Ultralarge Photoluminescence Enhancement of Monolayer Molybdenum Disulfide by Spontaneous Superacid Nanolayer Formation

Due to the direct band gap nature, extensive studies have been conducted to improve the optical behavior in monolayer transition metal dichalcogenides (TMDCs) with a formula of MX2 (M = Mo, W; X = S, Se, Te). One of the strongest modulating agents of optical behavior is a molecular superacid treatment; however, the chemical event has not been unveiled. Also, the engineering protocol for keeping the treatment is immature. In this work, we systematically study the superacid treatment procedures on monolayer molybdenum disulfide (MoS2) and propose that the interaction, a hydrophilic interaction, between the superacid molecule and MoS2 surface would be critical. As a result of the interaction, the superacid molecules spontaneously form an acidic layer with the thickness of several nanometers on the surface. The power-dependent photoluminescence (PL) measurement indicates the edge of MoS2 flake is more effective and electronically modulated by the treatment. By understanding the superacid nanolayer formation by the treatment, we succeeded in maintaining the ultrastrong PL in the superacid-treated MoS2 for more than 30 days in the ambient air by encapsulation with transparent organic polymers. This study advances the understanding and designing applications of strong luminescent properties in the superacid-treated TMDCs and paves the way toward engineering exciton dynamics and an experimental platform for treating multibody states.