Large-Gap Quantum Spin Hall Insulators in Two-Dimensional Hafnium Halides: Unraveling the Impact of Strain and Substrate.

Two-dimensional (2D) topological insulators (TIs) or quantum spin Hall (QSH) insulators, characterized by insulating 2D electronic band structures and metallic helical edge states protected by time-reversal symmetry, offer a platform for realizing the quantum spin Hall effect, making them promising candidates for future spintronic devices and quantum computing. However, observing a high-temperature quantum spin Hall effect requires large-gap 2D TIs, and only a few 2D systems have been experimentally confirmed to possess this property. In this study, we employ first-principles calculations, combined with a structural search based on an evolutionary algorithm, to predict a class of 2D QSH insulators in hafnium halides, namely, HfF, HfCl, and HfBr with sizable band gaps of 0.12, 0.19, and 0.38 eV. Their topological nontrivial nature is confirmed by a Z 2 invariant which equals to 1 and the presence of gapless edge states. Furthermore, the QSH effect in these materials remains robust under biaxial tensile strain of up to 10%, and the use of h -BN as a substrate effectively preserves the QSH states in these materials. Our findings pave the way for future theoretical and experimental investigations of 2D hafnium halides and their potential for realizing the QSH effect.