Small-particle composites. I. Linear optical properties

Absorption and extinction spectra of fractal and nonfractal small-particle composites are studied. General solutions of the coupled-dipole equations with the exact operator for the dipole interaction (including the near-, intermediate-, and far-zone terms) are found and compared with those in the quasistatic approximation. Broad-scale numerical simulations of optical spectra for clusters containing a large number of particles (up to 10 000) are performed. A significant fraction of dipolar eigenmodes in fractal aggregates is shown to be strongly localized. The eigenmodes cover a wide spectral region providing resonant enhancement in the visible and infrared parts of the spectrum. In contrast to previous predictions, the absorption spectrum is shown to be significantly different from the spectral distribution of the density of dipole eigenmodes. It clearly indicates the importance of symmetry properties of the modes and corresponding selection rules for the absorption by different modes in random fractal composites. Our experimental data obtained for extinction spectra of silver colloid fractal aggregates are in good agreement with the results of numerical simulations.