Excitonic Rydberg States in a Trilayer to Monolayer H2-Aided CVD-Grown Large-Area MoS2 Film with Excellent UV to Visible Broad Band Photodetection Applications

The diverse nature of optoelectronic properties of few-layer or monolayer MoS2 is generally dominated by A and B excitons. Occasionally, strong Coulombic interactions within the 2D monolayer led to the creation of hydrogen-like Rydberg states of excitons in MoS2 similar to other 2D monolayers. In this paper, a simple process is used to convert trilayer MoS2 films to a monolayer by introducing H2 gas during chemical vapor deposition. Remarkably, alongside the usual A, B excitons, and A- trion, the appearance of the Rydberg states is evidenced by photoluminescence spectra even at room temperature; also, there is an increase in their areal percentage with an increase in H2 content. The s-type excited Rydberg states up to the fourth order (n = 5) and third order (n = 4) of A and B excitons, respectively, have been probed from the photoluminescence spectra at 93 K. Unprecedentedly, the first-order derivative of room-temperature photocurrent spectrum reveals the Rydberg states concurrently and elaboratively. Furthermore, the large-area MoS2 films exhibit photoresponse in a broad UV to visible region with excellent photosensitivity (∼102) toward both UV and visible lights. Not only does this provide a profound understanding of the excitonic Rydberg states but also highlights the considerable potential of large-area monolayer MoS2 overcoming the difficulty of tiny flake-related 2D device endeavors.