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From 59Co and 23Na NMR, we demonstrate the impact of the Na+ vacancy orderingon the cobalt electronic states in Na0.75CoO2: at long time scales, there isneither a disproportionation into 75 % Co3+ and 25 % Co4+ states, nor amixed-valence metal with a uniform Co3.25+ state. Instead, the system adopts anintermediate configuration in which 30 % of the lattice sites form an orderedpattern of localized Co3+ states. Above 180 K, an anomalous mobility ofspecific Na+ sites is found to coexist with this electronic texture, suggestingthat the formation of the latter may contribute to stabilizing the Na+ordering. Control of the ion doping in these materials thus appears to becrucial for fine-tuning of their thermoelectric properties.

Electronic texture of the thermoelectric oxide Na0.75CoO2