The combination of graphene with noble-metal nanostructures is currently being explored for strong light-graphene interaction enhanced by plasmons. We introduce a novel hybrid graphene-metal system for studying light-matter interactions with gold-void nanostructures exhibiting resonances in the visible range. Strong coupling of graphene layers to the plasmon * To whom correspondence should be addressed â DTU Fotonik ⥠CNG ¶ Fudan University § DTU Nanotech CINF 1 modes of the nanovoid arrays results in significant frequency shifts of the underlying plasmon resonances, enabling more than 30% absolute light absorption in a single layer of graphene and up to 700-fold enhancement of the Raman response of the graphene. These new perspectives enable us to verify the presence of graphene on gold-void arrays and the enhancement even allows us to accurately quantify the number of layers. Experimental observations are further supported by numerical simulations and perturbation-theory analysis. The graphene gold-void platform is beneficial for sensing of molecules and placing R6G dye molecules on top of the graphene, we observe a strong enhancement of the R6G Raman fingerprints. These results pave the way toward advanced substrates for surface-enhanced Raman scattering (SERS) with potential for unambiguous single-molecule detection on the atomically well-defined layer of graphene.Graphene is an atomic monolayer formed by carbon hexagons, whose extraordinary electrical and optical properties have led to a range of promising optoelectronic devices, 1-3 such as photodetectors, 4 optical modulators, 5 and ultra-fast lasers. 6 However, all such devices suffer from the inherently weak interaction between pristine graphene and light (2.3% light absorption at normal incidence), therefore imposing substantial challenges and restrictions for many electro-optical and all-optical applications. 7,8 Doped graphene nanostructures which support surface plasmons in the teraherz and infrared regions offer an exciting route to increase the light-graphene interaction by confining the optical fields below the diffraction limit. 9-13 However, graphene is less attractive when the interband loss becomes large, and it effectively mimics a dielectric material in the visible and near-infrared frequencies. 14 One alternative way to enhance the light-graphene interaction in short wavelengths is the combination of graphene with conventional plasmonic nanostructures based on noble metals. 15 These graphene-plasmonic hybrid structures could be beneficial for both fields of investigation: first of all, graphene can influence the optical response of plasmonic structures leading to graphene-based tunable plasmonics, 16 and in turn, plasmonic nanostructures can dramatically enhance the local electric field, leading to strong light absorption and Raman signature of graphene layers.In this Letter, a novel platform based on graphene-covered gold nanovoid arrays (GNVAs) is 2 proposed to enhance the light-matter interaction in graphene-plasmonic hybrid str...