We demonstrate, for the first time, high-order harmonic generation from C60 by an intense femtosecond Ti:sapphire laser. Laser-produced plasmas from C60-rich epoxy and C60 films were used as the nonlinear media. Harmonics up to the 19th order were observed. The harmonic yield from fullerene-rich plasma is about 25 times larger compared with those produced from a bulk carbon target. Structural studies of plasma debris confirm the presence and integrity of fullerenes within the plasma plume, indicating fullerenes as the source of high-order harmonics.

Abstract. Resonant enhancement of high harmonic generation can be obtained in plasmas containing ions with strong radiative transitions resonant with harmonic orders. The mechanism for this enhancement is still debated. We perform the first temporal characterization of the attosecond emission from a tin plasma under near-resonant conditions for two different resonance detunings. We show that the resonance considerably changes the relative phase of neighboring harmonics. For very small detunings, their phase locking may even be lost, evidencing strong phase distortions in the emission process and a modified attosecond structure. These features are well reproduced by our simulations, allowing their interpretation in terms of the phase of the recombination dipole moment.

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We demonstrate intense high-order harmonic generation from plasma that is created from different carbon targets. We obtain high-order harmonic energy in the multi-microjoule range for each harmonic order from the 11th to the 17th harmonic. By analyzing the target morphology and the plasma composition, we conclude that the intense harmonics from the bulk carbon targets originate from nanoparticles target.

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We present experimental studies of high-order harmonic generation in silver plasma ablation performed with the Ti:sapphire laser beams of the Advanced Laser Light Source ͑800 nm wavelength, 360 mJ total energy͒. We have independently varied the intensity of the prepulse ͑which creates the plasma ablation͒ and the intensity of the main pulse ͑which generates the harmonics͒, and studied their influence on the harmonic spectrum. We show here that the presence of doubly ionized atoms in the ablation, created either by a strong prepulse intensity or with the irradiation of the main pulse, is ineffective for the generation of harmonics.