Direct observation of the Mottness and p–d orbital hybridization in the epitaxial monolayer α-RuCl₃

Abstract

α-RuCl₃, a promising material to accomplish the Kitaev honeycomb model, has attracted enormous interest recently. Mottness and p-d bonds play vital roles in generating Kitaev interactions and underpinning the potential exotic states of quantum magnets, and the van der Waals monolayer is considered to be a better platform to approach a two-dimensional Kitaev model than the bulk. Here, we worked out the growth art of an α-RuCl₃ monolayer on a graphite substrate and studied its electronic structure, particularly the delicate orbital occupations, through scanning tunneling microscopy and spectroscopy. An in-plane lattice expansion of 2.67 ± 0.83% is observed and the pronounced t_2g-p_π and e_g-p_σ hybridization are visualized. The Mott nature is unveiled by an ∼0.6 eV full gap at the Fermi level located inside the t_2g-p_π manifold which is further verified by the density functional theory calculations. The monolayer phase of α-RuCl₃ fulfills the <i>a priori</i> criteria of recent theoretical predictions of tuning the relevant properties in this material and provides a novel platform to explore the Kitaev physics.