Non-linear increase and saturation of third-harmonic yield from supported silver nanostructures excited by IR femtosecond laser pulses

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. (letter)