semiconductors, including Si and Ge, the mobility drastically degrades when the channel thickness of the conductor is below 5 nm due to thickness-fluctuationinduced scattering. [2] On the other hand, 2D materials maintain high mobility even under the monolayer limit (0.3-0.6 nm) [3][4][5] and exhibit inherently high on-current, as evidenced by the stronger quantummechanical effect that is observed. [6] In particular, transition metal dichalcogenides (TMDCs) are attractive materials for semiconductor channels of nanoscale FETs because of their high stability against oxidation [7] as well as their superior electrical properties, such as a large bandgap and relatively high carrier mobility. [3][4][5] Here, the large challenge with 2D-FET always involves the formation of highquality ultrathin high-κ oxide insulators. The atomic layer deposition (ALD) of dielectrics on TMDCs has a disadvantage in that high capacitive top gate stacks are formed on TMDCs because the nucleation of the oxide predominantly occurs at defect sites or through the physical adsorption of precursors onto the surface due to the absence of dangling bonds, [8] as shown in Figure 1a. Therefore, thick dielectrics are required to cover the whole surface without pinholes. [9] To form thin oxides with high dielectric constants by the ALD method, it is necessary to intentionally form nucleation sites on TMDCs. In fact, various surface modification methods, including surface treatment [10,11] and the formation of a buffer layer, [12][13][14][15][16][17][18] have been reported for oxide formation on TMDCs with high uniformity and dielectric properties. A surface treatment, including O 2 plasma [10] and ultraviolet ozone, [11] has improved the coverage and uniformity of ALD oxide on TMDCs; however, this treatment induces additional defects that produce extra scattering sites or dopants on TMDCs.The deposition of a buffer layer, including thin metal layers [12][13][14][15] and organic molecules, [16][17][18] is an effective method to provide nucleation sites without forming defects. To date, the thinnest equivalent oxide thickness (EOT) of 1 nm on monolayer TMDCs has been successfully reported by combining an organic monolayer of 3,4,9,10-perylene-tetracarboxylic dianhydride (PTCDA) and ALD-HfO 2 for the top gate stack. [18] However, due to the quite low dielectric constant of PTCDA