Width of cluster plasmon resonances: Bulk dielectric functions and chemical interface damping

Abstract

The damping of collective electron resonances in clusters which develop into plasmon polaritons at larger sizes is investigated for free, supported, and embedded neutral metal clusters. Embedding of free 2 nm Ag clusters of 2-nm diameter into a ${\mathrm{SiO}}_{2}$ matrix leads to an increase of the width of the resonances by more than a factor of 3. The optical spectra are compared with the Mie theory using size-effect-modified dielectric functions of the solid state. The results corroborate the assumption that the widths of the resonances strongly depend on chemical interface effects. The results are briefly discussed with regard to limited-mean-free-path and quantum-size-effect theories and a recent approach by Persson. It is demonstrated that the widths of the spectra of supported and embedded clusters have to be interpreted with care since true intrinsic size effects of the clusters appear to be less effective than previously believed and can be obscured by the chemical interface damping.