Large third-order optical nonlinearity in Au:SiO2 composite films near the percolation threshold

Very large third-order optical nonlinearity, χ(3)∼2.5×10−6 esu, measured by a degenerate four wave mixing method using a short pulse (70 picosecond) laser, has been found in the rapid-thermal annealed Au:SiO2 composite films at concentrations below the Au percolation threshold. The dependence of the χ(3) on Au concentration, p, follows a cubic power law. The maximum figure of merit, χ(3)/α (with α being the absorption coefficient) is about 10−11 esu cm. We explain this result as due to local field enhancement arising from the Mie resonance of the Au nanoclusters, with strong interaction between the nanoclusters further promoting the effect.