Broadband optical properties of large-area monolayer CVD molybdenum disulfide

Recently emerging large-area single-layer MoS2 grown by chemical vapor deposition has triggered great interest due to its exciting potential for applications in advanced electronic and optoelectronic devices. Unlike gapless graphene, MoS2 has an intrinsic band gap in the visible which crosses over from an indirect to a direct gap when reduced to a single atomic layer. In this paper, we report a comprehensive study of fundamental optical properties of MoS2 revealed by optical spectroscopy of Raman, photoluminescence, and vacuum ultraviolet spectroscopic ellipsometry. A band gap of 1.42 eV is determined by the absorption threshold of bulk MoS2 that shifts to 1.83 eV in monolayer MoS2. We extracted the high precision dielectric function up to 9.0 eV, which leads to the identification of many unique interband transitions at high symmetry points in the MoS2 momentum space. The positions of the so-called A and B excitons in single layers are found to shift upwards in energy compared with those of the bulk form and have smaller separation because of the decreased interactions between the layers. A very strong optical critical point predicted to correspond to a quasiparticle gap is observed at 2.86 eV, which is attributed to optical transitions along the parallel bands between the M and Gamma points in the reduced Brillouin zone. The absence of the bulk MoS2 spin-orbit interaction peak at similar to 3.0 eV in monolayer MoS2 is, as predicted, the consequence of the coalescence of nearby excitons. A higher energy optical transition at 3.98 eV, commonly occurring in bulk semiconductors, is associated with a combination of several critical points. Additionally, extending into the vacuum ultraviolet energy spectrum are a series of newly observed oscillations representing optical transitions from valence bands to higher conduction bands of the monolayer MoS2 complex band structure. These optical transitions herein reported enhance our understanding of monolayer MoS2 as well as of two-dimensional systems in general and thus provide informative guidelines for MoS2 optical device designs and theoretical considerations.