Single-Layer Zirconium Dihalides ZrX2 (X = Cl, Br, and I) with Abnormal Ferroelastic Behavior and Strong Anisotropic Light Absorption Ability

Recently, two-dimensional (2D) metal halides have brought out an intensive interest for their unique mechanical, electronic, magnetic, and topological properties. Here, we theoretically report the existence of the single-layer (SL) zirconium dihalide materials ZrX2 (X = Cl, Br, and I) using first-principles calculations. SL ZrX2, which can be obtained from its bulk phase through simple mechanical exfoliation, shows the dynamic, thermodynamic, and mechanical stability. Halogen atoms can effectively tune the electronic structure, dipole moment transition, band alignment, and light absorption. Specifically, ZrX2 monolayers intrinsically exhibit a ferroelasticity with an abnormal 120° orientation rotation, possessing a moderate switching barrier of 24–39 meV/atom. Importantly, we observe superior anisotropic light absorption responses on SL ZrX2 in the visible region. Besides, a series of ZrX2-based excitonic solar cells have been proposed, which hold a large power conversion efficiency limit of 12.4–18.7%.