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Satoru UTSUGI, Takashi FUJISAWA, Yoshitaka EHARA, Tomoaki YAMADA, Shin ...
2010 年 118 巻 1380 号 p.
627-630
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Epitaxial tetragonal PZT films with (100)/(001) and (110)/(101) and (111) orientations were grown on various kinds of single crystal substrates having different thermal expansion coefficient. Volume fractions of (001) and (101) orientations in respective (100)/(001)- and (110)/(101)-oriented films were almost linearly increased with increasing thermal strain of the films that was generated under the cooling process after the deposition from the growth temperature to the Curie temperature. Perfectly (001)- and (101)-oriented films were grown on (111) CaF
2 substrates with large thermal expansion coefficient. Observed saturation polarization values linearly changed with the volume fractions of (100) and (101) orientations.
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Hiroshi YAMAZAKI, Tetsuo SHIMURA, Wataru SAKAMOTO, Toshinobu YOGO
2010 年 118 巻 1380 号 p.
631-635
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
The BiScO
3–PbTiO
3 binary system is known to have a morphotropic phase boundary (MPB) and a higher Curie temperature than Pb(Zr,Ti)O
3 and to exhibit excellent dielectric and ferroelectric properties. Perovskite BiScO
3–PbTiO
3 powders and thin films were synthesized via a chemical process using metal-organic precursor solutions. Homogeneous and stable precursor solutions, perovskite BiScO
3–PbTiO
3 single-phase powders and thin films on Pt/TiO
x/SiO
2/Si substrates were successfully prepared by optimizing the processing conditions. The 0.35BiScO
3–0.65PbTiO
3 composition was close to the MPB and had a Curie temperature of around 470°C. The electrical properties of BiScO
3–PbTiO
3 thin films showed a maximum at this composition. The dielectric permittivity of the 0.35BiScO
3–0.65PbTiO
3 thin film at the MPB was approximately 1700, with a dielectric loss tangent of less than 5% at room temperature. Furthermore, BiScO
3–PbTiO
3 thin films showed a typical ferroelectric polarization (
P)–electric field (
E) hysteresis loop. The remnant polarization (
Pr) and coercive field (
Ec) of the 0.35BiScO
3–0.65PbTiO
3 film were approximately 23 µC/cm
2 and 70 kV/cm, respectively.
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Hiromi SHIMA, Takashi IIJIMA, Takashi NAKAJIMA, Soichiro OKAMURA
2010 年 118 巻 1380 号 p.
636-639
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
The Zr/Ti ratio dependence of refractive index and electrooptic coefficient of epitaxial (Pb,La)(Zr,Ti)O
3 (PLZT) films were investigated. PLZT films were fabricated on La-doped SrTiO
3 (La-STO) substrates by a chemical solution deposition (CSD) method. Optical properties in TE- and TM-modes were measured individually using a prism coupling method. The refractive indexes both in TE- and TM-modes were as large as that of the polycrystalline film, and increased with increasing Ti/(Zr + Ti) ratio. The refractive index in TE-mode was larger than that in TM-mode because the PLZT films received compressive stress from the La-STO substrates due to lattice mismatch. The refractive index in TM-mode almost linearly decreased with increasing applied an electric field while that in TE-mode slightly increased and saturated around at 200 kV/cm. The Pockels coefficient in TM-mode
r33 showed large change for compositions, while that in TE-mode
r13 showed little change. The maximum Pockels coefficient
rc of 156 pm/V was obtained for the epitaxial PLZT film with Ti/(Zr + Ti) ratio of 50%.
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Yuta KASHIWAGI, Takashi IIJIMA, Takashi NAKAJIMA, Soichiro OKAMURA
2010 年 118 巻 1380 号 p.
