Impact and Origin of Interface States in MOS Capacitor with Monolayer MoS2 and HfO2 High-k Dielectric

Two-dimensional layered semiconductors such as molybdenum disulfide (MoS2) at the quantum limit are promising material for nanoelectronics and optoelectronics applications. Understanding the interface properties between the atomically thin MoS2 channel and gate dielectric is fundamentally important for enhancing the carrier transport properties. Here, we investigate the frequency dispersion mechanism in a metal-oxide-semiconductor capacitor (MOSCAP) with a monolayer MoS2 and an ultra-thin HfO2 high-k gate dielectric. We show that the existence of sulfur vacancies at the MoS2-HfO2 interface is responsible for the generation of interface states with a density (D-it) reaching similar to 7.03 x 10(11) cm(-2) eV(-1). This is evidenced by a deficit S: Mo ratio of similar to 1.96 using X-ray photoelectron spectroscopy (XPS) analysis, which deviates from its ideal stoichiometric value. First-principles calculations within the density-functional theory framework further confirms the presence of trap states due to sulfur deficiency, which exist within the MoS2 bandgap. This corroborates to a voltage-dependent frequency dispersion of similar to 11.5% at weak accumulation which decreases monotonically to similar to 9.0% at strong accumulation as the Fermi level moves away from the mid-gap trap states. Further reduction in D-it could be achieved by thermally diffusing S atoms to the MoS2-HfO2 interface to annihilate the vacancies. This work provides an insight into the interface properties for enabling the development of MoS2 devices with carrier transport enhancement.