Journal of the Ceramic Society of Japan
Online ISSN : 1348-6535
Print ISSN : 1882-0743
ISSN-L : 1348-6535
Volume 121, Issue 1416
(August)
Displaying 1-39 of 39 articles from this issue
Feature: Evolution of Dielectric Materials II: Preface
Feature: Evolution of Dielectric Materials II: Papers
  • Hiroki TANIGUCHI, Yasuhiro FUJII, Mitsuru ITOH
    2013 Volume 121 Issue 1416 Pages 579-582
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    A domain structure in periodically poled stoichiometric LiNbO3 was observed by confocal micro-Raman scanning spectroscopy. The 180°-domain, which is nominally invisible by Raman scattering due to equivalency of Raman selection rule for adjacent domains, was clearly visualized with a spatial resolution of 460 nm. At domain walls, an enhancement of Raman intensity was observed in optical modes that are closely related to the Nb–O bond, while there was no significant change in Li-ion related modes. Nb–O covalent bonds would be deformed by opposite ferroelectric displacements of ions across domain walls, to modify an electric polarizability of the Nb-ion related modes.
    Download PDF (1871K)
  • Takayuki KOMATSU, Takashi OIKAWA, Tsuyoshi HONMA
    2013 Volume 121 Issue 1416 Pages 583-588
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    BaTiO3 crystals synthesized through the crystallization of 40BaO–40TiO2–15SiO2–5Al2O3 glass were characterized from Raman scattering spectrum, second harmonic generation (SHG), and polarization measurements. The structure of BaTiO3 nanocrystals (~70 nm) formed initially was suggested to be pseudo-cubic (small tetragonality), and perovskite-type ferroelectric BaTiO3 crystals were formed in the heat-treatments at high temperatures of ~930°C. The lines consisting of BaTiO3 crystals were patterned at the surface of CuO-doped glass by irradiations of continuous-wave Yb:YVO4 lasers with a wavelength of 1080 nm. It was confirmed that BaTiO3 being present in the laser-irradiated parts exhibits SHGs and, in particular, BaTiO3 formed in the laser ablation region has a tetragonal structure and a Curie temperature of ~135°C.
    Download PDF (1300K)
  • Ichiro FUJII, Ryuta MITSUI, Kouichi NAKASHIMA, Nobuhiro KUMADA, Hisato ...
    2013 Volume 121 Issue 1416 Pages 589-592
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    0.3BaTiO3–0.1Bi(Mg1/2Ti1/2)O3–0.6BiFeO3 ceramics were either doped with vanadium or sintered in calcined powder with the same composition. Compared to an undoped ceramic sintered without the calcined powder, both ceramics showed reduced leakage current densities (lower than 1 × 10−7 A/cm2) and absence of dielectric relaxation behaviors observed in frequency- and temperature-dependent dielectric measurements. The Curie temperatures of both samples were higher than 460°C. The maximum field-induced strain over the applied field, Smax/Emax, of 366 pm/V for the undoped ceramic sintered without the calcined powder increased to 455 and 799 pm/V for the V-doped sample and the sample sintered with the calcined powder, respectively. The increase was discussed with reduced concentrations of bismuth vacancy–oxygen vacancy defect dipoles.
    Download PDF (158K)
  • Minoru OSADA, Makoto KOBAYASHI, Masato KAKIHANA
    2013 Volume 121 Issue 1416 Pages 593-597
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    High-quality rutile TiO2 nanocrystals have been synthesized by a simple hydrothermal treatment of a watersoluble titanium–glycolate complex at 200°C. The obtained samples were composed of rod- or whisker-like nanocrystals. The aspect ratios of these nanocrystals could be controlled by adding glycolic acid. Combined characterizations with X-ray diffraction, Raman scattering and high-resolution transmission electron microscopy revealed the formation of highly phase-pure and well-crystallized rutile nanorods/nanowhiskers with the c-axis orientation. Room-temperature dielectric measurements indicated that the permittivity for the rutile nanowhiskers is ~150 at 100 kHz, which is higher than that for the bulk rutile powder. These observations pave a way for morphological controlled rutile nanocrytals to find a broad class of technological uses.
    Download PDF (2374K)
  • Ken NISHIDA, Minoru OSADA, Joe SAKAI, Nobuaki ITO, Takashi KATODA, Rik ...
    2013 Volume 121 Issue 1416 Pages 598-601
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Resonant Raman spectroscopy was applied to evaluate oxygen vacancies in PbTiO3–x thin films that were heat treated in a hydrogen atmosphere at various temperatures. Additional mode related to oxygen vacancies occurred in the resonant Raman measurement condition, and its intensity was in proportion to the oxygen vacancy concentration. This correlation offers a simple and useful probe for oxygen vacancies in oxide-based devices.
    Download PDF (506K)
  • Eisuke MAGOME, Yoshihiro KUROIWA, Chikako MORIYOSHI, Ichiro FUJII, Kou ...
