Imaging of Defect-Accelerated Energy Transfer in MoS/hBN/WS Heterostructures.

Engineering energy transfer (ET) plays an important role in the exploration of novel optoelectronic devices. The efficient ET has been reasonably regulated using different strategies, such as dielectric properties, distance, and stacking angle. However, these strategies show limited degrees of freedom in regulation. Defects can provide more degrees of freedom, such as the type and density of defects. Herein, atomic-scale defect-accelerated ET is directly observed in MoS/hBN/WS heterostructures by fluorescence lifetime imaging microscopy. Sulfur vacancies with different densities are introduced by controlling the oxygen plasma irradiation time. Our study shows that the ET rate can be increased from 1.25 to 6.58 ns by accurately controlling the defect density. Also, the corresponding ET time is shortened from 0.80 to 0.15 ns, attributing to the participation of more neutral excitons in the ET process. These neutral excitons are transformed from trion excitons in MoS, assisted by oxygen substitution at sulfur vacancies. Our insights not only help us better understand the role of defects in the ET process but also provide a new approach to engineer ET for further exploration of novel optoelectronic devices in van der Waals heterostructures.