640-643
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Endurance properties of piezoelectric-induced longitudinal displacement for lead zirconate titanate (PZT) thick films were investigated to develop microelectromechanical systems (MEMS). A 5-µm-thick film was prepared using chemical solution deposition (CSD). Square and triangle waveforms and various frequencies of unipolar or bipolar electric fields were applied to the film. The effects of applied field switching cycles on the ferroelectric properties and longitudinal displacements were measured using a twin-laser interferometer system. Under the bipolar applied field switching condition, the remanent polarization and piezoelectric displacement decreased concomitantly with increasing applied field switching cycles, similar to fatigue behavior. The applied field switching waveform and frequency affect the fatigue profile. The piezoelectric displacement did not decrease when the unipolar square and triangle waveform were applied to the samples. These results suggest that the unipolar driven PZT thick films are applicable to MEMS devices.
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Masamichi NISHIDE, Maresuke KUZUHARA, Takeshi TAI, Takashi KATODA, Hit ...
2010 年 118 巻 1380 号 p.
644-647
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
The crystal structure and strain in a (100)/(001)-oriented PZT micro cantilever under applied voltage were characterized by in-situ Raman spectroscopy. A Pt/LaNiO
3/(100)/(001)PZT/LaNiO
3/Pt/Ti/SiO
2/silicon-on-insulator (SOI) multilayer structure was fabricated in a process based on a microelectromechanical system (MEMS). The volume fraction of the domain switching from
a-domains to
c-domains was monotonously increased with increases in the applied voltage. No compressive in-plane lattice strain was induced in the PZT film with the increases in the applied voltage. These results show that Raman spectroscopy is a useful method for in-situ observation of PZT micro cantilevers.
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Hiroshi NAGANUMA, Takamichi MIYAZAKI, Akihiko UKACHI, Mikihiko OOGANE, ...
2010 年 118 巻 1380 号 p.
648-651
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Amorphous Bi–Fe–O
x films prepared on SrTiO
3 (100) substrates using a conventional r.f. magnetron sputtering system were crystallized by post-annealing at 873 K in an atmosphere. Microstructural observations by X-ray diffraction and cross-sectional transmission electron microscopy revealed that the crystallized Bi–Fe–O
x films were well-epitaxially BiFeO
3 fabricated without interfacial layer although as-prepared film was amorphous structure with excess Bi. The crystallized BiFeO
3 films have fairly epitaxial compatibly ([001](001)BiFeO
3 // [001](001)SrTiO
3). These results indicate that (1) BiFeO
3 has good epitaxial compatibility with SrTiO
3 and (2) crystallizing amorphous Bi–Fe–O
x is one possible method that can be used to fabricate high-quality multiferroic barriers for tunnel junctions.
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Takeshi KAWAE, Yuki TERAUCHI, Takashi NAKAJIMA, Soichiro OKAMURA, Akih ...
2010 年 118 巻 1380 号 p.
652-655
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Pr and Mn co-substituted BiFeO
3 (BFO) thin films were fabricated on a Pt-coated (100) SrTiO
3 substrates by pulsed laser deposition (PLD) method. X-ray diffraction patterns indicated that the formation of impurity phases was suppressed by Pr substitution in the BFO thin films. Furthermore, by combining with small amount of Mn substitution, Pr substitution was effective for reducing the leakage current density. The polarization vs electric field curves showed well-saturated hysteresis loops with measurement frequency of 20 kHz at room temperature. The remnant polarization at a maximum electric field of 1500 kV/cm was approximately 50–70 µC/cm
2.
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Hiroshi NAGANUMA, Yosuke INOUE, Soichiro OKAMURA
2010 年 118 巻 1380 号 p.
656-658
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
A measurement system with a high driving frequency of 100 kHz is effective for measuring the ferroelectricity of leaky ferroelectric materials such as multiferroic BiFeO
3 films. A high driving frequency reduces the measurement time, leading to a drastic reduction in the influence of the leakage current density on ferroelectric hysteresis loops. Phase-delay compensation is essential in a system with a driving frequency of 100 kHz; in this study a standard capacitor was used for phase-delay compensation. The value of remanent polarization of a BiFeO
3 film measured by the 100-kHz system was confirmed by a positive, up, negative and down measurement.
