By creating defects via oxygen plasma treatment, we demonstrate optical properties variation of single-layer MoS 2 . We found that, with increasing plasma exposure time, the photoluminescence (PL) evolves from very high intensity to complete quenching, accompanied by gradual reduction and broadening of MoS 2 Raman modes, indicative of distortion of the MoS 2 lattice after oxygen bombardment. X-ray photoelectron spectroscopy study shows the appearance of Mo 6+ peak, suggesting the creation of MoO 3 disordered regions in the MoS 2 flake. Finally, using band structure calculations, we demonstrate that the creation of MoO 3 disordered domains upon exposure to oxygen plasma leads to a direct to indirect bandgap transition in single-layer MoS 2 , which explains the observed PL quenching. KEYWORDS 2D materials, defect engineering, optical properties, bandgap tuning, molybdenum trioxide
INTRODUCTIONThe ability to controllably tailor the properties of a material is a key factor in the development of many novel applications. In the case of bulk semiconductors, creating and manipulating defects constitutes an essential element in controlling the electrical, magnetic, and optical properties of the host material. 1 Although the role of defects is well understood in bulk semiconductors, it has received little attention in emerging two-dimensional (2D) layered semiconductors, preventing their full exploitation for tailored 2D nanoelectronic and photonic devices. Graphene and graphene oxide are examples of the impact that defects can have on 2D materials. Pristine graphene, which contains no intrinsic defect, is well known for its extraordinary high mobility, and is of great importance for high frequency device applications. 2, 3 However, its inherent lack of bandgap and low absorption of solar photons greatly limit its use in electronic and photonic devices. On the other hand, its solution processed counterparts, graphene oxide and reduced graphene oxide, have a large amount of defects, which lead to formation of a bandgap and open the way to many other applications in photodetectors, sensors, catalysis, and solar cell. [4][5][6][7][8] Recently, layered transition metal dichalcogenides (TMDs) have emerged as important materials for 2D device engineering. 9-11 Molybdenum disulfide (MoS 2 ), composed of weak van der Waals bonded S-Mo-S units, offers a large intrinsic bandgap that is strongly dependent on the number of layers, with an indirect bandgap (1.2 eV) in bulk MoS 2 transitioning to a direct