Ionisation of fullerenes and fullerene clusters using ultrashort laser pulses

Abstract

We give a brief review of the literature concerning the ultra-short pulse ionisation of fullerenes in the gas phase. Emphasis is placed on the excitation time dependence of different ionisation regimes as manifested by photoelectron spectroscopy. The ionisation rates are modelled for the intermediate situation where the excitation energy is equilibrated between electronic degrees of freedom but not yet coupled to vibrational degrees of freedom. The model is shown to describe many aspects of the experiments. New results are presented on the intra-cluster molecular fusion of fullerene molecules when van der Waals bound clusters of fullerenes are exposed to ultra-short laser pulses. Pump-probe measurements give a decay time constant for the intra-cluster fusion reaction of 520 +/- 55 fs. A comparison with monomer ionisation results suggests that the time window for the fusion reaction is influenced by the coupling of the electronic excitation energy to vibrational degrees of freedom of the molecules in the cluster.