Electronic phase diagram of the layered cobalt oxide system, LixCoO2 (0.0 <= x <= 1.0)

Abstract

Here we report the magnetic properties of the layered cobalt oxide system, LixCoO2, in the whole range of Li composition, 0 <= x <= 1. Based on dc-magnetic susceptibility data, combined with results of 59Co-NMR/NQR observations, the electronic phase diagram of LixCoO2 has been established. As in the related material NaxCoO2, a magnetic critical point is found to exist between x = 0.35 and 0.40, which separates a Pauli-paramagnetic and a Curie-Weiss metals. In the Pauli-paramagnetic regime (x <= 0.35), the antiferromagnetic spin correlations systematically increase with decreasing x. Nevertheless, CoO2, the x = 0 end member is a non-correlated metal in the whole temperature range studied. In the Curie-Weiss regime (x >= 0.40), on the other hand, various phase transitions are observed. For x = 0.40, a susceptibility hump is seen at 30 K, suggesting the onset of static AF order. A magnetic jump, which is likely to be triggered by charge ordering, is clearly observed at Tt = 175 K in samples with x = 0.50 (= 1/2) and 0.67 (= 2/3), while only a tiny kink appears at T = 210 K in the sample with an intermediate Li composition, x = 0.60. Thus, the phase diagram of the LixCoO2 system is complex, and the electronic properties are sensitively influenced by the Li content (x).

arXiv comment29 pages, 1 table, 9 figures

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• Electronic phase diagram of LixCoO2 revisited with potentiostatically de-intercalated single crystals
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• Novel electronic states realized by the interplay between Li diffusion and Co${}^{3+}$$/$Co${}^{4+}$ charge ordering in Li${}_{\mathrm{x}}$CoO${}_2$
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• Self-regulated ligand-metal charge transfer upon lithium ion de-intercalation process from LiCoO2 to CoO2
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• Theory of carrier concentration-dependent electronic behavior in layered cobaltates
• Interplay between magnetism and sodium vacancy ordering in NaxCoO2
• Li${}_x$CoO${}_2$ phase stability studied by machine learning-enabled scale bridging between electronic structure, statistical mechanics and phase field theories