    2013 Volume 121 Issue 1416 Pages 602-605
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    KNbO3 (KN)/BaTiO3 (BT) nanocomposite ceramics, in which a BT nanoparticle is thinly coated with KN crystals through the heteroepitaxial interface, are heat-treated at 1000°C for 10 h, and the crystal structures are investigated by synchrotron radiation powder diffraction. The Rietveld analysis based on the multicomponent models reveals that the volumes of gradually distorted tetragonal components of BT are significantly decreased and the BT-KN solid solutions emerge in the nanocomposites by the heat-treatment. The suppression of the piezoelectric response in the heat-treated nanocomposites compared with the as-synthesized ones is attributed to these changes in the crystal structure. The core/multishell structure model for the ceramic grain is proposed, and the changes in the crystal structure are revealed to be caused at the heteroepitaxial interface regain between BT and KN.
    Download PDF (1962K)
  • Susumu TAKAHASHI, Yusuke IMAI, Akinori KAN, Yuji HOTTA, Hirotaka OGAWA
    2013 Volume 121 Issue 1416 Pages 606-610
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    The dielectric and thermal properties of isotactic polypropylene/magnesium oxide (0–30 vol %) composites were investigated. The dielectric constant of the composite material increased from 2.3 to 3.2 on increasing the MgO content and the observed variation of the dielectric constant with the MgO fraction was in good agreement with the Bruggeman mixing model. Low dielectric losses at microwave frequencies, on the order of 10−4, were obtained using highly crystalline MgO as the filler, and it was also found that the use of larger MgO particle sizes led to further reductions in the dielectric loss. The absolute value of temperature coefficient of the dielectric constant as well as the coefficient of thermal expansion decreased with increasing MgO content, while thermal conductivity increased with increasing MgO content in a manner which could be predicted using the Maxwell-Garnett mixing model.
    Download PDF (1674K)
  • Masanobu NAKAYAMA, Shota HOTTA, Tomoaki NAKAMURA, Toshihiro KASUGA
    2013 Volume 121 Issue 1416 Pages 611-613
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    First-priciples density functional theory (DFT) techniques are used to provide atomic-scale insight into the surface structures and crystal morphologies of cubic barium titanate, BaTiO3. Relaxed surface structures and energies are calculated for 3 low index planes and resulting equilibrium morphology based on Wulff’s theorem with {001} and {011} faces were constructed. The calculated surface energies are strongly dependent on the coordination loss of TiO6 octahedra at the surface. The optimized structure at the low-energy surfaces shows that only atoms at 1st perovskite layer are displaced from ideal position, while no significant displacements are indicated. On the other hand, the Bader charge analysis shows that the ionicity of whole the cations in the slab (7 perovskite layers) is larger than that in the bulk. Therefore, change of electric property is expected at the surface region, which is not due to the surface reconstruction, but to the change of electronic structure.
    Download PDF (1221K)
  • Yoshikatsu KAWABATA, Wataru SAKAMOTO, Kenji YOSHIDA, Takashi IIJIMA, M ...
    2013 Volume 121 Issue 1416 Pages 614-618
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Multiferroic Pb(Zr,Ti)O3/CoFe2O4/Pb(Zr,Ti)O3 layered thin films were synthesized on Pt/TiOx/SiO2/Si substrates by chemical solution deposition using metal–organic precursor solutions. Layered composite films composed of polycrystalline perovskite Pb(Zr0.52Ti0.48)O3 and spinel CoFe2O4 phases with no secondary phases were successfully synthesized by controlling conditions such as the coating process. The layered structure of the Pb(Zr0.52Ti0.48)O3/CoFe2O4/Pb(Zr0.52Ti0.48)O3 was confirmed by scanning electron microscope observations. These layered films exhibited sufficiently high insulating properties, as well as ferroelectric polarization (P)-electric field (E) and ferromagnetic magnetization (M)-magnetic field (H) hysteresis loops at room temperature. Typical ferroelectric oxide strain behavior was observed under a driving AC (alternate current) field. Furthermore, due to magnetoelectric interaction between the ferroelectric and ferromagnetic (magnetostrictive) layers, the ferroelectric properties of the films altered under an applied magnetic field (approximately 0.5 T).
    Download PDF (2554K)
  • Naonori SAKAMOTO, Kotaro OZAWA, Tomoya OHNO, Takanori KIGUCHI, Takeshi ...
