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The contributions of localized surface plasmon resonance (LSPR) and Drude (free electrons) absorption to the complex dielectric function of ultrathin Au films were investigated with spectroscopic ellipsometry. When the Au film thickness is thinner than ~10 nm, Au nanoparticles (NPs) are formed as a result of the discontinuity in the films, leading to the emergence of LSPR of Au NPs; and the LSPR exhibits a splitting when the films thinner than ~8 nm, which could be attributed to the near-field coupling of the Au NPs and/or the inhomogeneous polarizations of the Au NPs. On the other hand, the delocalization of electrons in Au NPs due to the aggregation of Au NPs in a thicker film leads to an increase in the free-electron absorption and a suppression of the LSPR.

Influence of localized surface plasmon resonance and free electrons on the optical properties of ultrathin Au films: a study of the aggregation effect