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Keisuke YAZAWA, Shintaro YASUI, Hitoshi MORIOKA, Tomoaki YAMADA, Hiros ...
2010 年 118 巻 1380 号 p.
659-663
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Epitaxial
xBi(Zn
1/2Ti
1/2)O
3–(1 −
x)BiFeO
3 films were grown on (100)
cSrRuO
3//(100)SrTiO
3 substrates by metal organic chemical vapor deposition (MOCVD). The effects of
x value on the crystal structure and the electrical properties were investigated. Constituent phase changed from rhombohedral symmetry to two types of tetragonal ones with different unit cell volume and tetragonality. Rhombohedral phase and the tetragonal phase with smaller tetragonality were not ascertained to transform to cubic phase up to 800°C from high temperature XRD results. Relative dielectric constant measured at room temperature showed the maximum value at
x = 0.21 near the phase boundary between tetragonal and rhombohedral symmetries. Leakage current became small when the measurement temperature decreased at 80 K and the ferroelectricity monotonously decreased with increasing
x values and was not ascertained above 0.26.
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Naohiro HORIUCHI, Takuya HOSHINA, Hiroaki TAKEDA, Takaaki TSURUMI
2010 年 118 巻 1380 号 p.
664-668
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
We propose a calculation model that can predict the influence of interface on capacitance–voltage characteristics of metal-insulator-metal type thin film capacitor with perovskite type oxide. The simulation could successfully describe the results of capacitance–voltage measurements of the barium strontium titanate thin film capacitors with top electrodes of Pt, Au, and Ag. It is found that the electrode dependent on the tunability is derived from the work function of the electrode metal. The simulation model is base on the Schottky model that can be employed to explain the dielectric properties of metal/perovskite type oxide junction. The modified Schottky model considers the electric field dependence of permittivity and the back flow of electrons from metal to defect states located in the band gap of the perovskite oxide. This flow forms negatively charged space at the interface and affects the electric properties of the thin film capacitors.
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Naonori SAKAMOTO, Haruna YOSHIOKA, Junpei SUZUKI, Toshimasa SUZUKI, Na ...
2010 年 118 巻 1380 号 p.
669-673
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
BaTiO
3 (BT) based perovskite films are expected as ferroelectric and piezoelectric materials alternating Pb(Zr,Ti)O
3 (PZT) films which involve toxicity of the lead. In the present study, we focus effects of bottom electrode structures on electrical properties of the BT films fabricated by Chemical Solution Deposition (CSD) method. The BT films were fabricated on 1–6 layered LaNiO
3 (LNO) bottom electrode on Si or Pt/Ti/SiO
2/Si substrate. The dielectric constant of the BT films fabricated on LNO/Pt/Ti/SiO
2/Si substrate showed higher values than that on the LNO/Si substrate. The dielectric constant and piezoelectric properties increased with increasing layer numbers of the LNO. The microstructure and crystal structure of the BT films was studied by means of X-ray diffraction, scanning electron microscopy (SEM), and scanning transmission electron microscopy (STEM).
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Hirokazu SHIMOOKA, Shigemi KOHIKI, Makoto KUWABARA
2010 年 118 巻 1380 号 p.
