Engineered SERS Substrates with Multiscale Signal Enhancement: Nanoparticle Cluster Arrays

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Abstract
Defined nanoparticle cluster arrays (NCAs) with total lateral dimensions of up to 25.4 μm × 25.4 μm have been fabricated on top of a 10 nm thin gold film using template-guided self-assembly. This approach provides precise control of the structural parameters in the arrays, allowing a systematic variation of the average number of nanoparticles in the clusters (n) and the edge-to-edge separation (Λ) between 1 < n < 20 and 50 nm ≤ Λ ≤ 1000 nm, respectively. Investigations of the Rayleigh scattering spectra and surface-enhanced Raman scattering (SERS) signal intensities as a function of n and Λ reveal direct near-field coupling between the particles within individual clusters, whose strength increases with the cluster size (n) until it saturates at around n = 4. Our analysis shows that strong near-field interactions between individual clusters significantly affect the SERS signal enhancement for edge-to-edge separations Λ < 200 nm. The observed dependencies of the Raman signals on n and Λ indicate that NCAs support a multiscale signal enhancement which originates from simultaneous inter- and intracluster coupling and |E|-field enhancement. The NCAs provide strong and reproducible SERS signals not only from small molecules but also from whole bacterial cells, which enabled a rapid spectral discrimination between three tested bacteria species: Escherichia coli, Bacillus cereus, and Staphylococcus aureus.

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