Large Negative Thermal Expansion Induced by Synergistic Effects of Ferroelectrostriction and Spin Crossover in PbTiO 3 -Based Perovskites

Zhao Pan, Jun Chen, Runze Yu, Lokanath Patra, Ponniah Ravindran, Andrea Sanson, Ruggero Milazzo, Alberto Carnera, Lei Hu, Lu Wang, Hajime Yamamoto, Yang Ren, Qingzhen Huang, Yuki Sakai, Takumi Nishikubo, Takahiro Ogata, Xi'An Fan, Yawei Li, Guangqiang Li, Hajime HojoMasaki Azuma, Xianran Xing

Research output: Contribution to journalArticlepeer-review

17 Citations (Scopus)

Abstract

The discovery of unusual negative thermal expansion (NTE) provides the opportunity to control the common but much desired property of thermal expansion, which is valuable not only in scientific interests but also in practical applications. However, most of the available NTE materials are limited to a narrow temperature range, and the NTE effect is generally weakened by various modifications. Here, we report an enhanced NTE effect that occurs over a wide temperature range (α V = 5.24 × 10 -5 °C -1 , 25-575 °C), and this NTE effect is accompanied by an abnormal enhanced tetragonality, a large spontaneous polarization, and a G-type antiferromagnetic ordering in the present perovskite-type ferroelectric of (1-x)PbTiO 3 -xBiCoO 3 . Specifically, for the composition of 0.5PbTiO 3 -0.5BiCoO 3 , an extensive volumetric contraction of 4.8 % has been observed near the Curie temperature of 700 °C, which represents the highest level in PbTiO 3 -based ferroelectrics. According to our experimental and theoretical results, the large NTE originates from a synergistic effect of the ferroelectrostriction and spin crossover of cobalt on the crystal lattice. The actual NTE mechanism is contrasted with previous functional NTE materials, in which the NTE is simply coupled with one ordering such as electronic, magnetic, or ferroelectric ordering. The present study sheds light on the understanding of NTE mechanisms, and it attests that NTE could be simultaneously coupled with different orderings, which will pave a new way toward the design of large NTE materials.

Original languageEnglish
Pages (from-to)1296-1303
Number of pages8
JournalChemistry of Materials
Volume31
Issue number4
DOIs
Publication statusPublished - Feb 26 2019
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

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