Journal
JOURNAL OF SOLID STATE CHEMISTRY
Volume 180, Issue 11, Pages 3224-3233Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jssc.2007.08.031
Keywords
Complex perovskite; Oxynitride perovskite; Dielectric; Cation ordering; Pigment
Funding
- National Science Foundation [CHE-043567]
- Materials World Network [DMR-0603128]
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The following complex oxynitride perovskites have been prepared: LaMg1/3Ta2/3O2N, LaMg1/2Ta1/2O5/2N1/2, and BaSc0.05 Ta0.95O2.1N0.9. Synchrotron X-ray powder diffraction analyses show that LaMg1/3Ta2/3O2N and LaMg1/2Ta1/2O5/2N1/2 are isostructural to the oxide La2Mg(Mg1/3Ta2/3)O-6 (space group P2(1)/n), whereas BaSc0.05Ta0.95O2.1N0.9 has a simple cubic symmetry similarly to BaTaO2N. The orderings of octahedral cations are markedly diminished in the above oxynitrides, as compared with the related oxides such as La2Mg(Mg1/3Ta2/3)O-6 and Ba2ScTaO6. The optical band gaps are similar for the homologous compositions, LaMg1/3Ta2/3O2N, LaMg1/2Ta1/2O5/2N1/2 and LaTaON2 (1.9 eV), and BaSc0.05Ta0.95O2.1N0.9 and BaTaO2N (1.8 eV), while the absorption edges become broader for the complex derivatives. As revealed from the impedance spectroscopic analysis, the oxynitrides have clearly different dielectric components from those of comparable oxides containing Ta5+. Impedance spectroscopy reveals interesting capacitor geometry in BaSc0.05Ta0.95O2.1N0.9 in which the semiconducting oxynitride grains are separated by insulating secondary phases. Most notably BaSc0.05Ta0.95O2.1N0.9 has a bulk component with a high relative permittivity (k = 7300) and the grain boundary component with an even higher k. (C) 2007 Elsevier Inc. All rights reserved.
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