Unconventional Superconductivity Induced by Quantum Critical Fluctuations in Hydrate Cobaltate Na$_{x}$(H$_3$O)$_{z}$CoO$_{x}\cdot$ $y$H$_{2}$O -- Relationship between Magnetic Fluctuations and the Superconductivity Revealed by a Co Nuclear Quadrupole Resonance --

Abstract

Co nuclear-quadrupole-resonance (NQR) measurements were performed on various bilayered hydrate cobaltate Na_x(H_3O)_zCoO_2\cdot yH_2O with different values of the superconducting and magnetic-ordering temperatures, T_c and T_M, respectively. From measurements of the temperature and sample dependence of the NQR frequency, it was revealed that the NQR frequency is changed by the change of the electric field gradient (EFG) along the c axis ν_{zz} rather than the asymmetry of EFG within the ab-plane. In addition, it is considered that the change of ν_{zz} is gaverned mainly by the trigonal distortion of the CoO_2 block layers along the c axis, from the relationships between ν_{zz} and the various physical parameters. We found the tendency that samples with ν_{zz} larger than 4.2 MHz show magnetic ordering, whereas samples with lower ν_{zz} show superconductivity. We measured the nuclear spin-lattice relaxation rate 1/T_1 in these samples, and found that magnetic fluctuations depend on samples. The higher-ν_{zz} sample has stronger magnetic fluctuations at T_c. From the relationship between ν_{zz} and T_c or T_M, we suggest that the NQR frequency can be regarded as a tuning parameter to determine the ground state of the system, and develop the phase diagram using ν_{zz}. This phase diagram shows that the highest-T_c sample is located at the point where T_M is considered to be zero, which suggests that the superconductivity is induced by quantum critical fluctuations. We strongly advocate that the hydrate cobaltate superconductor presents an example of the magnetic-fluctuation-mediated superconductivity argued in the heavy-fermion compounds. The coexistence of superconductivity and magnetism observed in the sample with the highest ν_{zz} is also discussed on the basis of the results of our experiments.