Modulated Structure of Misfit-Layered Cobalt Oxide [Ca<sub>2</sub>(Co<sub>0.65</sub>Cu<sub>0.35</sub>)<sub>2</sub>O<sub>4</sub>]<sub>0.63</sub>CoO<sub>2</sub>

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  • Miyazaki Yuzuru
    Department of Applied Physics, Graduate School of Engineering, Tohoku University
  • Miura Tatsuro
    Department of Applied Physics, Graduate School of Engineering, Tohoku University
  • Onoda Mitsuko
    Advanced Materials Laboratory, National Institute for Materials Science
  • Uchida Masaya
    Advanced Materials Laboratory, National Institute for Materials Science
  • Ishii Yoshinobu
    Advanced Science Research Center, Japan Atomic Energy Research Institute
  • Ono Yasuhiro
    Department of Applied Physics, Graduate School of Engineering, Tohoku University
  • Morii Yukio
    Advanced Science Research Center, Japan Atomic Energy Research Institute
  • Kajitani Tsuyoshi
    Department of Applied Physics, Graduate School of Engineering, Tohoku University

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  • Modulated Structure of Misfit-Layered Cobalt Oxide [Ca2(Co0.65Cu0.35)2O4]0.63CoO2

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We have determined the crystal structure of novel thermoelectric compound [Ca2(Co0.65Cu0.35)2O4]0.63CoO2 by a superspace group approach. Structural parameters have been refined with a superspace group of C2⁄m(1 p 0)s0 using powder neutron diffraction data collected at 293 K. The compound consists of mutually interpenetrating triangular CoO2 layers and distorted four-layered rock salt-type Ca2(Co0.65Cu0.35)2O4 slabs, which are incommensurate parallel to the b-axis. The CoO2 layer is composed of the CdI2-type edge-shared CoO6 octahedra. Both the subsystems have common a- and c-axes, and β-angle with a=4.8212(4) Å, c=12.7671(8) Å and β=93.93(1)°. The b-axis lengths are b1=2.8103(3) Å for the [CoO2] subsystem and b2=4.4915(3) Å for the [Ca2(Co0.65Cu0.35)2O4] subsystem. A marked displacive modulation of the (Co,Cu) and O sites in the [Ca2(Co0.65Cu0.35)2O4] subsystem has been observed, yielding a large fluctuation of the (Co,Cu)–O distances in the range from 1.8 Å to 2.7 Å. Cu2+ ions appear to play an important role in stabilizing such a four-atom thick subsystem in this compound.

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