Two-dimensional (2D) structures composed of atomically thin materials with high carrier mobility have been studied as candidates for future transistors1-4. However, owing to the unavailability of suitable high-quality dielectrics, 2D field-effect transistors (FETs) cannot attain the full theoretical potential and advantages despite their superior physical and electrical properties3,5,6. Here we demonstrate the fabrication of atomically thin single-crystalline Al2O3 (c-Al2O3) as a high-quality top-gate dielectric in 2D FETs. By using intercalative oxidation techniques, a stable, stoichiometric and atomically thin c-Al2O3 layer with a thickness of 1.25 nm is formed on the single-crystalline Al surface at room temperature. Owing to the favourable crystalline structure and well-defined interfaces, the gate leakage current, interface state density and dielectric strength of c-Al2O3 meet the International Roadmap for Devices and Systems requirements3,5,7. Through a one-step transfer process consisting of the source, drain, dielectric materials and gate, we achieve top-gate MoS2 FETs characterized by a steep subthreshold swing of 61 mV dec-1, high on/off current ratio of 108 and very small hysteresis of 10 mV. This technique and material demonstrate the possibility of producing high-quality single-crystalline oxides suitable for integration into fully scalable advanced 2D FETs, including negative capacitance transistors and spin transistors.
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