Large area fabrication of metal alloy nanoparticles with tunable surface plasmon resonances, on low cost substrates is reported. A UV excimer laser was used to anneal 5nm thick Ag Au bilayer films deposited with different composition ratios to create alloy nanoparticles. These engineered surfaces are used to investigate how the wavelength of the surface plasmon resonance affects the optical detection capability of chemical species by Surface Enhanced Raman Spectroscopy.Metal nanoparticle films (MNFs) are attracting considerable attention in the fields of Raman biosensors[1, 2], gas sensors [3], solar cells [4,5] and light emitting diodes [6] due to enhancement in light coupling efficiency between the surface plasmons (SP) developed at the nanoparticles and the device.Use of metal alloy nanoparticles can optimize the surface effect of enhanced Raman scattering (SERS) by tuning their plasmon resonance absorption close to the laser frequency used to probe the Raman signal from molecules on their surface [7,8]. However, despite these attractive properties, challenges exist regarding large scale adoptation of plamonic nanoparticle surfaces. One of the major challenges in device fabrication is the production of uniform MNFs over large area substrates and repeatable tune-ability of their surface plasmon resonances (SPR). The maximum energy coupling in SERS coincides with the wavelength of the metal nanoparticles SPR and is localized at "hotspots" [7,9,10].Changes in the SPR optical absorption due to different composition of Ag and Au in alloy nanoparticles has been demonstrated previously [11,12]. The effect is attributed to the change in the dielectric function of the alloy nanoparticles from the volumetric contributions of Ag and Au. Unlike many other fabrication methods, which include chemical synthesis [13], pulsed laser deposition [14], or thermal annealing [15], pulsed laser nanostructuring of thin metal films can be applied over large areas at low cost to fabricate supported nanoparticle surfaces. Henley et al [16] and Trice et al [17] studied the process for single metal films. Herein, we present the synthesis and characterization of metal alloy nanoparticles with tunable SPR by laser nanostructuring of Ag Au bi-layer films and discuss how the position of the maximum absorption affects the SERS efficiencies.Corning glass substrates where cleaned in a ultrasonication bath for 10 min in acetone and blow dried with nitrogen. Metal films were deposited in two layers by evaporating silver and gold separately. The total film thickness was fixed at 5nm while the thickness of each individual layer was deposited according to (AgxAu5-x) where x = 1, 2, 3, 4, 5 in nm. The average deposition rate for all materials was 0.1 -0.2 Å/s and a pressure of 1.0 x 10 -6 Torr was maintained in the evaporation chamber during this process. A Lambda-Physik LPX 210i excimer laser operating at 248 nm, with a pulse duration of 25 ns was used for the rapid annealing. All the samples were mounted on X-Y translation stage moving at a typical ...