ACS Nano · 2023 · 37 citations · 49 references
Natural SciencesMaterials EngineeringMaterials ScienceNanotechnologyOptical MaterialsPhotonicsNonlinear Optical MaterialsNonlinear OpticsPlasmonic MaterialsPlasmonic NanomaterialsPlasmonicsUltrafast OpticsCarrier Relaxation DynamicsElectron Relaxation DynamicsHybrid Plasmonic StructuresInfrared Nonlinear Optical MaterialsMetamaterialsPhotoinduced AbsorptionPlasmonic MetamaterialsUltrafast Optical Response
Exploring emerging materials with enhanced optical nonlinearities at low power levels with ultrafast response and small footprints is of great interest for information processing, communication, sensing, and quantum systems. Recent progress on nonlinear metamaterials and metasurfaces suggests promising solutions to overcome the limitations of nonlinear materials in nature. Here we present a design concept for highly enhanced saturable absorption effect based on subwavelength-thick (<1/5λ 0 ) hybrid graphene-plasmonic metasurface structures in infrared wavelengths. Our theoretical and experimental results demonstrated that, by exciting nonequilibrium carriers inside nanoscale hotspots, one could not only enhance the saturable absorption in graphene, but also reduce the saturation fluence by over 3 orders of magnitude (from ∼1 mJ/cm 2 to ∼100 nJ/cm 2 ). Our pump–probe measurement results suggested an ultrashort saturable absorption recovery time (<60 fs), which is ultimately determined by the relaxation dynamics of photoexcited carriers in graphene. We also observed pulse narrowing effects in our devices based on the autocorrelation measurement results. Such design concepts can be tailored via structure engineering to operate in broader wavelength ranges up to mid- and far- infrared spectral regions. These ultrafast low-saturation fluence saturable absorber designs can enable low-threshold, compact, self-starting mode-locked lasers, laser pulse shaping, and high-speed optical information processing.
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