Local spin structure of the α−RuCl3 honeycomb-lattice magnet observed via muon spin rotation/relaxation

Abstract

We report a muon spin rotation/relaxation ($\ensuremath{\mu}\mathrm{SR}$) study of single-crystalline samples of the $\ensuremath{\alpha}\ensuremath{-}{\mathrm{RuCl}}_{3}$ honeycomb magnet, which is presumed to be a model compound for the Kitaev-Heisenberg interaction. It is inferred from magnetic susceptibility and specific-heat measurements that the present samples exhibit successive magnetic transitions at different critical temperatures ${T}_{\mathrm{N}}$ with decreasing temperature, eventually falling into the ${T}_{\mathrm{N}}=7$ K antiferromagnetic (7 K) phase that has been observed in only single-crystalline specimens with the least stacking fault. Via $\ensuremath{\mu}\mathrm{SR}$ measurements conducted under a zero external field, we show that such behavior originates from a phase separation induced by the honeycomb plane stacking fault, yielding multiple domains with different ${T}_{\mathrm{N}}$'s. We also perform $\ensuremath{\mu}\mathrm{SR}$ measurements under a transverse field in the paramagnetic phase to identify the muon site from the muon-Ru hyperfine parameters. Based on a comparison of the experimental and calculated internal fields at the muon site for the two possible spin structures inferred from neutron diffraction data, we suggest a modulated zigzag spin structure for the 7 K phase, with the amplitude of the ordered magnetic moment being significantly reduced from that expected for the orbital quenched spin-1/2 state.