. Atomic force microscopy images of the film surfaces revealed rms roughnesses of 2.5 nm and 8.0 nm for 1.0-μm thick NKN/LaAlO₃ and NKN/Al₂O₃ films, respectively. We believe surface scattering is one of the main sources of waveguide losses in the thin films.     

Ferroelectric field effect in (La,Sr)CoO3/Pb(Zr,Ti)O3/(La,Sr)CoO3 heterostructures

Abstract

Epitaxial LaCoO₃/Pb(Zr,Ti)O₃/(La,Sr)CoO₃ (LSCO) heterostructures have been grown on LaAlO₃ by pulsed laser deposition for investigating ferroelectric field effect. In the heterostructure, semiconducting LaCoO₃ was used as a conducting channel layer, instead Si. The resistivity of the LaCoO₃ (LCO) channel layer was found to be dependent on an oxygen ambient, primarily the ambient oxygen pressure during deposition. The resistivity of the LCO layer varied in the range of 0.1 – 100 Ω cm. Ferroelectric field effect induced in LaCoO₃ layer was observed by measuring the resistance modulation of the LCO layer with respect to the polarized state of the PZT layer. The resistance modulation of 9% was obtained in the 680 Å thick LCO layer. Further the resistance modulation was improved up to 45% after applying dc bias. It is suggested that the LCO/PZT/LSCO heterostructure can be used as a ferroelectric field effect transistor.     

Thickness dependent performance of Na0.5K0.5NbO3/sapphire thin film varactors

Abstract

Perfect c-axis oriented Na_0.5K_0.5NbO₃ (NKN) films have been pulsed laser deposited on Al₂O₃(0112) single crystals (r-cut sapphire) for voltage tunable microwave device applications. Thickness dependence of dielectric performance of the NKN/sapphire interdigital capacitors (IDCs) has been studied. 40 V bias tunability and dielectric loss tan δ of 4 μm slot IDCs have been found to be 24.6 % and 2.86 % for 1.2 μm thick NKN film, and 6.1 % and 0.83 % for 0.14 μm thick NKN film, respectively. Low leakage currents and high breakdown voltages are observed in these structures.     

Investigation of top electrode for PZT thick films based MEMS sensors

In this work processing of screen printed piezoelectric PZT thick films on silicon substrates is investigated for use in future MEMS devices. E-beam evaporated Al and Pt are patterned on PZT as a top electrode using a lift-off process with a line width down to 3 μm. Three test structures are used to investigate the optimal thickness of the top electrode, the degradation of the piezoelectric properties of the PZT film in absence of a diffusion barrier layer and finally how to fabricate electrical interconnects down the edge of the PZT thick film. The roughness of the PZT is found to have a strong influence on the conductance of the top electrode influencing the optimal top electrode thickness. A 100 nm thick top electrode on the PZT thick film with a surface roughness of 273 nm has a 4.5 times higher resistance compared to a similar wire on a planar SiO₂ surface which has a surface roughness of less than 10 nm. It is found that the piezoelectric properties of the PZT thick film are degraded up to 1,000 μm away from a region of the PZT thick film that is exposed directly to the silicon substrate without a diffusion barrier layer. Finally, ferroelectric hysteresis loops are used to verify that the piezoelectric properties of the PZT thick film are unchanged after the processing of the top electrode.     

Preparation and electrical properties of 0.4Pb(Zn1/3Nb2/3)O3-0.6Pb(Zr0.4Ti0.6)O3 thin films by 2-step annealing method

Films of (1−x)Pb(Zn_1/3Nb_2/3)O₃-xPb(Zr_0.4Ti_0.6) O₃ (x = 0.6, 40PZN-60PZT) were deposited on Pt/TiO₂/ SiO₂/Si substrate through spin coating. Using a combination of homogeneous precursor solution preparation and two-step pyrolysis process, we were able to obtain the 40PZN-60PZT thin films of perovskite phase virtually without pyrochlore phase precipitation after annealing above 650^∘C. But since annealing done at the high temperatures for extended time can cause diffusion of Pt, TiO₂ and Si, and precipitation of nonstoichiometric PbO, we adopted 2-step annealing method to circumvent these problems. The 2-step annealed films show dense microstructure than the 1-step films annealed at higher temperature. Furthermore, the root-mean-square surface roughness of 220 nm thick films which are annealed at 720^∘C for 1 min and then annealed at 650^∘C for 5 min was found to be 3.9 nm by atomic force microscopy as compared to the 12 nm surface roughness of the film annealed only at 720^∘C for 5 min. The electrical properties of 2-step annealed films are virtually same and those of the 1-step annealed films annealed at high temperature. The film 2-step annealed at 720^∘C for brief 1 min and with subsequent annealing at 650^∘C for 5 min showed a saturated hysteresis loop at an applied voltage of 5 V with remanent polarization (P _r) and coercive voltage (V _c) of 25.3 μC/cm² and 0.66 V respectively. The leakage current density was lower than 10⁻⁵A/cm² at an applied voltage of 5 V.     

