Magnetic Properties of A2Ni2TeO6 (A = K, Li): Zigzag Order in the Honeycomb Layers of Ni2+ Ions Induced by First and Third Nearest-Neighbor Spin Exchanges

Abstract

The static and dynamic magnetic properties and the specific heat of K₂Ni₂TeO₆ and Li₂Ni₂TeO₆ were examined and it was found that they undergo a long-range ordering at <i>T_N</i> = 22.8 and 24.4 K, respectively, but exhibit a strong short-range order. At high temperature, the magnetic susceptibilities of K₂Ni₂TeO₆ and Li₂Ni₂TeO₆ are described by a Curie-Weiss law, with Curie-Weiss temperatures Θ of approximately -13 and -20 K, respectively, leading to the effective magnetic moment of about 4.46 ± 0.01 <i>μ</i>_B per formula unit, as expected for Ni²⁺ (<i>S</i> = 1) ions. In the paramagnetic region, the ESR spectra of K₂Ni₂TeO₆ and Li₂Ni₂TeO₆ show a single Lorentzian-shaped line characterized by the isotropic effective <i>g</i>-factor, <i>g</i> = 2.19 ± 0.01. The energy-mapping analysis shows that the honeycomb layers of A₂Ni₂TeO₆ (A = K, Li) and Li₃Ni₂SbO₆ adopt a zigzag order, in which zigzag ferromagnetic chains are antiferromagnetically coupled, because the third nearest-neighbor spin exchanges are strongly antiferromagnetic while the first nearest-neighbor spin exchanges are strongly ferromagnetic, and that adjacent zigzag-ordered honeycomb layers prefer to be ferromagnetically coupled. The short-range order of the zigzag-ordered honeycomb lattices of K₂Ni₂TeO₆ and Li₂Ni₂TeO₆ is equivalent to that of an antiferromagnetic uniform chain, and is related to the short-range order of the ferromagnetic chains along the direction perpendicular to the chains.