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Due to the absence of dangling bonds, the integration of ultra-thin dielectric on 2D semiconductors has become a huge challenge, and its reliability research has been blank before. For the first time, we report the high $-\mathcal{K}$ dielectric reliability on Mos2. By PTCDA crystal as interface layer, we demonstrated excellent reliability of HfO 2 /PTCDA gate stack, including EBD over 8.9 MV/cm, $\mathrm{E}_{\text{BD}}\ ^{10\text{yrs}}$ over 6.5 MV/cm and ultra-low BD rate, all of which show better reliability than HfO 2 /Si.

2D semiconductors are considered to be one of the most promising channel materials to extend transistor scaling. However, the integration of ultra-thin dielectrics on 2D semiconductors has been challenging, and the reliability has not been investigated to date. Here, using monolayer 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) molecules as interface layer, we realize EOT as low as 1.7 nm on large-area monolayer CVD MoS 2 . The reliability of ultrathin high-κ dielectric on 2D semiconductors is systematically studied for the first time. The median breakdown (BD) field of HfO 2 /PTCDA stack is over 8.42 MV/cm, which is two times that of HfO 2 /Si under the same EOT. Through TDDB we project that the gate dielectric can work reliably for 10 years under E BD = 6.5 MV/cm, which shows 85% improvement than HfO 2 /Si. The BD current increase rate in our gate stack is several orders of magnitude smaller than HfO 2 /Si. The excellent reliability suggests that molecular interfacial layer is a promising dielectric technology for 2D electronics.