Polar-Nonpolar Transition-Type Negative Thermal Expansion with 11.1% Volume Shrinkage by Design

Takumi Nishikubo*, Takashi Imai, Yuki Sakai, Masaichiro Mizumaki, Shogo Kawaguchi, Norihiro Oshime, Ayumu Shimada, Kento Sugawara, Kenji Ohwada, Akihiko Machida, Tetsu Watanuki, Kosuke Kurushima, Shigeo Mori, Takashi Mizokawa, Masaki Azuma*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

6 Citations (Scopus)

Abstract

Chemical substitution for the tuning of the working temperature of phase-transition-type negative thermal expansion (NTE) materials generally reduces the volume shrinkage during the transition. We have investigated the effects of electron doping and reduction of 6s2 lone-pair activity in PbVO3 with a large polar distortion (c/a = 1.23) and found that the combination of Bi and Sr substitutions for Pb enables a temperature-induced polar to non-polar transition with 11% volume shrinkage, even larger than the pressure-induced volume collapse of PbVO3 (∼10.6%), and is the largest value among the NTE materials reported so far. The domain structure of the coexisting cubic and tetragonal phases with such a huge volume difference was successfully observed by high-angle annular dark-field scanning transmission electron microscopy and the spatial distribution of domains by Bragg coherent X-ray diffraction imaging. The temperature hysteresis is reduced by repeated heating/cooling cycles, suggesting that the changes in the domain structure dominate the NTE properties.

Original languageEnglish
Pages (from-to)870-878
Number of pages9
JournalChemistry of Materials
Volume35
Issue number3
DOIs
Publication statusPublished - 2023 Feb 14

ASJC Scopus subject areas

  • General Chemistry
  • General Chemical Engineering
  • Materials Chemistry

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