The surface plasmon damping induced by high excitation of the electron gas is studied in femtosecond pump-and-probe experiments on gold colloids embedded in a sol-gel matrix. Optical excitation of single-particle interband transitions leads to a pronounced broadening of the surface plasmon line. A similar behavior is observed for resonant excitation of the surface plasmon. This broadening is the dominant optical nonlinearity of the system, and reflects the excitation-induced damping of the surface plasmon resonance. The time evolution of the damping rate follows that of the electronic scattering rate.

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Abstract. Ag colloid-containing coatings on soda lime glass and fused silica are prepared via the sol-gel process. To incorporate Ag +-ions in the coatings homogeneously, they are stabilized by a functionalised silane (aminosilane) and then mixed with the basic sol prepared from 3-glycidoxypropyl trimethoxysilane (GPTS) and tetraethoxysilane (TEOS). Crack-free and transparent coatings with a thickness of 0.5 to 1.2/zm, are obtained by heat treatment between 120~ and 600~ The Ag-colloid formation was monitored by UV-VIS spectroscopy as a function of temperature. The investigations reveal that the substrate has a deciding influence on the Ag-colloid formation caused by alkali diffusion from the substrate into the coating. High resolution transmission electron microscopy (HRTEM) investigations prove that poly-crystalline AgxOy-nanoparticles are formed during thermal densification in the coatings and that this change is accompanied by a vanishing of the yellow colour of the coatings. A post-heat treatment in a reducing atmosphere (90% N2, 10% Ha) turns back the yellow colour and single-crystalline Agcolloids can be detected by HRTEM. A suitable choice of the temperature and time conditions allows the control of the colloid size during heat treatment in a reducing atmosphere. For comparison, ion-exchange experiments have been carried out which showed that a spontaneous Ag-colloid formation was achieved in the soda lime substrate at 400~ Since Ag containing SiO2-coatings remained colourless after thermal treatment between 400~ and 600~ in air, on soda lime substrates, a remarkable diffusion of Ag + into the substrate was excluded.