Chemistry of Materials
Chemistry of Materials
5 years ago

Topotactic Reduction toward a Noncentrosymmetric Deficient Perovskite Tb0.50Ca0.50Mn0.96O2.37 with Ordered Mn Vacancies and Piezoelectric Behavior

Topotactic Reduction toward a Noncentrosymmetric Deficient Perovskite Tb0.50Ca0.50Mn0.96O2.37 with Ordered Mn Vacancies and Piezoelectric Behavior
Ruqiang Zou, Hao Zhang, Jie Liang, Junliang Sun, Cheng Dong, Jingen Wu, Lin Gu, Fuhui Liao, Shuxiang Dong, Song Gao, Guobao Li, Jianhua Lin, Qinghua Zhang
Low-temperature reduction of perovskite Tb0.5Ca0.5MnO3–x yields novel crystal-structured noncentrosymmetric compound Tb0.50Ca0.50Mn0.962.33+O2.37, which unusually crystallizes in cubic lattice I23 (a ∼ 15.27 Å) based on a 4ap × 4ap × 4ap expansion relative to the simple cubic perovskite unit cell. Rietveld refinements and HAADF-STEM images are used for the structure determination, revealing a rare-typed metal-anion coordination framework which consists of corner-shared tetrahedra and pyramids, and edge-shared bipyramids and octahedra. 2/64 B-site Mn-ordered vacancies are observed for the first time acting as the apex and body center of the I lattice in reduced systems. Room-temperature piezoelectricity is detected, with a quasistatic d33 value of ∼0.32 pC N–1 and inverse d33 value of ∼10.5 pm V–1. This phase primarily exhibits antiferromagnetic ordering below TN ∼ 70 K, with ferromagnetic responses resulted from spin-canting below 40 K. This work provides a new way toward synthesizing unconventional acentric materials, in the absence of second-order Jahn–Teller active “distortion centers”.

Publisher URL: http://dx.doi.org/10.1021/acs.chemmater.7b04115

DOI: 10.1021/acs.chemmater.7b04115

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