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Li3Co2SbO6 is prepared by molten salt ion exchange and its structure refinedby the Rietveld method confirming the honeycomb-type Co/Sb ordering of its Naprecursor. Monoclinic rather than trigonal symmetry of Na3Co2SbO6 is directlydemonstrated for the first time by peak splitting in the high-resolutionsynchrotron XRD pattern. The long-range antiferromagnetic order is establishedat TN about 6.7 K and 9.9 K in Na3Co2SbO6 and Li3Co2SbO6, respectively,confirmed by both the magnetic susceptibility and specific heat. Spin-waveanalysis of specific heat data indicates the presence of 3D AFM magnons inNa3Co2SbO6 and 2D AFM magnons in Li3Co2SbO6. The field dependence of themagnetization almost reaches saturation in moderate magnetic fields up to 9 Tand demonstrates characteristic features of magnetic field inducedspin-reorientation transitions for both A3Co2SbO6 (A = Na, Li). Overallthermodynamic studies show that the magnetic properties of both compounds arevery sensitive to an external magnetic field, thus predicting a non-trivialground state with a rich magnetic phase diagram. The ground state spinconfiguration of Li3Co2SbO6 has been determined by low-temperature neutronpowder diffraction. It represents a ferromagnetic arrangement of moments in thehoneycomb layers with antiferromagnetic coupling between adjacent layers.

Synthesis, structure and magnetic properties of honeycomb-layered Li3Co2SbO6 with new data on its sodium precursor, Na3Co2SbO6