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Perovskite rare-earth cobaltites ACoO 3 (A = Sc, Y, La-Lu) have been of enduring interest for decades due to their unusual structural and physical properties associated with the spin-state transitions of low-spin Co 3+ ions. Herein, we have synthesized a non-rare-earth perovskite cobaltite, InCoO 3 , at 15 GPa and 1400 °C and investigated its crystal structure and magnetic ground state. Under the same high-pressure and high-temperature conditions, we also prepared a perovskite-type ScCoO 3 with an improved cation stoichiometry in comparison to that in a previous study, where synthesis at 6 GPa and 1297 °C yielded a perovskite cobaltite with cation mixing on the A-site, (Sc 0.95 Co 0.05 )CoO 3 . The two perovskite phases have nearly stoichiometric cation compositions, crystallizing in the orthorhombic Pnma space group. In the present investigation, comprehensive studies on newly developed and well-known Pnma ACoO 3 perovskites (A = In, Sc, Y, Pr-Lu) show that InCoO 3 does not fulfill the general evolution of crystal metrics with A-site cation size, indicating that InCoO 3 and rare-earth counterparts have different chemistry for stabilizing the Pnma structures. Detailed structural analyses combined with first-principles calculations reveal that the origin of the anomaly for InCoO 3 is ascribed to the A-site cation displacements that accompany octahedral tilts; despite the highly tilted CoO 6 network, the In-O covalency makes In 3+ ions reluctant to move from their ideal cubic-symmetry position, leading to less orthorhombic distortion than would be expected from electrostatic/ionic size mismatch effects. Magnetic studies demonstrate that InCoO 3 and ScCoO 3 are diamagnetic with a low-spin state of Co 3+ below 300 K, in contrast to the case of (Sc 0.95 Co 0.05 )CoO 3 , where the high-spin Co 3+ ions on the A-site generate a large paramagnetic moment. The present work extends the accessible composition range of the low-spin orthocobaltite series and thus should help to establish a more comprehensive understanding of the structure-property relation.

inorganic chemistry

Perovskite-Type InCoO<sub>3</sub> with Low-Spin Co<sup>3+</sup>: Effect of In–O Covalency on Structural Stabilization in Comparison with Rare-Earth Series

Perovskite-Type InCoO3 with Low-Spin Co3+: Effect of In–O Covalency on Structural Stabilization in Comparison with Rare-Earth Series

Perovskite-Type InCoO₃ with Low-Spin Co³⁺: Effect of In–O Covalency on Structural Stabilization in Comparison with Rare-Earth Series