Journal
SCIENTIFIC REPORTS
Volume 2, Issue -, Pages -Publisher
NATURE PORTFOLIO
DOI: 10.1038/srep00449
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Funding
- Global Centers of Excellence Program International Center for Integrated Research and Advanced Education in Materials Science''
- Ministry of Education, Culture, Sports, Science and Technology of Japan
- Japan Science and Technology Agency
- [19GS0207]
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Unusual high-valence states of iron are stabilized in a few oxides. A-site-ordered perovskite-structure oxides contain such iron cations and exhibit distinct electronic behaviors at low temperatures, e. g. charge disproportionation (4Fe(4+) -> 2Fe(3+) + 2Fe(5+)) in CaCu3Fe4O12 and intersite charge transfer (3Cu(2+) + 4Fe(3.75+) -> 3Cu(3+) + 4Fe(3+)) in LaCu3Fe4O12. Here we report the synthesis of solid solutions of CaCu3Fe4O12 and LaCu3Fe4O12 and explain how the instabilities of their unusual valence states of iron are relieved. Although these behaviors look completely different from each other in simple ionic models, they can both be explained by the localization of ligand holes, which are produced by the strong hybridization of iron d and oxygen p orbitals in oxides. The localization behavior in the charge disproportionation of CaCu3Fe4O12 is regarded as charge ordering of the ligand holes, and that in the intersite charge transfer of LaCu3Fe4O12 is regarded as a Mott transition of the ligand holes.
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