Controllable Oxidation of ZrS2 to Prepare High‐κ, Single‐Crystal m‐ZrO2 for 2D Electronics

High-κ materials that exhibit large permittivity and band gaps are needed as gate dielectrics to enhance capacitance and prevent leakage current in downsized technology nodes. Among these, monoclinic ZrO₂ (m-ZrO₂ ) shows good potential because of its inertness and high-κ with respect to SiO₂ , but a method to produce ultrathin single crystal is lacking. Here, the controllable preparation of ultrathin m-ZrO₂ single crystals via the in situ thermal oxidation of ZrS₂ is achieved. As-grown m-ZrO₂ presents an equivalent oxide thickness of ≈0.29 nm, a high dielectric constant of ≈19, and a breakdown voltage (E_BD ) of ≈7.22 MV cm^-1 . MoS₂ field effect transistor (FET) by using m-ZrO₂ as a dielectric layer shows comparable mobility to that using SiO₂ dielectric. The ultraclean interface of m-ZrO₂ /MoS₂ and high crystalline quality of m-ZrO₂ lead to negligible hysteresis in transfer curves. Single crystal m-ZrO₂ dielectric shows potential application in digital complementary metal oxidesemiconductor (CMOS) logic FET.