High-order harmonic generation from C60-rich plasma

We performed systematic investigation of high-order harmonic generation from fullerene-rich laser-produced plasmas. We studied harmonic generation by varying several experimental parameters, such as the delay between the ablation and driving pulses, and divergence and polarization of the pump laser. Enhancement of harmonic yield is observed near 20 eV, which is attributed to the influence of a broadband plasmon resonance of C60 on the nonlinear optical response of fullerene-rich plasma. This increase in the harmonic intensity occurs despite the increased absorption by C60 at these wavelengths. Using simulations based on time-dependent density-functional theory, we confirm that this effect is due to the influence of collective excitations. We compare harmonic generation from fullerenes using lasers with 793 nm and 396 nm wavelengths, which show the influence of plasmon resonance on the conversion efficiency of high-order harmonics for different laser wavelengths.