First demonstration of tuning between the Kitaev and Ising limits in a honeycomb lattice

Recent observations of novel spin-orbit coupled states have generated interest in 4d/5d transition metal systems. A prime example is the [Formula: see text] state in iridate materials and α-RuCl₃ that drives Kitaev interactions. Here, by tuning the competition between spin-orbit interaction (λ_SOC) and trigonal crystal field (Δ_T), we restructure the spin-orbital wave functions into a previously unobserved [Formula: see text] state that drives Ising interactions. This is done via a topochemical reaction that converts Li₂RhO₃ to Ag₃LiRh₂O₆. Using perturbation theory, we present an explicit expression for the [Formula: see text] state in the limit Δ_T ≫ λ_SOC realized in Ag₃LiRh₂O₆, different from the conventional [Formula: see text] state in the limit λ_SOC ≫ Δ_T realized in Li₂RhO₃. The change of ground state is followed by a marked change of magnetism from a 6 K spin-glass in Li₂RhO₃ to a 94 K antiferromagnet in Ag₃LiRh₂O₆.