High-Throughput Fabrication of Ultradense Annular Nanogap Arrays for Plasmon-Enhanced Spectroscopy

The confinement of light into nanometer-sized metallic nanogaps can lead to an extremely high field enhancement, resulting in dramatically enhanced absorption, emission, and surface-enhanced Raman scattering (SERS) of molecules embedded in nanogaps. However, low-cost, high-throughput, and reliable fabrication of ultra-high-dense nanogap arrays with precise control of the gap size still remains a challenge. Here, by combining colloidal lithography and atomic layer deposition technique, a reproducible method for fabricating ultra-high-dense arrays of hexagonal close-packed annular nanogaps over large areas is demonstrated. The annular nanogap arrays with a minimum diameter smaller than 100 nm and sub-1 nm gap width have been produced, showing excellent SERS performance with a typical enhancement factor up to 3.1 × 10⁶ and a detection limit of 10^-11 M. Moreover, it can also work as a high-quality field enhancement substrate for studying two-dimensional materials, such as MoSe₂. Our method provides an attractive approach to produce controllable nanogaps for enhanced light-matter interaction at the nanoscale.