Removal of Defect Bound Exciton in Aged Monolayer WS2 by Laser Processing

The exciton complexes in two-dimensional materials have long fascinated scientists and researchers for their mechanisms in fundamental photo-physics. And it is well established that the evolution of defect bound excitons in two-dimensional semiconducting TMDs brings largely unexplored opportunities for tailoring their optoelectronic properties. Yet thus far, the properties of defect bound excitons of TMDs have been rarely investigated. In this work, the intrinsic properties of defect bound excitons in aged CVD-grown monolayer WS2 are experimentally studied by the steady-state photoluminescence measurement. Specifically, the photoluminescence mapping experiment is conducted to demonstrate the spatial distribution of the defect bound excitons, whose spectral feature is located similar to 0.2 eV below the neutral free A-excitons. Additionally, the power-dependent photoluminescence experiment is applied to investigate the behavior of the defect-state photoluminescence and a significant nonlinear dependence of defect bound excitons on excitation power is revealed. Furthermore, we directly observed the disappearance of defect-state photoluminescence by exposing sample to high laser power irradiation, which can be explained by the enhanced desorption process of molecules physiosorbed on surfaces under laser irradiation. The results of our work provide a comprehensive understanding for the defect bound excitons in monolayer tungsten disulfide, which is essential in promoting the development of defect engineering about two-dimensional semiconducting TMDs and may pave the way for tailoring the performance of the optoelectronic device.