Magnetic order in single crystals of Na 3 Co 2 SbO 6 with a honeycomb arrangement of 3d 7 Co 2+ ions
We have synthesized single crystals of Na 3 Co 2 SbO 6 and characterized the structure and magnetic order by measuring anisotropic magnetic properties, heat capacity, and x-ray and neutron single crystal diffraction. Magnetic properties and specific heat of polycrystalline Na 3 Co 2 SbO 6 were also measured for comparison. Na 3 Co 2 SbO 6 crystallizes in a monoclinic structure (space group C 2 / m ) with [Co 2 SbO 6 ] 3- layers separated by Na + ions. The temperature dependence of magnetic susceptibility shows significant anisotropic behavior in the whole temperature range 2–350 K investigated in this work. An effective moment of about 5.5μ B /Co 2+ from a Curie-Weiss fitting of the magnetic susceptibility is larger than the spin only value and signals significant orbital contribution. Na 3 Co 2 SbO 6 single crystal undergoes a transition into a long-range antiferromagnetically ordered state below T N = 5K. Neutron single crystal diffraction confirmed the zigzag magnetic structure with a propagation vector k = (0.5,0.5,0). The ordered moment is found to be 0.9 μ B at 4 K and align along the crystallographic b axis. Density functional theory calculations suggest that the experimentally observed zigzag order is energetically competing with the Néel order. Furthermore, it is also found that the covalency between Co d and O p is quite strong and competes with the local spin-orbit coupling, suggesting a J eff = 1/2 ground state may not be realized in this compound.