Tuning of Interlayer Coupling in Large-Area Graphene/WSe2 van der Waals Heterostructure via Ion Irradiation: Optical Evidences and Photonic Applications

van der Waals (vdW) heterostructures are receiving great attentions due to their intriguing properties and potentials in many research fields. The flow of charge carriers in vdW heterostructures can be efficiently rectified by the interlayer coupling between neighboring layers, offering a rich collection of functionalities and a mechanism for designing atomically thin devices. Nevertheless, nonuniform contact in larger-area heterostructures reduces the device efficiency. In this work, ion irradiation had been verified as an efficient technique to enhance the contact and interlayer coupling in the newly developed graphene/WSe2 heterostructure with a large area of 10 mm × 10 mm. During the ion irradiation process, the morphology of monolayer graphene had been modified, promoting the contact with WSe2. Experimental evidence of the tunable interlayer electron transfer are displayed by investigation of photoluminescence and ultrafast absorption of the irradiated heterostructure. Besides, we have found that in graphene/WSe2 heterostructure, graphene serves as a fast channel for the photoexcited carriers to relax in WSe2, and the nonlinear absorption of WSe2 could be effectively tuned by the carrier transfer process in graphene, enabling specific optical absorption of the heterostructure in comparison with separated graphene or WSe2. On the basis of these new findings, by applying the ion beam modified graphene/WSe2 heterostructure as a saturable absorber, Q-switched pulsed lasing with optimized performance has been realized in a Nd:YAG waveguide cavity. This work paves the way toward developing novel devices based on large-area heterostructures by using ion beam irradiation.