Strongly enhanced second-harmonic generation (SHG), which is characterized by a nearly isotropic intensity distribution, is observed for gold-glass films near the percolation threshold. The diffuselike SHG scattering, which can be thought of as nonlinear critical opalescence, is in sharp contrast with highly collimated linear reflection and transmission from these nanostructured semicontinuous metal films. Our observations, which can be explained by giant fluctuations of local nonlinear sources for SHG due to plasmon localization, verify recent predictions of percolation-enhanced nonlinear scattering.
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