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A Sr analogue of Ca 0.5 Bi 0.5 FeO 3 , Sr 0.5 Bi 0.5 FeO 3 , containing unusually high valence Fe 3.5+ ions was synthesized by using a high-pressure technique. It relieves the electronic instability due to the unusually high valence of Fe 3.5+ by a single charge disproportionation (CD) transition (Fe 3.5+ → 0.75Fe 3+ + 0.25Fe 5+ ) rather than the successive CD and intermetallic charge transfer (CT) transitions seen in Ca 0.5 Bi 0.5 FeO 3 . Conduction-band narrowing due to the significant bend in the Fe-O-Fe bond in the rhombohedral R3̅c crystal structure stabilized the charge-disproportionated state at low temperatures. Most importantly, Bi 3+ ions in Sr 0.5 Bi 0.5 FeO 3 do not act as countercations accepting oxygen holes as they do in Ca 0.5 Bi 0.5 FeO 3 , resulting in the absence of the intermetallic CT transition. The large cavity of the A-site Sr ions prevents the charge-transferred Bi 5+ from being stabilized. In the charge-disproportionated state the nearest-neighbor Fe 3+ spins align antiferromagnetically and one-fourth of the Fe 3+ spins are randomly replaced by Fe 5+ spins coupled ferromagnetically with the neighboring Fe 3+ spins.

Charge Disproportionation in Sr0.5Bi0.5FeO3 Containing Unusually High Valence Fe3.5+

Charge Disproportionation in Sr_0.5Bi_0.5FeO₃ Containing Unusually High Valence Fe^3.5+