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Nonlinear optical phenomena play a critical role in understanding microscopiclight-matter interactions and have far-reaching applications across variousfields, such as biosensing, quantum information, optical switching, andall-optical data processing. Most of these applications require materials withhigh third-order absorptive and refractive optical nonlinearities. However,most materials show weak nonlinear optical responses due to their perturbativenature and often need to be improved for practical applications. Here, wedemonstrate that the charge donor-acceptor hybrid of VSe2-reduced grapheneoxide (rGO) hybrid exhibits enhanced ultrafast third-order absorptive andrefractive nonlinearities compared to the pristine systems, at least by oneorder of magnitude. Through density functional theory and Bader chargeanalysis, we elucidate the strong electronic coupling in the VSe2-rGO hybrid,involving the transfer of electrons from VSe2 to rGO. Steady-state andtime-resolved photoluminescence (PL) measurements confirm the electroniccoupling and charge transfer. Furthermore, we fabricate an ultrafast opticallimiter device with better performance parameters, such as an onset thresholdof 2.5 mJ cm-2 and differential transmittance of 0.42.

Enhancing the ultrafast third order nonlinear optical response by charge transfer in VSe2-reduced graphene oxide hybrid