We use a combination of experimental measurements and density functional theory calculations to show that modification of the band structure of Cu by additions of Al causes an unexpected enhancement of the dielectric properties. The effect is optimized in alloys with Al contents between 10 and 15 at.% and would result in strong localized surface plasmon resonances at suitable wavelengths of light. This result is surprising as, in general, alloying of Cu increases its DC resistivity and would be expected to increase optical loss. The wavelengths for the plasmon resonances in the optimized alloy are significantly blue-shifted relative to those of pure Cu and provide a new material selection option for the range 2.2-2.8 eV.