Magnetic structure, excitations and short-range order in honeycomb Na2Ni2TeO6

Na2Ni2TeO6 has a layered hexagonal structure with a honeycomb lattice constituted by Ni2+ and a chiral charge distribution of Na+ that resides between the Ni layers. In the present work, the antiferromagnetic (AFM) transition temperature of Na2Ni2TeO6 is confirmed at T-N approximate to 27 K, and further, it is found to be robust up to 8 T magnetic field and 1.2 GPa external pressure; and, without any frequency-dependence. Slight deviations from nominal Na-content (up to 5%) does not seem to influence the magnetic transition temperature, TN. Isothermal magnetization curves remain almost linear up to 13 T. Our analysis of neutron diffraction data shows that the magnetic structure of Na2Ni2TeO6 is faithfully described by a model consisting of two phases described by the commensurate wave vectors (k(c)) over right arrow, (0.5 0 0) and (0.5 0 0.5), with an additional short-range order component incorporated in to the latter phase. Consequently, a zig-zag long-range ordered magnetic phase of Ni2+ results in the compound, mixed with a short-range ordered phase, which is supported by our specific heat data. Theoretical computations based on density functional theory predict predominantly in-plane magnetic exchange interactions that conform to a J(1)-J(2)-J(3) model with a strong J(3) term. The computationally predicted parameters lead to a reliable estimate for T-N and the experimentally observed zig-zag magnetic structure. A spin wave excitation in Na2Ni2TeO6 at E approximate to 5 meV at T = 5 K is mapped out through inelastic neutron scattering experiments, which is reproduced by linear spin wave theory calculations using the J values from our computations. Our specific heat data and inelastic neutron scattering data strongly indicate the presence of short-range spin correlations, at T > T-N, stemming from incipient AFM clusters.

Automated summary

Na2Ni2TeO6 exhibits antiferromagnetic properties with a stable transition temperature even under high magnetic fields and external pressures. Deviations in Na content do not significantly affect the magnetic transition temperature. The compound consists of a long-range ordered magnetic phase of Ni2+ mixed with a short-range ordered phase, supported by specific heat data.