Functionalization induced quantum spin Hall to quantum anomalous Hall phase transition in monolayer jacutingaite

As novel states of quantum matter, quantum spin Hall (QSH) and quantum anomalous Hall (QAH) states have attracted considerable interest in condensed matter and materials science communities. Recently, a monolayer of the naturally occurring mineral jacutingaite (Pt2HgSe3), was theoretically proposed to be a large-gap QSH insulator and experimentally confirmed. Here, based on first-principles calculations and tight-binding modeling, we demonstrate QSH to QAH phase transition in jacutingaite by chemical functionalization with chalogen. We show that two-dimensional (2D) chalogenated jacutingaite, Pt2HgSe3-X (X = S, Se, Te), is ferromagnetic with Curie temperature up to 316 K, and it exhibits QAH effect with chiral edge states inside a sizeable topological gap. The physical mechanism lies in the adsorption induced transformation of the original Kane-Mele model into an effective four-band model involving (p(x), p(y)) orbitals on a hexagonal lattice, so that the topological gap size can be controlled by spin-orbit coupling strength of the chalogen (0.28 eV for Pt2HgSe3-Te). These results not only show the promise of functionalization in orbital-engineering of 2D functional structures, but also provide an ideal and practical platform for achieving exotic topological phases for dissipationless transport and quantum computing.