Optical chips based on plasmonic bimetal nanoparticles are of particular interest for various applications, including optical sensors, as well as plasmon-enhanced fluorescence and plasmon-enhanced Raman scattering due to their extraordinary optical properties. In the paper, the formation of the bimetallic nanoparticles on the BK7 substrate and tuning of the LSPR wavelengths by irradiation of excimer laser pulses (193 nm output wavelength and 15 ns temporal pulse linewidth) to silver-copper thin films deposited by the physical vapor deposition (PVD) method is studied. Applying four and five ArF laser pulses with the fluence of 140 mJ/cm2 leads to the formation of spherical Ag-Cu nanoparticles and clusters, respectively, with several LSPR peaks in the UV and visible ranges. Also, sharp and intense LSPR peaks in the 560 to 700 nm spectral range are observed in the absorption spectra of the produced samples with four laser pulses which indicates the ability of the method for tuning the LSPR wavelength. Furthermore, the highest enhancement in the Raman scattering of R6G solution is provided using this sample as a substrate for Raman spectroscopy. Therefore, the laser-produced spherical Ag-Cu NPs by these parameters of laser irradiation can be a good candidate for applications based on LSPR, and Raman or fluorescence enhancement.