Effects of charge doping on Mott insulator with strong spin-orbit coupling, Ba$_2$NaOsO$_6$

Abstract

The effects of doping on the electronic evolution of the Mott insulating state have been extensively studied in efforts to understand mechanisms of emergent quantum phases of materials. The study of these effects becomes ever more intriguing in the presence of entanglement between spin and orbital degrees of freedom. Here, we present a comprehensive investigation of charge doping in the double perovskite Ba$_2$NaOsO$_6$, a a complex Mott insulator where such entanglement plays an important role. We establish that the insulating magnetic ground state evolves from canted antiferromagnet (cAF)to N\'eel order for dopant levels exceeding ~ 10 %. Furthermore, we determine that a broken local point symmetry (BLPS) phase, precursor to the magnetically ordered state, occupies an extended portion of the (H-T) phase diagram with increased doping. This finding reveals that the breaking of the local cubic symmetry is driven by a multipolar order, most-likely of the antiferro-quadrupolar type.