Optical spectroscopic detection of Schottky barrier height at a two-dimensional transition-metal dichalcogenide/metal...

Atomically thin two-dimensional transition-metal dichalcogenides (2D-TMDs) have emerged as semiconductors for next-generation nanoelectronics. As 2D-TMD-based devices typically utilize metals as the contacts, it is crucial to understand the properties of the 2D-TMD/metal interface, including the characteristics of the Schottky barriers formed at the semiconductor-metal junction. Conventional methods for investigating the Schottky barrier height (SBH) at these interfaces predominantly rely on contact-based electrical measurements with complex gating structures. In this study, we introduce an all-optical approach for non-contact measurement of the SBH, utilizing high-quality WS₂/Au heterostructures as a model system. Our approach employs a below-bandgap pump to excite hot carriers from the gold into WS₂ with varying thicknesses. By monitoring the resultant carrier density changes within the WS₂ layers with a broadband probe, we traced the dynamics and magnitude of charge transfer across the interface. A systematic sweep of the pump wavelength enables us to determine the SBH values and unveil an inverse relationship between the SBH and the thickness of the WS₂ layers. First-principles calculations reveal the correlation between the probability of injection and the density of states near the conduction band minimum of WS₂. The versatile optical methodology for probing TMD/metal interfaces can shed light on the intricate charge transfer characteristics within various 2D heterostructures, facilitating the development of more efficient and scalable nano-electronic and optoelectronic technologies.