Third and fifth harmonic generation of an IR (1.064 μm) pulsed laser has been produced in ablation plasmas of the wide bandgap semiconductors CdS and ZnS. The study of the temporal behaviour of the harmonic emission has revealed the presence of distinct compositional populations in these complex plasmas. Species ranging from atoms to nanometre-sized particles have been identified as emitters, and their nonlinear optical properties can be studied separately due to strongly differing temporal behaviour. At short distances from the target (<1 mm), atomic species are mostly responsible for harmonic generation at early times (<500 ns), while clusters and nanoaggregates mostly contribute at longer times (>1 μs). Harmonic generation thus emerges as a powerful and universal technique for ablation plasma diagnosis and as a tool to determine the nonlinear optical susceptibility of ejected clusters or nanoparticles.
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