Effect of Buffer Layer on the Properties of Laser Ablated PZT Thin Films

Lead zirconate titanate (PbZr _x Ti_1?x O₃) or PZT ceramics are a class of piezoelectric materials that are currently experiencing widespread use in industry as electromechanical devices. PtSi/ZnO/PZT thin films were deposited by pulsed laser deposition at relatively low substrate temperature. The PZT thin films on PtSi substrates and on ZnO buffer layer were deposited at substrate temperature 300°C. The composition analysis shows that the film deposited at low temperature is stoichiometric. The films exhibit ferroelectric nature with coercive field of 19.6 kV/cm for 800 nm thick film. The leakage current density of the films shows a good insulating behavior.     

Ferroelectric switching and fatigue behavior for PZT/YBCO thin film heterostructures

Abstract

The dielectric and ferroelectric properties for Au/Pb(Zr,Ti)O₃/YBa₂Cu₃O_7?x heterostructures at low temperatures are reported. The fatigue behavior and the ferroelectric switching effect for the structures are also investigated. The PZT/YBCO thin film heterostructures were deposited on MgO(100) substrates by laser ablation. The ferroelectric and dielectric properties and optical response of the oriented PZT films with different thicknesses have been studied over the temperature range from 20 K to 300 K. The dielectric loss of the structure was found to decrease by an order of magnitude when the YBCO bottom electrode became superconducting. A very low fatigue rate of the structure has also been obtained below T _c of YBCO layer.     

Resonance properties and mass sensitivity of monolithic microcantilever sensors actuated by piezoelectric PZT thick film

The PZT thick film cantilever devices fabricated via MEMS process have much attraction because they are appropriate for biological transducer or sensor, resulting from their large actuating force and relatively high sensitivity especially in liquid. By means of resonance behavior, theoretical calculation and experimental verification of the PZT thick film cantilever devices have not been studied before. Accordingly, we focused on the sensitivity analysis and interpretation of the PZT thick film cantilevers in this study. Especially, the investigation for mass sensitivity of the PZT thick film cantilever is of importance for physical, chemical and biological sensing application. The PZT thick film cantilever devices were constructed on Pt/TiO₂/SiN _X /Si substrates using screen printing method and MEMS process. The harmonic oscillation response (resonance frequency) was measured using an optical laser interferometric vibrometer. The effect of cantilever geometry on the resonance frequency change was investigated. Compared with the theoretical resonant frequency change by mass loading, the experimental resonant frequency change of the PZT micromechanical thick film cantilever shows a variation of less than 2%. Mass sensitivities are estimated to be 30.7, 57.1 and 152.0 pg/Hz for the 400 × 380 μm, 400 × 480 μm and 400 × 580 μm cantilever, respectively.     

Thin pyroelectric PLZT film obtained with sol-gel technology

The sol-gel technology (J. Zarzycki in J.Sol-Gel Sci. Technol. 8:17–22, 1997) and the spin coating were employed for the production of PLZT 12/40/60 pyroelectric film. The starting materials were: lead acetate, lanthanum nitrate, metallo-organic compounds of zirconium and titanium and acetic acid. An alumina substrate with pre-deposited lanthanum-strontium cobalt oxide (LSCO) (H. Takahashi, et al in Phys. Rev. B. 57:15211–15218, 1998) bottom electrode was spin-coated with a sol several times. Following, the film was rapidly thermally processed. To obtain a continuous PLZT film these two operations were repeated a few times. The top electrode, made from LSCO, was subsequently applied on the PLZT film. The produced film has a lower pyroelectric coefficient than bulk ceramics and thick films formerly produced. Figure of merit F _v relating to the voltage responsivity is higher than those of the two earlier materials, due to much lower relative permittivity. The important advantage of applied method is that it requires much lower processing temperature (680°C) than that (1,150°C) needed to produce bulk and thick-film sensors.     

