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Wafer-scale surface-enhanced Raman scattering (SERS) substrates fabricated using maskless lithography are important for scalable production targets. Large-area, leaning silver-capped silicon nanopillar (Ag NP) structures suitable for SERS molecular detection at extremely low analyte concentrations are investigated. Theoretical results show that isolated Ag NPs essentially support two localized surface plasmon (LSP) modes. The most prominent LSP resonance is observed in the near-infrared region (∼800 nm) and can be tuned by changing the diameter of the silicon nanopillars (Si NPs). The corresponding electric field distribution maps indicate that the maximum E-field enhancement is found at the Ag cavity, i.e., the bottom part of the Ag cap. We argue that the plasmon coupling between the resonant Ag cap cavities contributes most to the enhancement of the Raman signal. We experimentally evaluate these findings and show that by exposing Si NPs to an O2-plasma the average Ag NP cluster size, and thus the overal...

Wafer-Scale Leaning Silver Nanopillars for Molecular Detection at Ultra-Low Concentrations