Enhancing Single-Molecule Fluorescence Spectroscopy with Simple and Robust Hybrid Nanoapertures.

Plasmonic nanoapertures have found exciting applications in optical sensing, spectroscopy, imaging, and nanomanipulation. The subdiffraction optical field localization, reduced detection volume (~attoliters), and background-free operation make them particularly attractive for single-particle and single-molecule studies. However, in contrast to the high field enhancements by traditional "nanoantenna"-based structures, small field enhancement in conventional nanoapertures results in weak light-matter interactions and thus small enhancement of spectroscopic signals (such as fluorescence and Raman signals) of the analytes interacting with the nanoapertures. In this work, we propose a hybrid nanoaperture design termed "gold-nanoislands-embedded nanoaperture" (AuNIs-e-NA), which provides multiple electromagnetic "hotspots" within the nanoaperture to achieve field enhancements of up to 4000. The AuNIs-e-NA was able to improve the fluorescence signals by more than 2 orders of magnitude with respect to a conventional nanoaperture. With simple design and easy fabrication, along with strong signal enhancements and operability over variable light wavelengths and polarizations, the AuNIs-e-NA will serve as a robust platform for surface-enhanced optical sensing, imaging, and spectroscopy.