Spin-Cluster Glassy and Long-Range Ordered Magnetic States in Honeycomb-Layered Compositionally Complex Oxides Na3-xLixT2SbO6 (T = Cu1/3Ni1/3Co1/3).

ABSTRACT

The concept of high-entropy oxides has triggered extensive research of this novel class of materials because their numerous functional properties are usually not mere linear combinations of those of the components. Here, we introduce the new series of compositionally complex honeycomb-layered magnets Na3-xLixT2SbO6 (T = Cu1/3Ni1/3Co1/3). An unusual feature of the system is its nonmonotonous dependences of the monoclinic lattice parameters b and ß on x. Rietveld refinement of the crystal structures of the Na and Li end members reveals apparent Sb-T site inversion in the former and considerable Li-Cu site inversion in the latter. The materials are characterized by measurements of specific heat Cp, magnetization M, and ac and dc magnetic susceptibility χ. Na3T2SbO6 exhibits sharp long-range antiferromagnetic order (TN = 10.2 K) preceded by noticeable correlation effects at elevated temperatures. The magnetic phase diagram of Na3T2SbO6 is established. Introduction of Li, just at x = 0.8, destroys AFM order, resulting in spin-cluster glass behavior attributed to Li/Cu inversion, with TG growing with x to 10.4 K at x = 3.