Magnetic Correlation of NaxCoO2 and Successive Phase Transitions of   Na0.5CoO2 -NMR and Neutron Diffraction Studies-
  Data taken by various kinds of methods including NMR/NQR and neutron scattering are presented for NaxCoO2, in particular, for Na0.5CoO2. Attentions have also been paid to the x dependence of the electronic nature. The pseudo-gap-like behavior observed in the region of x<xc~0.6 is emphasized. For samples with x<0.6, signals from two kinds of Co sites with different quadrupole frequencies nQ, ~4.1 MHz and ~2.8 MHz were observed, and the former value of nQ, which is nearly equal to that of the superconducting system Na0.3CoO2.yH2O, becomes dominant with decreasing x to 0.3. For Na0.5CoO2, the Co sites with the larger nQ value have the larger magnetic moments. They align antiferromagnetically at Tc1~87 K with their direction within the plane, while the Co sites with the smaller nQ value have the smaller moments. They align along the direction parallel to the c axis. The ordered moments at the two distinct sites exhibit the same T dependences, indicating that the existence of these sites is not due to a macroscopic phase separation. Although we have observed the splitting of the zero-field NMR signals from the Co sites with the smaller nQ value at the second transition temperature Tc2~53 K, any other anomaly of the ordered magnetization has not been observed there in the T dependences of the neutron and the NMR data. As x decreases, the two-dimensional nature of the electrons is enhanced and the antiferromagnetic correlation increases. Based on these results, the superconducting pair state in Na0.3CoO2.yH2O is discussed. 
Mai Yokoi, Taketo Moyoshi, Yoshiaki Kobayashi, Minoru Soda, Yukio   Yasui, Masatoshi Sato and Kazuhisa Kakurai