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 (EBD) 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.