Preparation and characterization of PZT ferroelectric thin films by plasma enhanced metalorganic chemical vapor deposition

Abstract

PZT thin films with a uniform distribution of components were prepared by plasma enhanced chemical vapor deposition (PECVD) using Pb(C₂H₅)₄, Z (O-i-C₄H₉)₄, Ti(O-i-C₃H₇)₄, and oxygen. The crystallization of films was occure after annealing in the temperature range between 450 and 550°C under O₂ ambient for 1 hr. The significant change of Pb concentration in PECVD PZT thin films was not observed in the relation to annealing temperature and time. The dielectric constant PECVD PZT thin films increased with the Ti content, showed the maximum value in the vicinity of morphotropic phase boundary (MPB) composition of PZT material, and decreased with the Ti content. The leakage current density of PZT (65/35) thin film of 180 nm in thickness was 3·37 × 10^?7 A/cm² at the applied voltage of 3 V. Remanent polarization increased with increasing of Zr content in the film and coercive field was nearly independent of the composition. The typical values of electrical properties were ε_r = 570, E_c = 90 kV/cm, and P_r = 19 μC/cm² in the PECVD PZT (54/46) thin film of 220 nm in thickness.     

Fabrication and Electromechanical Properties of Pb(Zr0.52,Ti0.48)O3 Micro-Diaphragm

ABSTRACT

Multilayered piezoelectric micro-diaphragms have been successfully fabricated by micro-electro-mechanical-system (MEMS) processing. The micro-diaphragms consisted of diol based sol-gel derived Pb(Zr_0.52Ti_0.48)O₃ (PZT) capacitor, sputtered Pt electrode, and low temperature oxide(LTO)/SiN_x/Si substrate. The PZT film exhibited (111) oriented structure. The dielectric constant and loss of the PZT thin films were 800 and 3% at 100～ 100 kHz, respectively. The remanent polarization was 20 μ C/cm². The lateral dimension of the PZT film was varied relative to the square-shaped supporting membrane with 300 or 400 μ m length. The relative size (ratio of lateral dimensions) of the PZT film to the supporting membrane was varied from 0.7 to 1.1 to investigate its influence on the system performance. The micro-diaphragm exhibited mechanical displacement from 0.067 to 0.135 μ m at 15 V and had a maximum displacement at a ratio of relative size of 0.8, regardless of the lateral size of the supporting membrane. The fundamental resonant frequency of the micro-diaphragm which has 300 μ m length supporting membrane was in the range of 348 kHz to 365 kHz, depending on the relative size. As the PZT size increased relative to the supporting membrane, the resonant frequency decreased and reached a minimum at the relative size of 0.8. The micro-diaphragm with the supporting membrane (400 μ m length) had a lower resonant frequency, i.e., 251～270 kHz, but showed a similar behavior to the micro-diaphragm with the supporting membrane (300 μ m length) in relation to the resonant frequencies with the relative size.     

Preparation of BaPbO3 Electrode Thin Films by RF Magnetron Sputtering

For electrode materials of Pb(Zr,Ti)O₃ (PZT) thin films in ferroelectric random access memory (FeRAM), various materials have been studied. As new electrode material with which the polarization and fatigue properties are improved, we take notice of barium metaplumbate BaPbO₃ (BPO). Because the BPO contained lead (Pb) and oxygen is conductor that adopted same perovskite structure as PZT. BPO thin films were prepared by rf magnetron sputtering on various substrates. (SiO₂/Si, MgO, Al₂O₃ and Pt-coated substrates), and influence of growth conditions (sputtering gas, rf power, the substrate-heating temperature and post anneals) on crystallization and conductivity were investigated. In case of post anneal after sputtering at room temperature, perovskite single phase was obtained above 400°C. In case of substrate heating while sputtering, without post anneal, perovskite single phase was obtained at 350–500°C on SiO₂/Si substrates (110) preferred orientation BPO films obtained at low temperature, and resistivity of the films decreased at decreasing sputtering temperature. Resistivity of the film at substrate temperature 350°C was 3 × 10^?3 Ω cm. In the case of single crystal substrate, the BPO films were epitaxially grown. Orientation of the films was varied with the sputtering condition. The epitaxial PZT thin films were also grown on the BPO, revealing that PZT(111)[011] //BPO(111)[011] //Pt(100)[011] //MgO(100)[011] and PZT(111)[011] //BPO(111)[011] //Pt(111)[011] //Al₂O₃(001)[100] structures were obtained, and their ferroelectric properties were also evaluated.     

The resistance degradation of (Ba0.5Sr0.5)TiO3 thin films

Abstract

The leakage current and dielectric properties of (Ba_0.5Sr_0.5)TiO₃(BST) thin films prepared by pulsed laser deposition (PLD) were investigated. It was found that leakage currents for positive bias voltage were higher than that for negative bias voltage, which was attributed to the lattice mismatch between bottom Pt electrode and BST thin film. The time-dependent breakdown process under positive voltage was observed, which was interpreted as the increase of the internal electric field in the film near the bottom electrode. However, the internal electric field can be decreased and eventually recovered by applying negative bias voltage. It was found that internal electric field near the interface can influence the capacitance of the BST thin film capacitor. An explanation for the thickness effect of BST thin films was given.     