    2013 Volume 121 Issue 1416 Pages 619-622
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    LaNiO3 (LNO) is one of an excellent candidate for oxide electrodes especially for perovskite ferroelectric films since it is perovskite type crystal structure, and therefore it is suitable for lattice matching with conventional perovskite ferroelectrics, Pb(Zr,Ti)O3 (PZT), BaTiO3 (BTO), etc. We have been investigating an effect of thermal expansion of the LNO film as PZT/LNO/Si and BTO/LNO/Si structures, where ferroelectric and piezoelectric properties can be improved by a compressive thermals stress implied from the LNO layer to the ferroelectric films. The ferroelectric films also shows high [001] orientation owing to [100] orientation of the LNO film. In the present study, microstructures and crystal structures of the LNO films fabricated on Si substrates by CSD method is investigated by X-ray Diffraction (XRD), field emission scanning electron microscopy (FE-SEM) and transmission electron microscopy (TEM) in order to understand self-orientation along [100] perpendicular to the film plane. The results obviously indicate that the 1 layer deposited LNO film has almost no orientation, whereas it shows tendency of orientation of [100] perpendicular to the film plane when the layer number increased (upto 4 layers). TEM analysis also shows in-plane tensile stress applied to the LNO film is effectively decreased by porous LNO structure, which leads in-plane compressive stress to the ferroelectric films prepared on the LNO films.
    Download PDF (750K)
  • Kazuya TABUCHI, Hajime NAGATA, Tadashi TAKENAKA
    2013 Volume 121 Issue 1416 Pages 623-626
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Bismuth potassium titanate, (Bi1/2K1/2)TiO3 (BKT), ceramics were fabricated using KHCO3 as a starting material to control K amount precisely. Then, we fabricated (Bi1/2K(1+x)/2)TiO3 [BKT-10000x] ceramics to clarify an effect of poor or excess K ions in BKT ceramics for physical and electrical properties. The BKT-10000x ceramics were prepared by a conventional ceramic fabrication process, and then high density ratios of about 97% were obtained in all BKT-10000x ceramics (10000x = −10–100). The precise control of K amount did not strongly affect the sinterability for BKT ceramics. On the other hand, electrical properties such as ferroelectric, strain and piezoelectric behaviors of BKT ceramics are very sensitivity to the amount of K ions. Therefore, it is very important to control the amount of K in BKT ceramics.
    Download PDF (1795K)
  • Takahisa SHIRAISHI, Hiro EINISHI, Shintaro YASUI, Mutsuo ISHIKAWA, Tom ...
    2013 Volume 121 Issue 1416 Pages 627-631
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Epitaxial (KxNa1−x)NbO3 films with 3 µm in thickness were deposited at 240°C on (100)cSrRuO3//(100)SrTiO3 substrates by hydrothermal method. XRD patterns and Raman spectra were systematically changed with increasing x values. XRD patterns and Raman spectra was not dramatically changed by the annealing treatment at 600°C for 10 min under O2 atmosphere. On the other hand, the electrical and piezoelectric properties were improved by this annealing treatment; leakage current density was diminished and longitudinal piezoelectric response was increased to 69 pm/V at x = 0.51.
    Download PDF (3458K)
  • Yuuki KITANAKA, Yuji NOGUCHI, Masaru MIYAYAMA, Yutaka KAGAWA, Chikako ...
    2013 Volume 121 Issue 1416 Pages 632-637
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    The behaviors of intrinsic unit-cell strains under applied electric fields (E) along the ⟨100⟩ direction were investigated for rhombohedral Pb(Zn1/3Nb2/3)O3–(6–7%)PbTiO3 (PZN–PT) single crystals by in-situ high-energy synchrotron radiation X-ray diffraction study. The E-induced unit-cell strains accompanied with a reversible phase transition from rhombohedral to tetragonal via two monoclinic phases agree well with the macroscopic strain properties observed for the crystals. The structural analyses using the single-crystal X-ray diffraction and domain observations with piezoresponse force microscopy lead to a conclusion that the E-induced unit-cell strains are mainly responsible for the high piezoelectric performance of the PZN–(6–7%)PT single crystals.
    Download PDF (2592K)
  • Takanori KIGUCHI, Tomohito TSUKAMOTO, Cangyu FAN, Masahiko NISHIJIMA, ...
    2013 Volume 121 Issue 1416 Pages 638-643
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    This study investigated the effect of excess PbO and post-annealing on the crystallinity and the microstructure of Pb(Mg1/3Nb2/3)O3 (PMN) epitaxial thin films. PMN thin films were deposited on SrTiO3 (STO) (001) substrates using a chemical solution deposition (CSD) process with rapid thermal annealing (RTA) of spin-coated metallo-organic decomposition (MOD) solutions. The nominal film composition was Pbx(Mg1/3Nb2/3)O3 (x = 1.0 or 1.1). All films showed the (001)PMN//(001)STO, [001]PMN//[001]STO epitaxial relationship and were single phase perovskite PMN without any pyrochlore phases. The Pb1.1(Mg1/3Nb2/3)O3/SrTiO3 thin film post-annealed at 973 K with facing treatment showed the highest crystallinity of 0.8° in full width at half maximum (FWHM) of the 002PMN rocking curve. Transmission electron microscopy (TEM) revealed PbO nanoparticles on the surface of the PMN thin films. The film composition was almost stoichiometric. On the other hand, the Pb1.1(Mg1/3Nb2/3)O3/SrTiO3 thin film post-annealed at 973 K without facing treatment showed crystallinity of 1.0° and no PbO nanoparticles. The film composition was almost stoichiometric. These results indicate that the excess PbO is not incorporated into the PMN films. Instead, it volatizes from the film surface, which improves the crystallinity and inhibits the PMN decomposition.
