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By utilizing multifrequency electron paramagnetic resonance (EPR) spectroscopy, the iron functional center in ${\mathrm{Fe}}^{3+}$-modified polycrystalline lead zirconate $(\mathrm{Pb}\mathrm{Zr}{\mathrm{O}}_{3})$ was studied. The single phase polycrystalline sample remained orthorhombic and antiferroelectric down to $20\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ as confirmed by high-resolution synchrotron powder diffraction. The ${\mathrm{Fe}}^{3+}$ ions were identified as substituting for ${\mathrm{Zr}}^{4+}$ at the B-site of the perovskite $\mathrm{AB}{\mathrm{O}}_{3}$ lattice. Similarly as found for ${\mathrm{Fe}}^{3+}:\mathrm{Pb}\mathrm{Ti}{\mathrm{O}}_{3}$ [Me\ifmmode \check{s}\else \v{s}\fi{}tri\ifmmode \acute{c}\else \'{c}\fi{} et al., Phys. Rev. B 71, 134109 (2005)], the value of the fine-structure (FS) parameter ${B}_{2}^{0}$ is only consistent with a model in which a charged ${({\mathrm{Fe}}_{\mathrm{Zr}}^{\ensuremath{'}}\char21{}{V}_{\mathrm{O}}^{\ifmmode\bullet\else\textbullet\fi{}\ifmmode\bullet\else\textbullet\fi{}})}^{\ifmmode\bullet\else\textbullet\fi{}}$ defect associate is formed. In contrast to a well defined iron functional center in lead titanate $(\mathrm{Pb}\mathrm{Ti}{\mathrm{O}}_{3})$ with FS parameters exhibiting variances of less than 3%, a strong broadening of the EPR powder pattern was observed in lead zirconate, indicating a much larger variance of FS parameters. It is suggested that the apparent broad distribution of fine-structure parameters arises from the system's capability to realize different oxygen vacancy positions in the first coordination shell around the iron site. This proposed model of a small number of distinct iron-oxygen vacancy sites is supported by the observation that corresponding ${B}_{2}^{0}$ and orthorhombic ${B}_{2}^{2}$ FS parameters of these sites are anticorrelated, a property not expected for random distributions of fine-structure parameters.

physical review b

Iron-oxygen vacancy defect association in polycrystalline iron-modified<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:mi mathvariant="normal">Pb</mml:mi><mml:mi mathvariant="normal">Zr</mml:mi><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:mrow></mml:math>antiferroelectrics: Multifrequency electron paramagnetic resonance and Newman superposition model analysis

Iron-oxygen vacancy defect association in polycrystalline iron-modifiedPbZrO3antiferroelectrics: Multifrequency electron paramagnetic resonance and Newman superposition model analysis