Origin of the Spin-Orbital Liquid State in a Nearly J=0 Iridate Ba₃ZnIr₂O₉

We show using detailed magnetic and thermodynamic studies and theoretical calculations that the ground state of Ba₃ZnIr₂O₉ is a realization of a novel spin-orbital liquid state. Our results reveal that Ba₃ZnIr₂O₉ with Ir⁵⁺ (5d⁴) ions and strong spin-orbit coupling (SOC) arrives very close to the elusive J 1⁄4 0 state but each Ir ion still possesses a weak moment. Ab initio density functional calculations indicate that this moment is developed due to superexchange, mediated by a strong intradimer hopping mechanism. While the Ir spins within the structural Ir₂O₉ dimer are expected to form a spin-orbit singlet state (SOS) with no resultant moment, substantial frustration arising from interdimer exchange interactions induce quantum fluctuations in these possible SOS states favoring a spin-orbital liquid phase down to at least 100 mK.