Large area single crystal gold of single nanometer thickness for nanophotonics

Two-dimensional single crystal metals, in which the behavior of highly confined optical modes is intertwined with quantum phenomena, are highly sought after for next-generation technologies. Here, we report large area (>10 4 μm 2 ), single crystal two-dimensional gold flakes (2DGFs) with thicknesses down to a single nanometer level, employing an atomic-level precision chemical etching approach. The decrease of the thickness down to such scales leads to the quantization of the electronic states, endowing 2DGFs with quantum-confinement-augmented optical nonlinearity, particularly leading to more than two orders of magnitude enhancement in harmonic generation compared with their thick polycrystalline counterparts. The nanometer-scale thickness and single crystal quality makes 2DGFs a promising platform for realizing plasmonic nanostructures with nanoscale optical confinement. This is demonstrated by patterning 2DGFs into nanoribbon arrays, exhibiting strongly confined near infrared plasmonic resonances with high quality factors. The developed 2DGFs provide an emerging platform for nanophotonic research and open up opportunities for applications in ultrathin plasmonic, optoelectronic and quantum devices. 2D metallic single crystals are sought after for nanophotonic applications, but their synthesis remains challenging. Here, the authors report an atomic level precision etching method to fabricate large-area crystalline gold flakes with nanometre thickness, showing enhanced plasmonic and nonlinear optical properties.