Abstract
A second-power yield of resonantly enhanced third harmonic and three-photon luminescence of 744 nm femtosecond laser pump pulses, weakly focused onto a layer of silver nanorolls on a silica substrate, was spectrally detected in the fluence range of 4–20 mJ cm−2, saturating at higher fluences. The third-harmonic yield and its saturation were explored in terms of ultrafast carrier dynamics, based on direct three-photon or cascade one- and two-photon transitions balanced by Auger recombination (and the final band-filling effect) which limited the radiative recombination output in the form of the third harmonic and three-photon luminescence.
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