Spin-Cluster Glassy and Long-Range Ordered Magnetic States in Honeycomb-Layered Compositionally Complex Oxides Na_3–xLi_xT₂SbO₆ (T = Cu_1/3Ni_1/3Co_1/3)

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 Na 3−x Li x T 2 SbO 6 (T = Cu 1/3 Ni 1/3 Co 1/3 ). An unusual feature of the system is its nonmonotonous dependences of the monoclinic lattice parameters b and β 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 C p , magnetization M, and ac and dc magnetic susceptibility χ. Na 3 T 2 SbO 6 exhibits sharp long-range antiferromagnetic order (T N = 10.2 K) preceded by noticeable correlation effects at elevated temperatures. The magnetic phase diagram of Na 3 T 2 SbO 6 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 T G growing with x to 10.4 K at x = 3.