    Download PDF (2455K)
  • Tohru MORIYAMA, Akinori KAN, Hirotaka OGAWA
    2013 Volume 121 Issue 1416 Pages 644-648
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    The crystal structure, piezoelectric and ferroelectric properties of the Bi0.5−0.5xNa0.5−0.5xSrxTi1−xZrxO3 (BNSTZ) ceramics were characterized in this study. From the variations in the lattice parameters, the solubility limit of the BNSTZ ceramics was determined to be x = 0.075. The crystal structure refinement revealed that the distortion of (Bi, Na and Sr)O12 polyhedron decrease with increasing x and such the variation in the distortion exerts an influence on the decrease in remnant polarization from 35 to 28 µC/cm2. Although the slight shifts of the depolarization temperature (Td) and rhombohedral-tetragonal phase transition temperature (TR-T) to lower temperature were recognized, it suggested that the shift of Td is predominant for the increase in dielectric constant at room temperature which leads to the enhancement of the d33 value. As a result, the d33 and kp values were 85 pC/N and 18.7%, respectively at x = 0. 075.
    Download PDF (1155K)
  • Hitoshi OHSATO, Jeong-Seog KIM, Chae-Il CHEON, Isao KAGOMIYA
    2013 Volume 121 Issue 1416 Pages 649-654
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Cordierite (Mg2Al4Si5O18) is a candidate for millimeter-wave dielectrics, and has two polymorphs due to ordering of Si and Al ions on Si/AlO4 tetrahedra: disordered high symmetry form called as indialite and ordered low symmetry form cordierite. Indialite/cordierite glass ceramics exhibited much higher Qf value of 200,000 GHz than conventional solid state reaction ceramics of 40,000 GHz, which were fabricated by crystallization of glass pellet. The glass ceramics having indialite as a dominant phase showed high Qf. The crystal phases are analyzed by Rietveld method. In this paper, the ordering ratios of indialite and cordierite are estimated by the volumes and covalencies of Si/AlO4 tetrahedra.
    Download PDF (5308K)
  • Hiroshi MAIWA
    2013 Volume 121 Issue 1416 Pages 655-658
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Barium titanate (BaTiO3, BT) ceramics with various grain sizes were prepared by hot isostatic pressing (HIP) and post-annealing. The dielectric and piezoelectric properties were evaluated. Grain growth was suppressed in the ceramics prepared by HIP. The average grain sizes of the ceramics were controlled by changing the post-annealing temperature. Dense BT ceramics with submicron grain sizes were obtained by annealing below 1000°C. The highest piezoelectric d33 coefficient, 172 pC/N, measured by a d33 meter was obtained in the BT ceramics prepared by HIP at 900°C under the pressure of 200 MPa and annealed at 1100°C in air for 48 h. The dynamic electric field-induced strain increased with the annealing temperature, and 700 pm/V of Strain/Field was obtained in the BT ceramics prepared by HIP under the same conditions and annealed at 1300°C in air for 48 h.
    Download PDF (1676K)
  • Jong-Min OH, Takuya HOSHINA, Hiroaki TAKEDA, Takaaki TSURUMI
    2013 Volume 121 Issue 1416 Pages 659-663
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    We designed advanced transparent-comb-electrode photonic crystals (TCE PCs) to use the longitudinal electro-optic (LEO) effect, so they are composed of Al-doped ZnO (AZO) layers, which serve as internal/external electrodes, and centered (Pb,La)(Zr,Ti)O3 (PLZT) layers, which serve as EO material. The simulated transmittance spectra of a multilayer interference (MLI) model revealed the conditions in the AZO and PLZT film thicknesses and the AZO/PLZT period number for a narrow photonic band gap (PBG). The TCE PCs consisted of four periods of AZO/PLZT, and it was fabricated by RF magnetron sputtering through metal mask patterning. Finally, a refractive index change induced by the LEO effect of the PLZT layers was accomplished by applying the voltage dependence of transmittance spectra that were well fitted with a revised (MLI) model considering light absorption and scattering. The PCs exhibit large refractive index changes of 1.3 × 10−2 and 2.9 × 10−2 at DC voltages of 4 and 8 V, respectively. The corresponding PBG shifts were 3.9 and 8.5 nm, implying high a PBG tunability of ~1 nm/V.
