Piezoelectric anomalies at the ferroelastic phase transitions of lead-free tungsten bronze ferroelectrics

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  • WATANABE Takayuki
    Corporate R&D Headquarters, CANON INC.
  • HAYASHI Jumpei
    Corporate R&D Headquarters, CANON INC.
  • MATSUDA Takanori
    Corporate R&D Headquarters, CANON INC.
  • IFUKU Toshihiro
    Corporate R&D Headquarters, CANON INC.
  • LEE Bong-Yeon
    Research Center for Hydrogen Industrial Use and Storage, National Institute of Advanced Industrial Science and Technology (AIST)
  • IIJIMA Takashi
    Research Center for Hydrogen Industrial Use and Storage, National Institute of Advanced Industrial Science and Technology (AIST)
  • FUNAKUBO Hiroshi
    Department of Innovative and Engineered Materials, Tokyo Institute of Technology
  • YU Houzhona
    Department of Research Interdisciplinary Graduate School of Medicine and Engineering, University of Yamanashi
  • KUMADA Nobuhiro
    Department of Research Interdisciplinary Graduate School of Medicine and Engineering, University of Yamanashi

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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 Sr1.9Ca0.1NaNb5O15 (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.<br>Second, the ferroelastic phase transition was investigated for epitaxial films of (1 − x)(Sr3Ba2)Nb10O30–xBa4Bi2/3Nb10O30 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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