Abstract Interlayer charge‐transfer (CT) in 2D atomically thin vertical stacks heterostructures offers an unparalleled new approach to regulation of device performance in optoelectronic and photonics applications. Despite the fact that the saturable absorption (SA) in 2D heterostructures involves highly efficient optical modulation in the space and time domain, the lack of explicit SA regulation mechanism at the nanoscale prevents this feature from realizing nanophotonic modulation. Here, the enhancement of SA response via CT in WS2/graphene vertical heterostructure is proposed and the related mechanism is demonstrated through simulations and experiments. Leveraging this mechanism, CT‐induced SA enhancement can be expanded to a wide range of nonlinear optical modulation applications for 2D materials. The results suggest that CT between 2D heterostructures enables efficient nonlinear optical response regulation.
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