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The impact of oxygen deficiency on physical properties of Na2/3CoO2-x hasbeen investigated. From the combined thermogravimetric, magnetic susceptibilityand synchrotron X-ray Laue diffraction studies, it is demonstrated thatNa2/3CoO2 shows no superlattice ordering due to Na ions; however Na2/3CoO1.98,which has the same Co valence as that of Na0.71CoO2, shows nearly identicalmagnetic and transport properties and the same simple hexagonal superlatticeordering of sqrt(12)a. It is proposed that the Na ion ordering found inNa2/3CoO1.98 is identical to the ideal Na0.71CoO2 of large sqrt(12)a xsqrt(12)a x 3c superlattice but with additional Na vacancies which are bound tothe oxygen defects at room temperature. We conclude that oxygen vacancies playa key role in stabilizing the superlattice structure and must be accounted forin its modeling.

Oxygen non-stoichiometry and the origin of Na ion ordering in P2-NaxCoO2