Low-threshold lasing and broad-band multiphoton-excited light emission from Ag aggregate-adsorbate complexes in microcavity

A novel class of composites for optics, microcavities doped with metal fractal aggregates, is studied. Lasing and broad-band Stokes and anti-Stokes emission from (Ag colloidal aggregates)/(adsorbed molecules)/(micro-cavity) composite at low-intensity cw and pulse laser excitation has been found. At 633 nm cw excitation wavelength the emission spectrum contains many peaks, spanning a range from wavelength 200 nm to 800 nm. Experiments with pulse excitation of Ag/dye/microcavity composite show that the duration of the observed broad-band anti-Stokes emission significantly exceeds the pump pulse duration, dye molecule fluorescence time, and relaxation times in silver particles. It may be interpreted as a luminescence governed by long-living triplet states of dye molecules. These observations were made possible by use of a fractal-microcavity composite, where coupling the localized plasmon modes in fractal aggregates with microcavity resonances is provided. The important role of multiphoton resonant transitions between discrete states of a finite-size metal particle in enhanced local fields is shown. Analysis, based on the model of a spherical potential well, shows that the observed spectra contain fingerprints of the quantum size effect.