The Effect of La-Doped Bi4Ti3O12 Buffer Layer on Crystallinity and Ferroelectric Properties of PbZr0.58Ti0.42O3/Bi3.25La0.75Ti3O12 Multilayered Thin Films

PbZr_0.58Ti_0.42O₃ (PZT) ferroelectric thin films with Bi_3.25La_0.75Ti₃O₁₂ (BLT) buffer layer of various thickness were fabricated on Pt/TiO₂/SiO₂/p-Si(100) substrates by rf-magnetron sputtering method. The pure PZT film showed (111) preferential orientation in the XRD patterns, and the PZT/BLT films showed (110) preferential orientation with increasing thickness of the BLT layer. There were no obvious diffraction peaks for the BLT buffer layer, for its thin thickness in PZT/BLT multilayered films. There were the maximum number of largest-size grains in PZT/BLT(30 nm) film among all the samples from the surface images of FESEM. The growth direction and grain size had significant effects on ferroelectric properties of the multilayered films. The fatigue characteristics suggested that 30-nm-thick BLT was just an effective buffer layer enough to alleviate the accumulation of oxygen vacancies near the PZT/BLT interface. The comparison of these results suggests that the buffer layer with an appropriate thickness can improve the ferroelectric properties of multilayered films greatly.     

Ferroelectric Na0.5K0.5NbO3 thin films by pulsed laser deposition

Abstract

Highly c-axis oriented single phase Na_0.5K_0.5NbO₃ (NKN) thin films have been deposited onto polycrystalline Pt₈₀lr₂₀ substrates and SiO₂/Si(001) wafers using pulsed laser ablation of stoichiometric ceramic target. Strong self-assembling of NKN films along the [001] direction has been observed. Properties of NKN/Pt thin film structures have been successfully tailored by oxygen pressure control from the ferroelectric state, characterized by the remnant polarization of 12 uC/cm², dielectric constant ? ～ 520 and tan δ ～ 0.024 @ 100 kHz, to superparaelectric state with tan δ as low as 0.003 and ? = 210 with very small 1.7% dispersion in the frequency domain 0.4–100 kHz and less than 10% variation in the temperature range 77–415 K. NKN films grown onto SiO₂/Si(001) substrates show quadrupled super-lattice structure along c-axis, loss tan δ less than 0.01, and ? ～ 110 @ 1 MHz. C-V measurements for Au/NKN (270nm)/SiO₂/Si MFIS-diode structure yield memory window of 3.26 V at the programmable voltage of 8 V.     

Preparation and evaluation of sub-100 nm Pb(Zr,Ti)O3 films derived from modified sol-gel solutions for low-voltage operation of feram

Abstract

Sub-100 nm PbZr_0.3Ti_0.7O₃ (PZT) films were prepared on Pt/SiO₂/Si substrates from modified sol-gel solutions without using any seeding layers. Firstly, we studied Pb content [Pb/(Zr+Ti)] dependence of 90-nm-thick films. In the wide Pb content region of 108 – 125%, the films had perovskite-single-phase fine columnar grains with (111)-orientation and no voids. Electric properties were dependent on Pb content. The film with good microstructure, rectangular hysteresis, high remanent polarization (P_r), and low leakage current was gained for Pb content of 116%. Secondly, we studied film thickness dependence of PZT(116/30/70) films. Films from 90 down to 61 nm in thickness were prepared. We found that the sub-100 nm films with good microstructures could be prepared from the modified solutions. The sub-100 nm films had saturation voltage of 1.25 V and high P_r even at 1 V or less. In particular, a 61-nm-thick film had high.P_r of 17 μC/cm2 at 0.75 V.     

Scaling Effect on the Dielectric Constant in Ba(Ti x Zr1−x )O3 Thin Films

Recent work on PZT and BST thin films reveal a thickness dependence of the dielectric constant for a film thickness below 100 nm. This effect is commonly attributed to an interfacial layer between the electrode and the dielectric film (dead layer). In this contribution we report on the influence of the film thickness on the dielectric constant of Ba(Ti_xZr_{1 – x})O₃ thin films with different Zr-contents (x = 0–30 at.%). The films were prepared by chemical solution deposition (CSD) with thickness between 30 and 350 nm.The electrical characterization was performed in a temperature range between 25 and 200C. Results were interpreted with respect to the formation of a serial dead layer capacitance.