674-678
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
This paper reports on two topics regarding nanosized barium titanate (BaTiO
3) prepared by the sol–gel method using a highly concentrated alkoxides precursor solution. One topic concerns the crystallographic features of the BaTiO
3 nanoparticles. In the case of using a highly concentrated precursor solution, non-core–shell BaTiO
3 nanocrystals with a small amount of intraparticle voids, lattice hydroxyl groups and remaining alkoxy groups were efficiently generated by the addition of less excess water during aging at room temperature. The generation of the high-quality BaTiO
3 nanocrystals is considered to be due to the hydrolysis and polycondensation reaction of the alkoxides being well promoted in such a concentrated solution. The lattice volume of the BaTiO
3 nanocrystals with a crystallite size of 15 nm fired at 600°C was approximately 1 vol % larger than that of bulk crystal. This lattice expansion is more likely to be caused by an intrinsic size effect than an extrinsic effect due to the lattice defects, such as lattice hydroxyl groups. The other topic concerns the dielectric properties of dense nanograin free-standing films with a grain size of 57 nm after applying the same sol–gel method. Significant frequency dispersion behavior of dissipation factor was observed at temperatures less than the Curie temperature. This finding may indicate that the dielectric properties reflect an intrinsic grain size effect without any influence being attributed to the film/substrate interface or lattice defects.
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Takashi TERANISHI, Naohiro HORIUCHI, Takuya HOSHINA, Hiroaki TAKEDA, T ...
2010 年 118 巻 1380 号 p.
679-682
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Analysis of asymmetric Raman line shape disclosed the variation of phonon correlation length in A
1(3TO) mode,
LA1(3TO), with temperature in the ceramics of BaTiO
3 (BT), Ba
0.6Sr
0.4TiO
3 (BST-0.6) and BaZr
0.25Ti
0.75O
3 (BZT-0.25), namely normal ferroelectrics, ferroelectrics with diffuse phase transition (DPT ferroelectrics) and relaxor ferroelectrics, respectively. In BT,
LA1(3TO) exhibited steep increase at the Curie temperature (
Tc) on cooling. This is attributed to the formation of the ferroelectric domains at the
Tc. Both BST-0.6 and BZT-0.25 showed gradual increase in
LA1(3TO) on cooling across the dielectric maximum temperature (
Tm), indicating the continuous increase in the average size of the polar nanoregions (PNRs). Normal ferroelectrics can be distinguished from DPT and relaxor ferroelectrics in this point.
LA1(3TO) of BZT-0.25 was longer than that of BST-0.6 near the
Tm. This suggests the size of PNRs in BZT-0.25 is larger than that in BST-0.6. Huge dipole polarization of BZT-0.25, giving rise to the strong relaxor behavior, could be originated from the contribution of the large PNRs near the
Tm. DPT ferroelectrics can be also differentiated from relaxor ferroelectrics in terms of the average size of PNRs.
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Satoshi WADA, Keisuke YAMATO, Petr PULPAN, Nobuhiro KUMADA, Bong-Yeon ...
2010 年 118 巻 1380 号 p.
683-687
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Barium titanate (BaTiO
3, BT)–bismuth magnesium titanium oxide (Bi(Mg
0.5Ti
0.5)O
3, BMT) solid solution system ceramics were prepared using nanoparticles in atmosphere to enhance Curie temperature (Tc) of BT, 132°C, to much higher temperature. Optimization of calcination and sintering conditions resulted in a formation of a perovskite single-phase, and their densities were always greater than 94%. The synchrotron XRD measurement revealed that the all ions in the ceramics had almost homogeneous distribution. Temperature dependence of dielectric property revealed that the BT–BMT system ceramics was typical relaxor materials, and for the 0.5BT–0.5BMT ceramics, the dielectric maximum was clearly observed at 360°C. Finally, their apparent piezoelectric constant (
d*) were measured by electric-field dependence of strain at room temperature, and the
d* value was measured at around 60 pm/V for the 0.4BT–0.6BMT ceramics.
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Satoshi WADA, Ai NOZAWA, Shogo IWATSUKI, Tetsuo KUWABARA, Takahiro TAK ...
2010 年 118 巻 1380 号 p.
