Colloidal Continuous Injection Synthesis of Fluorescent MoX₂ (X = S, Se) Nanosheets as a First Step Toward Photonic Applications

Transition-metal dichalcogenide (TMD) nanosheets have become an intensively investigated topic in the field of 2D nanomaterials, especially due to the direct semiconductor nature, and the broken inversion symmetry in the odd-layer number, of some of their family members. These properties make TMDs attractive for different technological applications such as photovoltaics, optoelectronics, valleytronics, and hydrogen evolution reactions. Among them, MoX2 (X = S and Se) are turned to direct gap when their thickness is thinned down to monolayer, and thus, efforts toward obtaining large-scale monolayer TMDs are crucial for technological applications. Colloidal synthesis of TMDs has been developed in recent years, as it provides a cost-efficient and scalable way to produce few-layer TMDs having homogeneous size and thickness, yet obtaining a monolayer has proven challenging. Here, we present a method for the colloidal synthesis of mono- and few-layer MoX2 (X = S and Se) using elemental chalcogenide and metal chloride as precursors. Using a synthesis with slow injection of the MoCl5 precursor under a nitrogen atmosphere, and optimizing the synthesis parameters with a design of experiments approach, we obtained a MoX2 sample with the semiconducting (1H) phase and optical band gaps of 1.96 eV for 1H–MoS2 and 1.67 eV for 1H–MoSe2, respectively, consistent with a large monolayer yield in the ensemble. Both display photoluminescence at cryogenic and room temperature, paving the way for optical spectroscopy studies and photonic applications of colloidal TMD nanosheets.