Aluminum Metasurface with Hybrid Multipolar Plasmons for 1000-Fold Broadband Visible Fluorescence Enhancement and Multiplexed Biosensing

Aluminum (Al)-based nanoantennae traditionally suffer from weak plasmonic performance in the visible range, necessitating the application of more expensive noble metal substrates for rapidly expanding biosensing opportunities. We introduce a metasurface comprising Al nanoantennae of nanodisks-in-cavities that generate hybrid multipolar lossless plasmonic modes to strongly enhance local electromagnetic fields and increase the coupled emitter's local density of states throughout the visible regime. This results in highly efficient electromagnetic field confinement in visible wavelengths by these nanoantennae, favoring real-world plasmonic applications of Al over other noble metals. Additionally, we demonstrate spontaneous localization and concentration of target molecules at metasurface hotspots, leading to further improved on-chip detection sensitivity and a broadband fluorescence-enhancement factor above 1000 for visible wavelengths with respect to glass chips commonly used in bioassays. Using the metasurface and a multiplexing technique involving three visible wavelengths, we successfully detected three biomarkers, insulin, vascular endothelial growth factor, and thrombin relevant to diabetes, ocular and cardiovascular diseases, respectively, in a single 10 μL droplet containing only 1 fmol of each biomarker.