No abstract

Using powder neutron diffraction, we have discovered an unusual magnetic order-order transition in the Ising spin chain compound Ca3Co2O6. On lowering the temperature, an antiferromagnetic phase with a propagation vector k=(0.5,-0.5,1) emerges from a higher temperature spin density wave structure with k=(0,0,1.01). This transition occurs over an unprecedented time scale of several hours and is never complete.

Abstract. -We present single-crystal neutron-diffraction data for the spin-chain compound Ca3Co2O6. The intensity and line shapes of the two families of Bragg peaks characterising both the antiferromagnetic and the ferromagnetic components of the magnetic order present in this material have been measured as a function of temperature and applied magnetic fields of up to 5 T. We have studied the microscopic nature of the magnetic order at each step seen in the bulk magnetisation and investigated the evolution of the long and short-range components of the magnetic order in Ca3Co2O6.

We present polarised-neutron diffraction measurements of the Ising-like spin-chain compound Ca3Co2O6 above and below the magnetic ordering temperature TN. Below TN, a clear evolution from a single-phase spin-density wave (SDW) structure to a mixture of SDW and commensurate antiferromagnet (CAFM) structures is observed on cooling. For a rapidly-cooled sample, the majority phase at low temperature is the SDW, while if the cooling is performed sufficiently slowly, then the SDW and the CAFM structure coexist between 1.5 and 10 K. Above TN, we use Monte Carlo methods to analyse the magnetic diffuse scattering data. We show that both intra-and inter-chain correlations persist above TN, but are essentially decoupled. Intra-chain correlations resemble the ferromagnetic Ising model, while inter-chain correlations resemble the frustrated triangular-lattice antiferromagnet. Using previously-published bulk property measurements and our neutron diffraction data, we obtain values of the ferromagnetic and antiferromagnetic exchange interactions and the single-ion anisotropy.