Complex magnetic differentiation of cobalts in Na$_{x}$CoO$_{2}$ with 22K N\'eel temperature

Abstract

Single crystals of sodium cobaltates Na$_{x}$CoO$_{2}$ with $x \approx 0.8$ were grown by the floating zone technique. Using electrochemical Na de-intercalation method we reduced the sodium content in the as-grown crystals down to pure phase with 22 K N\'eel temperature and $x \approx 0.77$. The $^{59}$Co NMR study in the paramagnetic state of the $T_{N}=22$ K phase permitted us to evidence that at least 6 Co sites are differentiated. They could be separated by their magnetic behaviour into three types: a single site with cobalt close to non-magnetic Co$^{3+}$, two sites with the most magnetic cobalts in the system, and the remaining three sites displaying an intermediate behaviour. This unusual magnetic differentiation calls for more detailed NMR experiments on our well characterized samples.