Spin correlations and cobalt charge states: Phase diagram of sodium cobaltates
G. Lang, J. Bobroff, H. Alloul, G. Collin, and N. Blanchard
Phys. Rev. B 78, 155116 (2008) - Published 14 October, 2008
Using NMR measurements on sodium cobaltates at intermediate dopings , we establish the qualitative change in behavior of the local magnetic susceptibility at , from a low- Pauli-like regime to the high- Curie-Weiss regime. For , the presence of a maximum in the temperature dependence of the susceptibility shows the existence of an -dependent energy scale. relaxation measurements establish the predominantly antiferromagnetic character of spin correlations for . This contradicts the commonly assumed uncorrelated Pauli behavior in this range and is at odds with the observed ferromagnetic correlations for . It is suggested that at a given the ferromagnetic correlations might dominate the antiferromagnetic ones above . From NMR data, it is shown that moving toward higher away from results in the progressive appearance of nonmagnetic sites, breaking the homogeneity of Co states encountered for . The main features of the NMR-detected quadrupolar effects, together with indications from the powder x-ray diffraction data, lead us to sketch a possible structural origin for the sites. In light of this ensemble of experimental observations, a phase diagram taking into account the systematic presence of correlations and their dependence is proposed.