We report completely sustainable processes and materials for inexpensive and scalable fabrication of plasmonically active solid substrates, which are critical for emerging applications in sensing, catalysis, and metasurfaces. Our approach involves grafting of poly(ethylene glycol) (PEG) onto silicon oxide terminated solid substrates using all-water based processing leading to an ultrathin (12 nm) and smooth (roughness of ∼1 nm) functional layer. The resulting surfaces facilitate robust and

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... tive immobilization of gold nanoparticles (NPs) with a density that is superior to the organic solvent based processing. This new process achieves size dependent assembly of the citrate-stabilized gold NPs resulting in high plasmonic activity in surface-enhanced Raman scattering (SERS). The use of leaf extracts derived from Quercus pubescens as a reducing and stabilizing agent allowed for green synthesis of gold NPs with an average diameter of 25.6 ± 11.1 nm. The assembly of the green synthesized gold NPs on all-water processed PEG grafted layers enabled a fully sustainable route for fabrication of plasmonically active solid substrates. The resulting substrates exhibited high SERS response over the entire (∼1 cm 2 ) substrate surface with an analytical enhancement factor of 9.48 × 10 4 for the probe molecule rhodamine 6G under 532 nm laser excitation. A microfluidic device was also constructed on the fabricated platform for SERS mediated simultaneous detection of two nonsteroidal anti-inflammatory drugs, dexketoprofen and ibuprofen, which are widely used in human medicine and present as contaminants in wastewater. The biocompatibility of PEG together with all-water based processing overcome the need for waste management and ventilation of the working place enabling cost and energy efficient, environmentally benign fabrication of plasmonic devices. (1) Karker, N.; Dharmalingam, G.; Carpenter, M. A. Thermal energy harvesting plasmonic based chemical sensors.