Journal of Chemical Physics, Vol.120, No.3, 1572-1584, 2004
The dynamics of endohedral complex formation in surface pick-up scattering as probed by kinetic energy distributions: Experiment and model calculation for Cs@C-60(+)
Endohedral Cs@C-60 molecules were formed by implanting low energy (E-0=30-220 eV) Cs+ ions into C-60 molecules adsorbed on gold. Both growth and etching experiments of the surface deposited C-60 layer provide clear evidence for a submonolayer coverage. The Cs+ penetration and Cs@C-60 ejection stages are shown to be a combined, single collision event. Thermal desorption measurements did not reveal any Cs@C-60 left on the surface following the Cs+ impact. The Cs@C-60 formation/ejection event therefore constitutes a unique example of a pick-up scattering by endocomplex formation. Kinetic energy distributions (KEDs) of the outgoing Cs@C-60(+) were measured for two different Cs+ impact energies under field-free conditions. The most striking observation is the near independence of the KEDs on the Cs+ impact energy. Both KEDs peak around 1.2 eV with similar line shapes. A simple model for the formation/ejection/fragmentation dynamics of the endohedral complex is proposed. The model leads to a strong correlation between the vibrational and kinetic energy of the outgoing Cs@C-60. The KEDs are calculated taking into account the competition between the various decay processes: fragmentation and delayed ionization of the neutral Cs@C-60 emitted from the surface, fragmentation of the Cs@C-60(+) ion, and radiative cooling. It is concluded that the measured KEDs are heavily biased by the experimental breakdown function. Good agreement between experimental and calculated KEDs is obtained. (C) 2004 American Institute of Physics.