Structure and magnetic properties of bife0.75mn 0.25o3 perovskite prepared at ambient and high pressure

Alexei A. Belik, Artem M. Abakumov, Alexander A. Tsirlin, Joke Hadermann, Jungeun Kim, Gustaaf Van Tendeloo, Eiji Takayama-Muromachi

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71 Citations (Scopus)

Abstract

Solid solutions of BiFe1-xMnxO3 (0.0 ≥ x ≥ 0.4) were prepared at ambient pressure and at 6 GPa. The ambient-pressure (AP) phases crystallize in space group R3c similarly to BiFeO3. The high-pressure (HP) phases crystallize in space group R3c for x = 0.05 and in space group Pnma for 0.15 ≥ x ≥ 0.4. The structure of HP-BiFe 0.75Mn0.25O3 was investigated using synchrotron X-ray powder diffraction, electron diffraction, and transmission electron microscopy. HP-BiFe0.75Mn0.25O3 has a PbZrO3-related √2ap × 4ap × 2√2ap (ap is the parameter of the cubic perovskite subcell) superstructure with a = 5.60125(9) Å, b = 15.6610(2) Å, and c = 11.2515(2) Å similar to that of Bi0.82La 0.18FeO3. A remarkable feature of this structure is the unconventional octahedral tilt system, with the primary a-b 0a- tilt superimposed on pairwise clockwise and counterclockwise rotations around the b-axis according to the oioi sequence (o stands for out-of-phase tilt, and I stands for in-phase tilt). The (FeMn)O 6 octahedra are distorted, with one longer metal-oxygen bond (2.22-2.23 Å) that can be attributed to a compensation for covalent Bi-O bonding. Such bonding results in the localization of the lone electron pair on Bi3+ cations, as confirmed by electron localization function analysis. The relationship between HP-BiFe0.75Mn0.25O 3 and antiferroelectric structures of PbZrO3 and NaNbO3 is discussed. On heating in air, HP-BiFe0.75Mn 0.25O3 irreversibly transforms to AP-BiFe 0.75Mn0.25O3 starting from about 600 K. Both AP and HP phases undergo an antiferromagnetic ordering at TN ≈ 485 and 520 K, respectively, and develop a weak net magnetic moment at low temperatures. Additionally, ceramic samples of AP-BiFe0.75Mn 0.25O3 show a peculiar phenomenon of magnetization reversal.

Original languageEnglish
Pages (from-to)4505-4514
Number of pages10
JournalChemistry of Materials
Volume23
Issue number20
DOIs
Publication statusPublished - 25 Oct 2011
Externally publishedYes

Keywords

  • BiFeO
  • high pressure
  • multiferroics
  • superstructure

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