Papers by Author: Takaaki Tsurumi

Abstract: BaTiO₃ films were fabricated on Si substrate using inkjet printing technique. To achieve low-temperature fabrication of BaTiO₃ films, Ba-Ti-alkoxide ink was prepared. The mixing ratio and sequence of raw materials were optimized for controlling the chemical stability and viscosity of alkoxide ink. The inkjet printing films on Si substrate were annealed at 700 °C, and it resulted in the formation of BaTiO₃. It was found that the film quality was improved by adding BaTiO₃ nanoparticles into the Ba-Ti-alkoxide ink.

Abstract: Freestanding BaTiO₃ ceramics films were fabricated using the aerosol deposition (AD) method and the size effect of nanograined BaTiO₃ ceramics was demonstrated. Dense BaTiO₃ thick film fabricated by the AD method was crystallized and detached from substrate by an annealing treatment at 600 °C, and then the grain size was controlled by a reannealing treatment at various temperatures. As a result, freestanding BaTiO₃ thick films with various grain sizes from 24 to 170 nm were successfully obtained. Polarization–electric field (P–E) measurement revealed that BaTiO₃ ceramics with grain sizes of more than 58 nm showed ferroelectricity, whereas BaTiO₃ ceramics with an average grain size of 24 nm showed paraelectricity at room temperature. Dielectric measurement indicated that the permittivity decreased with decreasing grain size in the range of 170 to 24 nm.

Abstract: The effect of oxygen vacancies and their migrations on the dielectric responses of BaTiO₃ (BT) ceramics and (Ba, Ca)(Ti, Zr)O₃ (BCTZ) ceramics was studied using wideband dielectric spectroscopy. Both dipole and ionic polarization of BT ceramics after annealing in a reducing atmosphere markedly decreased. To elucidate the decrease of dipole and ionic polarization, we observed the domain width and the crystal structure of BT ceramics annealed in different PO₂. The mass fractions of constituted phases in 90^o domain were calculated using the refinement of XRD patterns to explain the degradation of ionic polarization by oxygen vacancies. From the results above, we judged that the decrease of dipole polarization was due to the domain wall clamping by oxygen vacancies, while that of ionic polarization was attributable to the lattice hardening by the incorporation of oxygen vacancies into the BT lattice. In the case of BCTZ ceramics, dipole polarization showed the same way as BT ceramics with annealing conditions but the ionic polarization was independent of PO₂ in annealing because of anti-reducing behavior of BCTZ ceramics. On the basis of the effect of oxygen vacancy in BT ceramics and BCTZ ceramics, we could clarify the oxygen vacancy migration in BCTZ ceramics under high direct-current voltage (DCV).

Abstract: We investigated an influence of interface layer on a tunability of parallel plate (Ba, Sr)TiO3 thin film capacitors. BST thin film capacitors with top electrode of Pt, Au and Ag were fabricated. BST films had thickness of 40, 60, 80 and 120nm. The tunability increased with increasing the BST film thickness. Considering the interfaces between BST films and electrodes as Schottky junctions, depletion layers were formed in the interfaces depending on the difference of the work function of metal electrodes. Larger external bias voltages were applied to the depletion layer than interior BST film, because the permittivity in the depletion layer was smaller than that in interior BST film. Therefore, the depletion layer lowered the tunability. Tunability decreased with increasing the thickness of the depletion layers.

Abstract: The piezoelectric shear response of 94.0(Ka0.5, Na0.5)NbO3 (KNN) + 5.0LiNbO3 (LN) + 0.5SrTiO3 (ST) + 0.5BiFeO3 (BF) ceramics was investigated by Laser Doppler Vibrometry (LDV) and resonance-antiresonance method. From resonance-antiresonance method, the piezoelectric d15 constant was obtained to be 273 pC/N. The shear strain obtained by LDV　at the frequency of 150kHz showed strong nonlinearity. This suggested that the domain contribution to piezoelectric response in shear mode of KNN-LN-ST-BF ceramics existed at the operational frequency for the shear mode divices.

Abstract: We researched the phenomenon that the permittivity of dielectric layers in multilayer ceramic capacitor (MLCC) increases with the number of dielectric layers. Finite element method (FEM) shows that the internal residual stress in MLCC was generated by the difference of thermal expansion coefficient between internal electrodes and dielectric layers. We developed a electric measurement system with applying external stress for understanding the stress influence on dielectric properties. The compressive stress along electric field increased the polarization. The polar nano regions (PNRs) in shell composition dielectrics were easily influenced by stress. Based on these results, the relationship between the number of dielectric layers and their permittivity in MLCCs was explained.

Abstract: Barium titanate (BaTiO3) ceramics with various grain sizes from 0.7 to 13 μm on average were prepared by a conventional sintering method, a two-step sintering method and a rate controlled two-step sintering method. The permittivity of the ceramics was increased with decreasing grain size to 1.1 μm on average. However, the permittivity of the ceramics was decreased when the grain size was below 1 μm. The field emission scanning electron microscope (FE-SEM) observations revealed that the 90º domain width decreased with decreasing the grain size. By ultrawide range dielectric spectra from kHz to THz range of the BaTiO3 ceramics, the domain contribution to the permittivity was investigated. For the BaTiO3 ceramics with grain sizes over 1 μm, the dipole polarizability and the ionic polarizability were enhanced by high domain-wall density. In contrast, for the BaTiO3 ceramics with grain sizes below 1 μm, these polarizabilities were weakened.

Abstract: Wide band dielectric spectroscopy was applied from kHz to THz region for the analysis of both the ionic and the dipole polarization in Ba0.6Sr0.4TiO3 ceramics. The dielectric permittivity above the dielectric maximum temperature (Tm) is mostly dominated by the ionic polarization, while that below Tm is governed by the dipole polarization. Dielectric permittivity given by the dipole polarization increased and the relaxation frequency decreased with decreasing temperature. These phenomena are related to a increase of the size of polar nanoregions (PNRs).

Abstract: In the aerosol deposition method (ADM), we investigated an influence of pre-treatments for barium titanate powders as raw material on the deposition rate of thick films. By sieving and drying the powder, deposition rate of the films fabricated by ADM was effectively enhanced. On the other hand, heating the powders at 400-800°C, the resulting powders caused low deposition rate of the films. When a planetary milling was performed prior to charge aerosol chamber, the deposition rate of the films was four times higher than that in deposition using the powder without milling. By changing the milling rotation rate, we control size of agglomerated particles consisting of powders, which results in the control of deposition rate of the films.

Abstract: Artificial super-lattices of [(BaTiO3)/(SrTiO3)10]4 (BTO10/STO10) were fabricated on STO(001) substrate by the molecular beam epitaxy method (MBE), and the molecular layers of SrRuO3(SRO) was introduced into these superlattices as conductive layers. The superlattices introduced two conductive layers showed the enormous dielectric permittivity. On the other hand, the permittivity of the superlattice introduced one conductive layer was almost same as that of BTO10/STO10. In the case of introducing two conductive layers, the moving electrons between two layers induced the interfacial polarization. Especially, the superlattice with two SRO conductive layers, the distance between these layers in a superlattice is 18 molecular layers, showed the highest relaxation frequency 132 kHz and biggest capacitance.