Impact of reduced dimensionality on the correlation length and magnetization dynamics of the spin chain cobaltite Ca3Co2O6

We have recently applied the magnetic field and temperature dependence of magnetic entropy change as a probe of the magnetic states of a single crystal of Ca3Co2O6 to establish a more comprehensive magnetic phase diagram for this exotic system. The results are consistent with the spin-density wave description of the ground state and indicate the suppression of the modulated state in favor of a ferrimagnetic up-up-down arrangement of the spin chains with the application of a moderate field. We demonstrate, in this study, that the features of the static magnetic phase diagram are preserved when the grain size of Ca3Co2O6 is reduced to 440 nm (below the maximum c-axis correlation length of similar to 550 nm in Ca3Co2O6), although the polycrystalline materials show a non-saturating behavior, rounded steps, and reduced magnetization when compared to the single crystal. Our new finding of the multiple low-temperature magnetization steps in the 440 nm sample, together with conflicting reports concerning such steps in nanostructured samples, suggests that correlations in the ab plane are more important than correlations along the c-axis in the appearance of the plateaus. The relaxation processes in the system are studied through the decay of remanent magnetization, ac susceptibility, and Argand diagrams. The introduction of grain boundaries in Ca3Co2O6 weakens the slow-dynamic state, widens the low-temperature distribution of relaxation times, and lowers activation energies within the Arrhenius-like relaxation regime.