    Download PDF (2533K)
  • Muneyasu SUZUKI, Jun AKEDO
    2013 Volume 121 Issue 1416 Pages 664-669
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Self-supported (Bi0.5Na0.5)TiO3 (BNT) dense ceramic films with a thickness of approximately 20 µm have been fabricated by use of an aerosol deposition method with heat treatment and sapphire single crystal substrates. Investigations of their constitution phase and crystal structure, observation of their microstructure, and measurement of polarization properties and leakage current density (J) were performed. Wlile the films heat-treated at 800 and 900°C in air indicated the low J ≈ 10−7 A/cm2 at 150 kV/cm, the sintered bulks and the films annealed at 900°C in the BNT starting raw powder showed the relatively high J of approximately 10−6 A/cm2 at 150 kV/cm. These films heat-treated at 800 and 1000°C in air and sintered bulks showed the almost the same coercive field (Ec) of approximately 57 kV/cm (in the 56 to 58 kV/cm range), and the films heat-treated at 1000°C in air exhibited good polarization properties and remanent polarization (Pr) of 25 µC/cm2. The AD method is proposed to be effective for obtaining self-supported BNT thick films with good saturated hysteresis loops and low J.
    Download PDF (2196K)
  • Takashi IIJIMA, Naoto KOCHI, Soichiro OKAMURA
    2013 Volume 121 Issue 1416 Pages 670-674
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Micromachined ultrasonic transducers (MUTs) are attractive devices for medical imaging systems. In order to observe biological tissue images clearly, ultrasonic waves above 100 MHz in a thickness oscillation mode are required. Therefore, the film thickness of the piezoelectric materials like lead zirconate titanate (PZT) is required less than 10 µm. In this study, to adapt the demand of high frequency ultrasonic, thickness mode transducers using the PZT thick film were prepared with a CSD process, a FEM simulation, and a micro fabrication process. The effects of the side length of PZT thick film structure and the Si substrate thickness on the electrical impedance properties were investigated, because the mechanical oscillation was equivalent to the electrical impedance oscillation. To reduce a series of resonance frequency like a composite resonator, a back side of the Si substrate was removed with deep Si etching process. The PZT thick film with Si substrate cavity structure showed sharp fundamental thickness mode resonance peak at around 168 MHz. Therefore, the fabricated device structure is applicable to the high frequency ultrasonic medical imaging system in the future.
    Download PDF (660K)
  • Takeshi YOKOTA, Rintaro AOYAGI, Manabu GOMI
    2013 Volume 121 Issue 1416 Pages 675-678
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    We investigated the thermoelectric properties of doped multiferroic material: Co-doped BiFeO3 (BFO) and related materials: Bi24CoO37 and Bi24CoO37–BFO composite systems. Because of their insulating nature, the BFO-based samples showed high Seebeck coefficients compared with other oxides being explored as candidates for new thermoelectric materials such as NaCo2O4, and La0.9Sr0.99Ca0.11CoO4. On the other hand, the Bi24CoO37 sample showed high conductivity. The Bi24CoO37 (20%)–BFO composite sample showed a high power factor, because of its high conductivity and high Seebeck coefficient. These results indicated that the BFO matrix plays an important role in maintaining a high Seebeck coefficient, and that Bi24CoO37 works as a conductive pass on this system.
    Download PDF (343K)
  • Tohru MORIYAMA, Akinori KAN, Hirotaka OGAWA
    2013 Volume 121 Issue 1416 Pages 679-683
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    In this study, Bi0.5+0.5xNa0.5−0.5xTi1−xMn0.75xMo0.25xO3 (BNTMM) ceramics were synthesized and the influence on their crystal structure and ferroelectric properties of the Bi, Mn and Mo substitutions for Na and Ti was investigated. Based on variations in the lattice parameters, the solubility limit was determined to be x = 0.0075. From crystal structural refinement in the single phase region, it was found that the Bi, Mn and Mo substitutions for Na and Ti may exert an influence on the covalency of B–O (B = Ti, Mn, and Mo) and (Bi,Na)–O bonds, leading to a structural distortion of BO6 octahedra and (Bi,Na)O12 polyhedra, which may affect the remnant polarization (Pr). The highest Pr value of 40.3 µC/cm2 was obtained for x = 0.0075 and the corresponding coercive field Ec was 70.3 kV/cm.
    Download PDF (1714K)
  • Hirotaka OGAWA, Tohru MORIYAMA, Akinori KAN, Yuki UEDA
    2013 Volume 121 Issue 1416 Pages 684-689
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    The effects of Mn2O3 addition on the ferroelectric and piezoelectric properties of (K0.474Na0.474Li0.052)(Nb0.948Sb0.052)O3 (KNLNS) defined as KNLNS(Sb2O3) and KNLNS(Sb2O5) which was synthesized using Sb2O3 or Sb2O5 powders have been investigated. From X-ray powder diffraction profiles, the coexistence of orthorhombic–tetragonal phases, which have a morphotropic phase boundary (MPB), is shown in the KNLNS–xmol %Mn2O3 ceramics. The addition of Mn2O3 to the KNLNS(Sb2O5) ceramic led to significant improvements in ferroelectric properties, piezoelectric property, and bulk density; moreover, the orthorhombic–tetragonal phase transition temperature was shifted to room temperature. As a result, the d33 values of the KNLNS(Sb2O5)–xmol %Mn2O3 ceramics increased, ranging from 187 to 264 pC/N, whereas the d33 values of KNLNS(Sb2O3)–xmol %Mn2O3 were decreased by the Mn2O3 addition. These results indicate that the KNLNS(Sb2O5)–xmol %Mn2O3 ceramics may be a promising candidate material for lead-free piezoelectric ceramics.
