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•The Langmuir–Blodgett technique offers a two-degree control for nanoparticle layers.•Tunable plasmonic substrates can be easily obtained with gold nanoparticle monolayers.•Optimizing the lateral packing or hotspot size reveals a resonance in SERS intensity.
Nanoparticle self-assembly is a robust and versatile strategy for the development of functional nanostructured materials, offering low-cost and scalable methods that can be fine-tuned for many different specific application. In this work, we demonstrate a pathway for the fabrication of tailorable quasi-two-dimensional lattices of gold nanoparticles to be used in Surface Enhanced Raman Scattering (SERS) detection of biomolecules. As a first step, nanoparticles are spread as a monolayer at the water/air interface, compressed to a target lateral density in a Langmuir–Blodgett technique, and transferred to a properly functionalized substrate surface. Once firmly adhered to the substrate, the lattice of nanoparticles can be directly used or be further processed using electroless gold deposition to let the nanoparticle grow thus tuning the plasmonic response and SERS enhancement. Compared to direct deposition or self-assembly methods, our protocol enables to obtain consistent results and much higher coverage of Au nanoparticles thanks to the active control of the surface pressure of the spread monolayer.