$J=1/2$ Pseudospins and $d$-$p$ Hybridization in the Kitaev Spin Liquid Candidates Ru$X_3$ ($X$ = Cl, Br, I)

Abstract

The recent synthesis of ruthenium trihalides Ru$X_3$ ($X$ = Cl, Br, I) has enlarged the set of material candidates for Kitaev spin liquid. The realization of Kitaev model necessitates the formation of $J=1/2$ pseudospins in the octahedral crystal field. We use Ru $L_3$-edge resonant inelastic x-ray scattering to investigate the evolution of multiplet structures in Ru$X_3$. We identified quasi-elastic magnetic correlations and spin-orbit transitions to the $J=3/2$ states without discernible trigonal splitting, thereby validating the $J=1/2$ description of magnetism in the Ru$X_3$ family. Lineshape broadening in RuI${}_3$ provides evidence for its bulk metallicity in the vicinity of a bandwidth-controlled metal-insulator transition. Our results highlight the pivotal role of halogen $p$ orbitals in controlling the electronic properties of Ru$X_3$.