Relation between the Co-O bond lengths and the spin state of Co in layered Cobaltates: a high-pressure study

层状钴酸盐中Co-O键长与Co自旋态的关系:一项高压研究

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Abstract

The pressure-response of the Co-O bond lengths and the spin state of Co ions in a hybrid 3d-5d solid-state oxide Sr(2)Co(0.5)Ir(0.5)O(4) with a layered K(2)NiF(4)-type structure was studied by using hard X-ray absorption and emission spectroscopies. The Co-K and the Ir-L (3) X-ray absorption spectra demonstrate that the Ir(5+) and the Co(3+) valence states at ambient conditions are not affected by pressure. The Co Kβ emission spectra, on the other hand, revealed a gradual spin state transition of Co(3+) ions from a high-spin (S = 2) state at ambient pressure to a complete low-spin state (S = 0) at 40 GPa without crossing the intermediate spin state (S = 1). This can be well understood from our calculated phase diagram in which we consider the energies of the low spin, intermediate spin and high spin states of Co(3+) ions as a function of the anisotropic distortion of the octahedral local coordination in the layered oxide. We infer that a short in-plane Co-O bond length (<1.90 Å) as well as a very large ratio of Co-O(apex)/Co-O(in-plane) is needed to stabilize the IS Co(3+), a situation which is rarely met in reality.

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