Water flattens graphene wrinkles: Laser shock wrapping of graphene onto substrate-supported crystalline plasmonic nanoparticle arrays

Hot electron injection into an exceptionally high mobility material can be realized in graphene-plasmonic nanoantenna hybrid nanosystems, which can be exploited for several front-edge applications including photovoltaics, plasmonic waveguiding and molecular sensing at trace levels. Wrinkling instabilities of graphene on these plasmonic nanostructures, however, would cause reactive oxygen or sulfur species to diffuse and react with the materials, decrease charge transfer rates and block intense hot-spots. No ex situ graphene wrapping technique has been explored so far to control these wrinkles. Here, we present a method to generate seamless integration by using water as a flyer to transfer the laser shock pressure to wrap graphene onto plasmonic nanocrystals. This technique decreases the interfacial gap between graphene and the covered substrate-supported plasmonic nanoparticle arrays by exploiting a shock pressure generated by the laser ablation of graphite and the water impermeable nature of graphene. Graphene wrapping of chemically synthesized crystalline gold nanospheres, nanorods and bipyramids with different field confinement capabilities is investigated. A combined experimental and computational method, including SEM and AFM morphological investigation, molecular dynamics simulation, and Raman spectroscopy characterization, is used to demonstrate the effectiveness of this technique. Graphene covered gold bipyramid exhibits the best result among the hybrid nanosystems studied. We have shown that the hybrid system fabricated by laser shock can be used for enhanced molecular sensing. The technique developed has the characteristics of tight integration, and chemical/thermal stability, is instantaneous in nature, possesses a large scale and room temperature processing capability, and can be further extended to integrate other 2D materials with various 0-3D nanomaterials.