Spin-glass and spin-fluctuation in Mo-doped Ca3Co4O9 system

Structural, magnetic, resistivity and thermal transport measurements have been performed to study the Mo-doping effect on a layered cobaltite Ca3Co4−xMoxO9 ( 0 ≤ x ≤ 0.4 ) system. The results indicate that the low-temperature magnetic behavior of the system changes from a ferrimagnetic state to a spin-glass-like state upon Mo doping, which is due to the decrease in the average valence of Co ions. Moreover, all the Mo-doped samples have a higher resistivity and larger thermopower S compared with the Mo-free sample. The variation in the resistivity and thermopower between the Mo-doped and the Mo-free samples is dominated by the change in the carrier concentration of the samples. In the Mo-doped samples with x ≥ 0.1 , both the resistivity and thermopower decrease gradually with increasing Mo-doping level, which is suggested to mainly originate from the variation in the carrier mobility of the samples. In addition, an obvious thermopower upturn is observed in the S ( T ) curve of all the Mo-doped samples, which can be explained by the enhancement of spin-fluctuation induced by Mo-doping.