688-690
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Barium titanate (BaTiO
3, BT) and strontium titanate (SrTiO
3, ST) nanocube particles were prepared by a solvothermal method. The prepared particles were collected by a centrifugal separator. The X-ray diffraction (XRD) measurement and a transmittance electron microscope (TEM) observation confirmed the formation of perovskite BT and ST nanocube particles with sizes of around 17 nm. These nanocube particles were monodistributed in hexane with tri-n-butylphosphine oxide (TBPO) as dispersant, separately, and then, the accumulations composed of the BT and ST nanocubes were built up using a selective catalytic reaction between 3-bromopropylphosphonic acid (BP) and aminomethylphosphonic acid (AM) as smart glue. The TEM observation confirmed that a part of accumulations showed a hetrointerface connection between BT and ST.
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Satoshi WADA, Shigehito SHIMIZU, Petr PULPAN, Nobuhiro KUMADA, Daisuke ...
2010 年 118 巻 1380 号 p.
691-695
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Barium titanate (BaTiO
3, BT)–potassium niobate (KNbO
3, KN) solid solution system (0.5BT–0.5KN) ceramics with various microstructures were prepared by two-step sintering method, and their piezoelectric properties were investigated. For 0.5BT–0.5KN ceramics, two phases, ferroelectric tetragonal and ferroelectric orthorhombic, coexisted in different grains at room temperature, owing to the limited solid solution system. The volume fraction of interface region between BT-rich tetragonal and KN-rich orthorhombic grains was controlled by sintering temperatures, and increased with decreasing sintering temperatures. Apparent piezoelectric constant
d33* was measured using slope of strain vs. electric field curves. As the results, the
d33* increased with decreasing sintering temperatures, which revealed that interface region between tetragonal and orthorhombic grains could contribute to enhancement of piezoelectric properties.
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Ken-ichi KAKIMOTO, Keisuke SUGIYAMA, Isao KAGOMIYA
2010 年 118 巻 1380 号 p.
696-700
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Platelet KNbO
3 particles having perovskite single phase have been successfully synthesized by a new simple procedure based on the dry-mixing technique and self-flux method using KNO
3 source that required no washing and filtration process. Well-crystalline edge-shaped platelet KNb
3O
8 particles were first obtained by the reaction between KNO
3 and Nb
2O
5. Next, they were reacted with second KNO
3 to form platelet KNbO
3 particles by the topochemical conversion method. The platelet KNbO
3 particles synthesized at 800°C demonstrated a relatively high aspect ratio of around 5 with edge lengths of about 2–10 and 10–40 µm in size for the tabular and thickness directions, respectively. The topochemical conversion mechanism from KNb
3O
8 to KNbO
3 was also proposed in this study.
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Takashi FURUHASHI, Makoto MORIYA, Wataru SAKAMOTO, Toshinobu YOGO
2010 年 118 巻 1380 号 p.
701-705
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Rhombohedrally distorted perovskite BiFeO
3–K
0.5Na
0.5NbO
3 ceramics with ferroelectricity and ferromagnetism were synthesized by solid-state reaction. The effect of K
0.5Na
0.5NbO
3 content on the crystal structure, electrical and magnetic properties of a BiFeO
3–K
0.5Na
0.5NbO
3 system was examined with a view to achieving multiferroic BiFeO
3-based ceramics. Perovskite BiFeO
3–K
0.5Na
0.5NbO
3 single phase was obtained by formation of solid solution with K
0.5Na
0.5NbO
3, whereas pure BiFeO
3 ceramics contained a small amount of a second phase, such as Bi
36Fe
2O
57. The crystallographic symmetry of BiFeO
3–K
0.5Na
0.5NbO
3 changed from rhombohedral to cubic when the content of K
0.5Na
0.5NbO
3 exceeded 15 mol %. The rhombohedrally distorted BiFeO
3–K
0.5Na
0.5NbO
3 showed a high Curie temperature (>770°C) and weak ferromagnetism at room temperature. Dielectric properties of the resultant ceramics were improved by controlling the amount of Mn doping to facilitate ferroelectric measurements.