    Download PDF (1325K)
  • Tomoaki YAMADA, Itaru TAKUWA, Takafumi KAMO, Takashi IIJIMA, Masahito ...
    2013 Volume 121 Issue 1416 Pages 690-692
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    The in-plane compressed (001)-epitaxial (Ba,Sr)TiO3 [BST] films with different Ba/Sr ratio were fabricated on (001)cSrRuO3/(001)SrTiO3 and (001)cSrRuO3/(001)(La,Sr)(Al,Ta)O3 by RF magnetron sputtering. Regardless of the Ba/Sr ratio, the in-plane compressive strain shifts the ferroelectric phase transition to higher temperatures; however, the magnitude of its impact varies by the Ba/Sr ratio. With increasing the Ba/Sr ratio, the sensitivity to the strain becomes larger, which can be associated with the compositional dependence of Curie–Weiss constant, electrostrictive constant and elastic constant of BST.
    Download PDF (807K)
  • Kouichi NAKASHIMA, Ichiro FUJII, Satoshi WADA
    2013 Volume 121 Issue 1416 Pages 693-697
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Potassium niobate (KNbO3) was prepared using a solvothermal method. The synthesis was conducted using niobium oxide (Nb2O5) and potassium hydroxide (KOH) as starting materials and ethanol as the reaction medium. X-ray diffraction (XRD) confirmed the presence of perovskite KNbO3 particles and indicated that the lattice of the KNbO3 was orthorhombic. The morphology of the KNbO3 was investigated using scanning electron microscopy (SEM), transmission electron microscopy (TEM), and scanning transmission electron microscopy (STEM). Energy-dispersive X-ray (EDX) spectrometry was conducted with TEM/STEM, which clearly revealed that the KNbO3 particles were nanosized and possessed a cubic shape with sharp-edged corners. The STEM-EDX observations indicated that all three elements of potassium (K), niobium (Nb), and oxygen (O) were distributed homogeneously across the nanocubes. Only K, Nb, and O were detected in the EDX spectrum of the KNbO3 powders obtained. Thus, KNbO3 nanocubes were successfully prepared using a solvothermal method at low temperature.
    Download PDF (2137K)
  • Kazuki MAEDA, Ichiro FUJII, Kouichi NAKASHIMA, Gakuyo FUJIMOTO, Kazuhi ...
    2013 Volume 121 Issue 1416 Pages 698-701
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Porous barium titanate (BaTiO3, BT) ceramics were prepared by a conventional sintering method using two kinds of BT particles. The relationship between pore structure (porosity and pore size) of BT ceramics and their sensor properties was investigated. Since a piezoelectric constant d33 of BT depends largely on the pore structures, the microstructure control of porous BT ceramics is important to improve the figure-of-merit of piezoelectric stress sensor application (g33/ρ). In this study, the maximal piezoelectric g33 constant value of 14.8 × 10−3 V·m·N−1 and the maximal g33/ρ value of 3.14 × 103 V·m4·N−1·g−1 were obtained at a porosity of approximately 23%.
    Download PDF (2119K)
Papers
  • Man Gyu HUR, Takaki MASAKI, Byung Ki CHOI, Jin Hyoung LEE, Kwang Choon ...
    2013 Volume 121 Issue 1416 Pages 702-705
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    A thin silicon dioxide (SiO2) layer coating on the surfaces of 150 and 300-nm BaTiO3 particles was applied by a hydrothermal hydrolysis method. Sodium silicate (Na2SiO3) was used as a raw material, and the concentration, temperature, and pH were controlled. The surface-treated BaTiO3 particles were dried at 120°C and fired at 650°C for 30 min. The thickness of the coated layer was about 4.52 nm, and the layers were homogenously coated onto the BaTiO3 particles. The structure and morphology of the coated layers were analyzed by XRD, FE-SEM, TEM, and EDX.
