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Os Doping Suppressed Cu-Fe Charge Transfer and Induced Structural and Magnetic Phase Transitions in LaCu3Fe4-xOsxO12 (x = 1 and 2)

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Wang,  Xiao
Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Hu,  Zhiwei
Zhiwei Hu, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Agrestini,  Stefano
Stefano Agrestini, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Citation

Wang, X., Liu, Z., Ye, X., Zhou, B., Hu, Z., Wang, W., et al. (2021). Os Doping Suppressed Cu-Fe Charge Transfer and Induced Structural and Magnetic Phase Transitions in LaCu3Fe4-xOsxO12 (x = 1 and 2). Inorganic Chemistry, 60(9), 6298-6305. doi:10.1021/acs.inorgchem.1c00009.


Cite as: https://hdl.handle.net/21.11116/0000-0008-88A5-4
Abstract
B-site Os-doped quadruple perovskite oxides LaCu3Fe4-xOsxO12 (x = 1 and 2) were prepared under high-pressure and high-temperature conditions. Although parent compound LaCu3Fe4O12 experiences Cu-Fe intermetallic charge transfer that changes the Cu3+/Fe3+ charge combination to Cu2+/Fe3.75+ at 393 K, in the Os-doped samples, the Cu and Fe charge states are found to be constant 2+ and 3+, respectively, indicating the complete suppression of charge transfer. Correspondingly, Os6+ and mixed Os4.5+ valence states are determined by X-ray absorption spectroscopy for x = 1 and x = 2 compositions, respectively. The x = 1 sample crystallizes in an Fe/Os disordered structure with the Im3¯ space group. It experiences a spin-glass transition around 480 K. With further Os substitution up to x = 2, the crystal symmetry changes to Pn3¯, where Fe and Os are orderly distributed in a rocksalt-type fashion at the B site. Moreover, this composition shows a long-range Cu2+(↑)Fe3+(↑)Os4.5+(↓) ferrimagnetic ordering near 520 K. This work provides a rare example for 5d substitution-suppressed intermetallic charge transfer as well as induced structural and magnetic phase transitions with high spin ordering temperature. ©