Femtosecond pump-probe experiments with a time resolution of 100 fs have been performed for copper particles with a radius of 4 nm. Differential absorption spectra for a pump centered at 2.05 eV indicates the broadening of the absorption band due to the surface plasmon. The nonlinear response time derived from the recovery time of the nonlinear absorption is dependent on the pumping laser fluences, and is as short as 0.7 ps for 210 μJ/cm2. The relaxation dynamics of nonequilibrium electrons can be described by the usual electron-phonon coupling model.
Ultrafast Kerr-type nonlinearities and relaxation dynamics of photoexcited electrons in silver nanocrystals embedded in glass have been investigated by means of femtosecond pump and probe spectroscopy. The transient absorption spectrum induced by the surface plasmon excitation shows a redshift and broadening of the surface plasmon band. The additional broadening is ascribed to the increase of surface plasmon damping and the redshift originates from a change in the real part of the dielectric function of the silver nanocrystals due to nonequilibrium electron heating. The observed redshift yields the nonlinear refractive index n2 of +2.4×10−10 esu and its time response is 1.9 ps.
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