    Download PDF (2310K)
  • Tomofumi YAMADA, Rintaro AOYAGI, Takeshi YOKOTA, Manabu GOMI
    2013 Volume 121 Issue 1416 Pages 706-709
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    High-temperature thermoelectric properties of BaFexTi1−xO3−δ (BFT100x) ceramics in air were investigated. Crystal structures of BFT100x ceramics were found to be a mixture of tetragonal or cubic provskite and hexagonal BaTiO3 phases for x = 0.05–0.20, and a single phase of hexagonal BaTiO3 for x > 0.30. X-ray diffraction pattern of BFT90 revealed a mixture of hexagonal BaTiO3 and monoclinic Ba2Fe2O5 phases. Conductivity of BFT100x increased with increase in temperature and Fe concentration. This increase in conductivity originated from the substitution of Ti4+ with Fe3+, which increased the oxygen vacancy of the system. A maximum conductivity of 3.1 × 102 S/m was obtained for BFT90 at 1100 K. Activation energy calculated by resistivity decreased with increase in Fe concentration. Seebeck coefficient of BFT100x increased with increase in temperature and decreased with increase in Fe concentration for x = 0.40–0.80. These results suggested an increase in carrier concentration. Seebeck coefficient of BFT90 was larger than that of BFT80, which is attributable to the mixed structure of BFT90. Power factor of BFT100x increased with increase in temperature and Fe concentration. These results suggested that BaFexTi1−xO3−δ with mixed structure of hexagonal and monoclinic phases have good potential for enhancing the thermoelectric properties of BaFexTi1−xO3−δ ceramics.
    Download PDF (147K)
  • Shunsuke MURAI, Tomohiko MATOBA, Christopher T. NELSON, Takuya KOMINE, ...
    2013 Volume 121 Issue 1416 Pages 710-713
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    We have prepared composites with anisotropic microstructure consisting of silver nanoparticles and zinc oxide pillars using an oblique angle deposition technique, and examined the optical response originating from their anisotropic morphology. The sample was obtained in three steps. First, the assembly of silver nanoparticles was prepared on a silica glass substrate by electron-beam deposition of the silver thin film and subsequent heat treatment. Next, zinc oxide was obliquely grown by using a pulsed laser deposition. Finally the zinc oxide was crystallized by the post annealing to make an array of inclined pillars grown on the top of the silver nanoparticles. The structure and morphology of the composites were elucidated by a combination of X-ray diffraction analysis and transmission electron microscopy. Optical rotation spectroscopy clarifies that the composite shows optical birefringence due to its inclined pillar morphology. The optical rotation spectrum exhibits two peaks, one being associated to the localized surface plasmon resonance of the silver nanoparticles and the other the excitons in the zinc oxide pillars. The present fabrication method is simple and can be applied to obtain anisotropic composites with relatively large dimensions.
    Download PDF (762K)
  • Kiyoko SAKAMOTO, Takuya NOMOTO, Shunro YAMAGUCHI, Ichiro FUJIHARA, Kat ...
    2013 Volume 121 Issue 1416 Pages 714-722
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    In this study, we investigated the hardening processes and compressive strengths of binary and ternary calcium phosphate cements based on β-tricalcium phosphate [Ca3(PO4)2] (β-TCP) ground by a mortar grinder. The cements were prepared by adding tetracalcium phosphate [Ca4(PO4)2O] (TTCP) and/or calcium hydrogenphosphate dihydrate [CaHPO4·2H2O] (DCPD) to the ground β-TCP, which hardened on mixing with disodium hydrogenphosphate [Na2HPO4] aqueous solution. The binary cement β-TCP/TTCP with a molar ratio of 2:1 showed a compressive strength of 35 MPa after hardening, which is based on a 1-day acid–base reaction. The ternary cement β-TCP/TTCP/DCPD with molar ratios of β-TCP (50–60%), TTCP (20–30%), and DCPD (14–20%,) showed early hardening and an adequate compressive strength of 30–43 MPa after a 1-day reaction. In particular, the ternary cement with a molar ratio of 3:2:1 (β-TCP:TTCP:DCPD) showed compressive strengths of 17, 43, and 56 MPa after 1 h in air, and 1 and 7 days’ soaking in saline solution, respectively. These ternary cements hardened to give well-connected acicular apatite crystals. The hardening process involved hydrolysis of the ground β-TCP and acid–base reactions of β-TCP/TTCP and DCPD/TTCP.
    Download PDF (3125K)
  • Masanobu NAKAYAMA, Takashi OKAJIMA, Yoshihiro YAMAMOTO, Shinji BABA, K ...
    2013 Volume 121 Issue 1416 Pages 723-729
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Supplementary material
    Development of all solid-state Li secondary based on the use of dry polymer or inorganic electrolytes is vital as they will be free of solvent leakages and improve inflammability. However, both are still under development for many years due to low ionic conductivity, poor mechanical property and/or large internal impedance associated to poorly defined interfaces. In this paper, we report on a preparation and physicochemical property of mesoporous silica (MPS)/Li conductive polyethylene oxide (Li-PEO)-based polymer hybrid electrolytes (MPS+Li-PEO), and electrochemical performance of the Li/MPS+Li-PEO/LiFePO4 cell. The hybrid electrolytes showed an improvement of Li+ transportation number and a decrease of melting point and glass transition temperature, indicating a positive hybrid effect, or deviation from rule-of-mixtures behavior. The Li/MPS+Li-PEO/LiFePO4 cell showed a stable charge–discharge capacity of >70 mA h g−1 for 100 cycles at moderate temperature of 60°C and rate of 0.2 C, whereas severe capacity fade began after several of cycles for the cell using conventional Li-PEO electrolyte. AC impedance measurements revealed that the interface Li exchange between electrode and electrolytes related to the stable cyclic performance for the cell using hybrid electrolytes.
