Layer‐Dependent Dielectric Function of Wafer‐Scale 2D MoS₂

Abstract Wafer‐scale, high‐quality, and layer‐controlled 2D MoS₂ films on c‐sapphire are synthesized by an innovative two‐step method. The dielectric functions of MoS₂ ranging from the monolayer to the bulk are investigated by spectroscopic ellipsometry over an ultra‐broadband (0.73–6.42 eV). Up to five critical points (CPs) in the dielectric function spectra are precisely distinguished by CP analysis, and their physical origins are identified in the band structures with the help of first‐principles calculations. Results demonstrate that the center energies of these CPs exhibit intriguing layer dependency, which are interpreted by the intrinsic layer‐dependent transitions in MoS₂. Specially, the change in the imaginary part of the dielectric functions versus the thickness exhibits a “W” like curve, and the two valley bottoms appear at about four‐layer and 10‐layer respectively. These complex fluctuations are attributed to the alternating domination of the decreasing excitonic effect, the increasing joint density of states, and the mass density increase in relative thick MoS₂ samples.