Emergence of the isotropic Kitaev honeycomb lattice α− RuCl3 and its magnetic properties

We present a comprehensive investigation of the crystal and magnetic structures of the van der Waals antiferromagnet α− RuCl3 using single crystal x-ray and neutron diffraction. The crystal structure at room temperature is a monoclinic ( C2/m ). However, with decreasing temperature, a remarkable first-order structural phase transition is observed, leading to the emergence of a rhombohedral ( R3ˉ ) structure characterized by three-fold rotational symmetry forming an isotropic honeycomb lattice. On further cooling, a zigzag-type antiferromagnetic order develops below TN=6∼6.6 K. The critical exponent of the magnetic order parameter was determined to be β=0.11(1) , which is close to the two-dimensional Ising model. Additionally, the angular dependence of the magnetic critical field of the zigzag antiferromagnetic order for the polarized ferromagnetic phase reveals a six-fold rotational symmetry within the ab− plane. These findingsreflect the symmetry associated with the Ising-like bond-dependent Kitaev spin interactions and underscore the universality of the Kitaev interaction-dominated antiferromagnetic system.