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Hiroaki TAKEDA, Jun-ichi YAMAURA, Takuya HOSHINA, Takaaki TSURUMI
2010 年 118 巻 1380 号 p.
706-710
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
We report the structure and electric properties of La
3Ta
0.5Ga
5.5−xAl
xO
14 (LTGA
x,
x = 0.0 (LTG), 0.3 and 0.5) single crystals, with a Ca
3Ga
2Ge
4O
14-type structure, suitable for high temperature piezoelectric application. A single-crystal X-ray structure analysis reveals that Al atoms are distributed in all cation sites except for the decahedral site occupied by La, which favors instead the octahedral site. The piezoelectric moduli
d11 kept a constant, whereas |
d14| increased 14% with the increasing Al content,
x, up to 0.5. The LTGA0.5 crystals showed a low temperature dependence (2% deviation from room temperature to 400°C) of
d11 and a higher electric resistivity ρ than those of the LTG crystals. The Al substitution is effective for improving the electrical properties of the LTG.
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Yuji NOGUCHI, Masaru MIYAYAMA
2010 年 118 巻 1380 号 p.
711-716
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
Single crystals of K
0.14Na
0.86NbO
3 (KNN) and Mn-substituted KNN (Mn-KNN, K
0.14Na
0.86Mn
0.005Nb
0.995O
y) were grown by a flux method, and the effects of Mn substitution on the leakage current, polarization and dielectric properties were investigated along [100]
cubic. As-grown and annealed (850°C in air) crystals did not show an apparent polarization hysteresis loop due to its large leakage current density (∼10
−3 A/cm
2). The annealing at 1100°C in air led to a marked decrease in leakage current density of the order of ∼10
−6 A/cm
2 for KNN crystals. Mn-KNN crystals annealed at 1100°C in air exhibited a low leakage current density of ∼10
−8 A/cm
2. Electron spin resonance measurements and defect chemistry analysis show that the average valence increase of Mn by oxidation treatment (the annealing in air) absorbs electron hole, the carrier of the leakage current, which is suggested to be the origin of the low leakage current observed for Mn-KNN crystals.
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Takayuki WATANABE, Jumpei HAYASHI, Takanori MATSUDA, Toshihiro IFUKU, ...
2010 年 118 巻 1380 号 p.
717-721
発行日: 2010/08/01
公開日: 2010/08/01
ジャーナル
フリー
This paper reports on the piezoelectric anomalies at the temperature or composition-induced ferroelastic phase transitions of tungsten bronze ferroelectrics. First, the temperature-dependent piezoelectric properties of Sr
1.9Ca
0.1NaNb
5O
15 (SCNN) ceramics were characterized using a resonance/anti-resonance method. SCNN has a ferroelastic phase transition manifested by a broad dielectric peak in the temperature range of −60°C to 20°C. The electromechanical coupling factor and elastic compliance showed the maximum at −40°C, increasing the transverse piezoelectric constant (
d31) by 38% compared with the room temperature value. Tungsten bronze ferroelectrics follow a trade-off relationship between the longitudinal piezoelectric constant (
d33) and the Curie temperature, while SCNN deviates significantly from the trend curve. This deviation is attributed to the ferroelastic phase transition close to room temperature.
Second, the ferroelastic phase transition was investigated for epitaxial films of (1 −
x)(Sr
3Ba
2)Nb
10O
30–
xBa
4Bi
2/3Nb
10O
30 as a function of the composition. A careful structural analysis by X-ray diffraction revealed that there is a ferroelastic phase boundary between tetragonal and orthorhombic crystals at
x = 0.06–0.3. The electric field-induced strain and the relative dielectric constants characterized at 80 K for the epitaxial films increased in the vicinity of the phase boundary composition. These results suggest that engineering the ferroelastic phase transition is an approach to improving the piezoelectric properties of lead-free tungsten bronze ferroelectrics.
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