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The crystal structure, magnetic ground state, and the temperature dependentmicroscopic spin-spin correlations of the frustrated honeycomb latticeantiferromagnet Na2Co2TeO6 have been investigated by powder neutrondiffraction. A three dimensional (3D) long-range antiferromagnetic ordering hasbeen found below TN ~ 24.8 K. The magnetic ground state, determined to bezigzag antiferromagnet [k = (1/2 0 0)], occurs due to the competing exchangeinteractions up to third nearest neighbors within the honeycomb lattice. Theexceptional existence of a limited magnetic correlation length along the c axis(perpendicular to the honeycomb layers in the ab planes) has been found withinthe 3D long-range ordered state, even at 1.8 K, well below TN. The observedlimited correlation along the c axis is explained by the disorder distributionof the Na ions within the intermediate layers. The reduced ordered momentsmCo(1) = 2.77(3) muB/Co2+ and mCo(2) = 2.45(2) muB/Co2+ at 1.8 K reflect thepersistence of spin fluctuations in the ordered state. Above TN, the presenceof short-range magnetic correlations, manifested by broad diffuse magneticpeaks, has been found. Reverse Monte Carlo analysis of the experimental diffusemagnetic scattering data reveals that the spin correlations are mainly confinedwithin the 2D honeycomb layers (ab plane) with a correlation length of ~ 12{\AA} at 25 K. The nature of spin arrangements is found to be similar in boththe short-range and long-range ordered magnetic states. This implies that theshort-range correlation grows with decreasing temperature and leads to thezigzag AFM ordering at T < TN. The present study provides a comprehensivepicture of the magnetic correlations over the temperature range above and belowTN and their relation to the crystal structure. The role of intermediate softNa-layers on the magnetic coupling between honeycomb planes is discussed.

Zigzag antiferromagnetic ground state with anisotropic correlation lengths in the quasi-2D honeycomb lattice compound Na2Co2TeO6