    Download PDF (1482K)
  • Hitoshi NISHIJIMA, Ryosuke MAKI, Yoshikazu SUZUKI
    2013 Volume 121 Issue 1416 Pages 730-733
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    In this study, we have tried to prepare porous Al2TiO5 ceramics with potato starch as a pore-forming agent at relatively low sintering temperatures by reactive sintering method using fine-grained starting materials. α-Al2O3 powder (0.1 µm) and TiO2 rutile powder (2 µm) were wet-ball milled in ethanol for 2 h in a planetary ball-mill. The mixed powder was blended with 5–30 wt % of potato starch powder in an agate mortar with ethanol. Green samples with no binder were sintered at 1300–1500°C for 2 h in air. The sample contained finer closed pores (<1 µm) as well as the larger pores (5–80 µm). The finer microstructure formation can be explained by (1) the local heating effect via the combustion of potato starch, and (2) water vapor-assisted effect.
    Download PDF (1803K)
  • Noriya IZU, Gunter HAGEN, Franz SCHUBERT, Daniela SCHÖNAUER-KAMIN ...
    2013 Volume 121 Issue 1416 Pages 734-737
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Planar resistive type SO2 sensors based on V2O5/WO3/TiO2 (VWT) have been reported to respond well to SO2 but with large cross-effects of NO and NH3. In this study, we added a porous Pt/alumina cover layer on a VWT film in order to decrease the cross sensitivities. The sensor response to SO2 is hardly affected by the Pt/alumina layer in the case of VWT sensor with 3.0 wt % V2O5 with Au electrodes, while the Pt/alumina layer affects the response of other VWT sensors. The VWT sensor (3.0 wt % V2O5) with Au electrodes with the porous Pt/alumina cover layer shows much smaller responses to CO, H2, H2O, NH3, and NO compared with the sensor without Pt/alumina cover layer. The porous Pt/alumina cover layer has a potential to improve the selectivity of the VWT sensor.
    Download PDF (1591K)
  • Geun-Hyoung LEE
    2013 Volume 121 Issue 1416 Pages 738-740
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    ZnO crystals with controllable morphology were synthesized by employing the different source materials. A simple thermal evaporation technique was employed to synthesize ZnO crystals. Morphologies such as tetrapods and inverted cone-shaped rods were realized experimentally through thermal evaporation of Zn and ZnS powder, respectively. The morphology of ZnO crystals could also be controlled by designing the source material. Peculiar ZnO tetrapods with inverted cone-shaped legs were obtained via thermal evaporation of a mixture of Zn and ZnS powder mixed with a certain ratio. The intensity of green emission in the photoluminescence spectrum increased with the increase in the ratio of ZnS to Zn in the source material.
    Download PDF (551K)
Notes
  • Yusuke YAMAMOTO, Hirotaka YOKOTA, Natsuko KOJIMA, Shigenobu HAYASHI, T ...
    2013 Volume 121 Issue 1416 Pages 741-744
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Cubic silicon nitride (c-Si3N4) was prepared at 37–38 GPa and ~1773 K by shock compression of residues of polysilazane, perhydropolysilazane (PHPS), pyrolyzed at 873, 1073 and 1273 K for 2 h. The residues pyrolyzed at 873 and 1073 K were amorphous materials, while the residue pyrolyzed at 1273 K consisted mainly of crystalline α-Si3N4. The relative amount of c-Si3N4 was the smallest in the shock-compressed product of the residue pyrolyzed at 1273 K, indicating that use of amorphous residues is advantageous for formation of c-Si3N4.
    Download PDF (409K)
  • Linlin YANG, Yonggang WANG, Yujiang WANG, Xiaofeng WANG, Gaorong HAN
    2013 Volume 121 Issue 1416 Pages 745-748
    Published: August 01, 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Single-crystal PbMoO4 nanorods with diameters of 70–80 nm and lengths of about 300–400 nm have been successfully obtained via a surfactant-free sonochemical method. The obtained samples were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and electron diffraction (ED). It is found that the precursor played a key role in the preparation of PbMoO4 nanorods. PbMoO4 nanorods can be successfully obtained when PbCrO4 nanorods were used as precursor. Once PbCrO4 were replaced with Pb(NO3)2, PbMoO4 nanoparticles were formed. The synthesis mechanism was also discussed. It is rational to expect that some other one-dimensional metal molybdates may also be synthesized by this method.
    Download PDF (2123K)
Announcement
  • Ceramics Processing through Energy Consumption Reduction (Green Processing) Journal of the Ceramics Society of Japan announces a special focus issue for January 2014.
    2013 Volume 121 Issue 1416 Pages A8-1
    Published: 2013
    Released on J-STAGE: August 01, 2013
    JOURNAL FREE ACCESS
    Download PDF (85K)
feedback
Top