Jeff=1/2 Mott spin-orbit insulating state close to the cubic limit in Ca4IrO6

Abstract

The J_eff=1/2 state is manifested in systems with large cubic crystal field splitting and spin-orbit coupling that are comparable to the on-site Coulomb interaction, U. 5d transition metal oxides host parameters in this regime and strong evidence for this state in Sr2IrO4, and additional iridates, has been presented. All the candidates, however, deviate from the cubic crystal field required to provide an unmixed canonical J_eff=1/2 state, impacting the development of a robust model of this novel insulating and magnetic state. We present experimental and theoretical results that not only show Ca4IrO6 hosts the state, but furthermore uniquely resides in the limit required for a canonical unmixed J_eff=1/2 state.