Magnetic susceptibility of BaPb1−xBixO3 system

doi:10.1016/0921-4534(88)90121-9

Physica C: Superconductivity

Volume 156, Issue 1, 1 August 1988, Pages 157-164

https://doi.org/10.1016/0921-4534(88)90121-9 Get rights and content

Abstract

Systematic measurements of magnetic susceptibility have been performed on the BaPb_1−xBi_xO₃ system. The precise measurements on the samples with various compositions make it possible to extract a small Pauli paramagnetic contribution in the metallic compositional region 0⩽x<0.35. the small Pauli paramagnetism is consistent with the low density of states inferred from other measurements such as specific heat and the band calculational result as well. It turns out that the Pauli paramagnetic term decreases when x increases beyond 0.2. This can be explained as a percursor of the metal-semiconductor transition at x−0.35. In the semiconducting phase 0.35<x⩽1, a different and unusual paramagnetic contribution is showing up which makes the semiconducting phase more paramagnetic than the metallic phase.

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The magnetic susceptibilities for BaBiO_3−δ, Ba_1−xLa_xBiO₃ and Ba_1−xK_xBiO₃ were measured in order to investigate the excess paramagnetic contribution χ_p which is found in semiconducting phase of Ba_1−xK_xBiO₃ and BaPb_xBi_1−xO₃. χ_p is maximum when the Bi formal valence is +4, and decreases as the valence goes to +5 or +3. The change of χ_p corresponds to that of the supposed density of states at the Fermi surface in a metallic phase. Coexistence of charge density wave and spin density wave is suggested in the semiconducting phase of Ba_1−xK_xBiO₃ and BaPb_xBi_1−xO₃.
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X-ray absorption spectroscopy (XAS) measurements at the PbL₃ and BiL₃ edges have been made for Bi-based perovskite oxides: BaPb_1−xBi_xO_3−δ (x = 0, δ ≤ 0.2; x = 0.25, δ ≤ 0.15; x = 1, δ ≤ 0.4) and Ba_0.6K_0.4BiO_3−δ (δ ≤ 0.2). Oxygen reduction leads to larger changes in the BiL₃ edge of BaPb_1−xBi_xO_3−δ (x = 0.25, 1.0) and Ba_0.6K_0.4BiO_3−δ than in the PbL₃ edge of BaPb_1−xBi_xO_3−δ (x = 0, 0.25). Single-electron calculations of the X-ray absorption near-edge structure (XANES) spectra in BaBiO_3−δ and BaPbO_3−δ could not predict a different behaviour of the BiL₃ and the PbL₃ edges under oxygen reduction. This may be explained by assuming many-body states in the electronic structure of the BiO complexes. Extended X-ray absorption fine structure (EXAFS) measurements indicate a very small increase of the single PbO bond length with δ in BaPb_1−xBi_xO_3−δ (x = 0, 0.25). On the other hand, the separation between two different BiO bond lengths increases with δ in BaPb_1−xBi_xO_3−δ (x = 0.25, 1). Two BiO distances, separated by 0.07 Å, could be distinguished for Ba_0.6K_0.4BiO_3−δ in the semiconducting phase (δ ≥ 0.2). The superconductivity destruction in BaPb_0.75Bi_0.25O_3−δ and Ba_0.6K_0.4BiO_3−δ upon oxygen reduction is mainly accompanied by changes in the electronic and local structures of the BiO complexes. The results were employed to test some models of charge disproportionation in BaPbBiO and BaKBiO. Neither the Bi³⁺ + Bi⁵⁺ model nor the model of charge ordering on BiO bonds with normal bismuth states (Bi^{4 + ± Δ}) have been directly supported by the XAS data. As an alternative, we have proposed a charge disproportionation model in the form: 2Bi⁴⁺ → Bi³⁺ + Bi³⁺ L², where L² denotes two holes spread on 2p orbital of six oxygen atoms surrounding the Bi ion. This model is in agreement with the X-ray absorption, photoelectron spectroscopy, muon spin rotation and structural experiments on BaPbBiO and BaKBiO.
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¹: Present address: Central Research Laboratory Hitachi, Ltd. Kokubunji, Tokyo 185, Japan.

²: Present address: Department of Industrial Chemistry, University Hongo 7-3-1, Tokyo 113, Japan.

³: Present address: Department of Physics, Tokai University, Hiratsuka, Kanagawa 259-12, Japan.

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Magnetic susceptibility of BaPb1−xBixO3 system

Abstract

Physica B

Physica B

Phys. Rev. B

Phys. Rev. B

Phys. Rev.

Phys. Rev.

J. Phys. C

Phase Transitions

Appl. Phys.

Phys. Rev. Lett.

J. Phys. Soc. Jpn.

Europhys. Lett.

Phys. Rev. B

J. Phys. Soc. Jpn.

Phys. Rev. B

Magnetic susceptibility of BaPb_1−xBi_xO₃ system