Laser Parallel Nanofabrication of Dual‐Au‐Nanoholes on Microsphere‐Lens‐Array for Polarization‐Dependent SERS

Abstract High‐efficient fabrication of well‐ordered nanostructures on flexible substrates is a challenge to surface‐enhanced Raman spectroscopy (SERS) for analytical fingerprinting trace‐detection. In this work, a laser parallel nanofabrication method is reported via incident‐angle‐dependent photonic nanojet ablating Au film on the bottom surface of microsphere‐lens‐array (MLA), for combination with formed dual Au‐nanoholes (MLA/2‐Au NH s) as the flexible SERS substrates. The process parameters, i.e., pulsed laser energy, MLA diameter, Au film thickness, and laser incident angle, are optimized for high finish‐quality of dual‐Au NH s with a diameter of ≈875 nm and a tip gap of ≈90 nm. The SERS substrate demonstrates the limit of detection down to 10 −11 M for 4‐nitrobenzenethiol molecules by the multiple optical regulations, including self‐aligned focusing to the hotspots and directional antenna, the strongly localized surface plasmon resonances, and optical whispering‐gallery modes for resonance energy transfer. The flexible PDMS film supporting the rigid MLA holds the SERS performance of MLA/2‐Au NHs with high flexibility. Moreover, the MLA/2‐Au NHs SERS substrate exhibits differential responses to orthogonally polarized excitation, by which the background noises can be eliminated to improve the Raman spectrum. The present work opens new opportunities to fabricate dielectric‐metal flexible SERS substrates by laser parallel nanofabrication via MLA for Raman trace detection.