Excitation, fragmentation and control of large finite systems: C 60 in moderately strong laser fields

Abstract

Recent progress in the understanding of the primary excitation mechanisms of the C60 fullerene in intense laser pulses is reported. By analyzing mass spectra as a function of pulse duration, laser intensity and time delay between pump- and probe pulse insight into fundamental photoinduced processes such as ionization and fragmentation is obtained. Using ultrashort sub-10fs pulses excitation times are addressed which lie well below the characteristic time scales for electron-electron and electron-phonon coupling. The measured saturation intensities of multiply charged parent ions indicate that for higher charge states the well known C60 giant plasmon resonance is involved in creating ions and a significant amount of large fragments through a non-adiabatic multi-electron dynamics. To enhance the formation of large fragments femtosecond laser pulses tailored with closed-loop, optimal control feedback were used. A characteristic pulse sequence excites oscillations in C60 with large amplitude by coherent heating of nuclear motion. Again, the experimental findings can be understood by a laser-induced multi-electron excitation via the electronically excited resonance followed by efficient coupling to the radial symmetric breathing vibration of C60. © 2008 Springer-Verlag.