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Achieving reliable and quantifiable performance in large-areasurface-enhanced Raman spectroscopy (SERS) substrates has long been aformidable challenge. It requires substantial signal enhancement whilemaintaining a reproducible and uniform response. Conventional SERS substratesare typically made of inhomogeneous materials with random resonator geometriesand distributions. As a result, they exhibit several or broadened plasmonicresonances, undesired absorptive losses, and inhomogeneous field enhancement.These limitations diminish the signal strength and hamper reproducibility,making it difficult to conduct comparative studies with high sensitivity. Inthis study, we propose an approach that utilizes monocrystalline gold flakes tofabricate well-defined gratings composed of plasmonic double-wire resonators,which are fabricated through focused ion-beam lithography. The geometry of thedouble wire grating substrate (DWGS) was evolutionary optimized to achieveefficient enhancement for both excitation and emission processes. The use ofmonocrystalline material minimizes absorption losses while enhancing the shapefidelity during the nanofabrication process. The DWGS shows notablereproducibility (RSD=6.6%), repeatability (RSD=5.6%), and large-areahomogeneity over areas $>10^4\,\mu$m$^2$. Moreover, it provides a SERSenhancement factor of $\approx 10^6$ for 4-Aminothiophenol (4-ATP) analyte anddetection capability for sub-monolayer coverage. The DWGS demonstratesreusability, as well as long-term stability on the shelf. Experimentalvalidation with various analytes, in different states of matter, includingbiological macromolecules, confirms the sensitive and reproducible nature ofDWGSs, thereby establishing them as a promising SERS substrate design forfuture sensing applications.

Evolutionary Optimized, Monocrystalline Gold Double Wire Gratings as a SERS Sensing Platform