Femtosecond Laser-Induced, Nanoparticle-Embedded Periodic Surface Structures on Crystalline Silicon for Reproducible and Multi-utility SERS Platforms

[Image: see text] Fabrication of reproducible and versatile surface-enhanced Raman scattering (SERS) substrates is crucial for real-time applications such as explosive detection for human safety and biological imaging for cancer diagnosis. However, it still remains a challenging task, even after several methodologies were developed by various research groups, primarily due to (a) a lack of consistency in detection of a variety of molecules (b) cost-effectiveness of the SERS substrates prepared, and (c) byzantine preparation procedures, etc. Herein, we establish a procedure for preparing reproducible SERS-active substrates comprised of laser-induced nanoparticle-embedded periodic surface structures (LINEPSS) and metallization of silicon (Si) LINEPSS. LINEPSS were fabricated using the technique of femtosecond laser ablation of Si in acetone. The versatile SERS-active substrates were then achieved by two ways, including the drop casting of silver (Ag)/gold (Au) nanoparticles (NPs) on Si LINEPSS and Ag plating on the Si LINEPSS structures. By controlling the LINEPSS grating periodicity, the effect of plasmonic nanoparticles/plasmonic plating on the Si NPs embedded periodic surface structures enormously improved the SPR strength, resulting in the consistent and superior Raman enhancements. The reproducible SERS signals were achieved by detecting the molecules of Methylene Blue (MB), 2,4-dinitrotoluene (DNT), and 5-amino-3-nitro-l,2,4-triazole (ANTA). The SERS signal strength is determined by the grating periodicity, which, in turn, is determined by the input laser fluence. The SERS-active platform with grating periodicity of 130 ± 10 nm and 150 ± 5 nm exhibited strong Raman enhancements of ∼10(8) for MB and ∼10(7) for ANTA molecules, respectively, and these platforms are demonstrated to be capable, even for multiple usages.