Refractive index and dielectric constant transition of ultra-thin gold from cluster to films

Using high-speed picometrology, the complete cluster-to-film dielectric trajectories of ultra-thin gold films on silica are measured at 488 nm and 532 nm wavelengths for increasing mass-equivalent thickness from 0.2 nm to 10 nm. The trajectories are parametric curves on the complex dielectric plane that consist of three distinct regimes with two turning points. The thinnest regime (0.2 nm-0.6 nm) exhibits increasing dipole density up to the turning point for the real part of the dielectric function at which the clusters begin to acquire metallic character. The mid-thickness regime (0.6 nm~2 nm) shows a linear trajectory approaching the turning point for the imaginary part of the dielectric function. The third regime, from 2 nm to 10 nm, clearly displays the Drude circle, with no observable feature at the geometric percolation transition.