Observation of photoluminescence from large-scale layer-controlled 2D ß-Cu₂S synthesized by the vapor-phase sulfurization of copper thin films

Two-dimensional (2D) copper chalcogenides (Cu_2-x X where X=S, Se, Te) have had much attention regarding various applications due to their remarkable optical and electrical properties, abundance, and environmentally friendly natures. This work indicates that highly uniform Cu_2-xS (where 0<x<1) nanosheets can be obtained by the two-step method of Cu deposition by sputtering with precisely controlled and extremely low growth rate followed by vapor-phase sulfurization. The phase transformations of thin Cu_2-xS films upon the Cu seed layer thickness are investigated. A unique thickness-constrained synthesis process using vapor-phase sulfurization is employed here, which evolves from a vertical to lateral growth mechanism based on the optimization of the Cu seed layer thickness. Atomically thin 2D β-Cu₂S film was successfully synthesized using the thinnest Cu seed film. We have systematically investigated the phase- and thickness-dependent optical properties of Cu_2-xS films at room temperature. Micro-photoluminescence (PL) spectroscopy reveals that the 2D β-Cu₂S film possesses a direct band gap with an energy of 1.1 eV while the PL intensities are greatly suppressed in the multilayer Cu_2-xS (where 0≤x<1).