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We report the observation of a stepwise "melting" of the low-temperatureNa-vacancy order in the layered transition metal oxide Na0.7CoO2.High-resolution neutron powder diffraction indicates the existence of twofirst-order structural transitions, one at T1 = 290 K, followed by a second atT2 = 400 K. Detailed analysis reveals that both transitions are linked tochanges in the Na mobility. Our data are consistent with a two-stepdisappearance of Na-vacancy order through the successive opening of firstquasi-1D (T1 > T > T2) and then 2D (T > T2) Na diffusion paths. These resultsshed new light on previous, seemingly incompatible, experimentalinterpretations regarding the relationship between Na-vacancy order and Nadynamics in this material. They also represent an important step towards thetuning of physical properties and the design of tailored functional materialsthrough an improved control and understanding of ionic diffusion.

1D to 2D Na Ion Diffusion Inherently Linked to Structural Transitions in Na$_{0.7}$CoO$_{2}$