Photoionization of C60 by 15 ns laser pulses at 193 and 308 nm and by
ca. 100 fs pulses at 310 and 620 nm has been studied with reflectron t
ime-of-flight mass spectrometry. The initial fragmentation process is
seen to be the ejection of C(n), n > 2, as opposed to successive C2 ev
aporation. The fragment ions produced in this initial fragmentation st
ep have sufficient internal energy to cool, by the emission of a C2 mo
lecule in the field-free region of the mass spectrometer. Pump-probe e
xperiments with 90 fs laser pulses at 620 nm give additional insights
into the ionization mechanism.