PhD Thesis: Ions colliding with molecules and molecular clusters
by
Tao Chen(Stockholm University, Department of Physics)
→
Europe/Stockholm
FD5
FD5
Description
In this work we will discuss fragmentation and molecular growth processes in collisions of Polycyclic Aromatic
Hydrocarbon (PAH) molecules, fullerenes, or their clusters with atoms or atomic ions. Simple collision models as well
as molecular structure calculations are used to aid the interpretations of the present and other experimental results.
Fragmentation features at center-of-mass collision energies around 10 keV are dominated by interactions between the fast
ion/atom and the electron cloud in the molecules/clusters (electronic stopping processes). This electronic excitation energy
is rapidly distributed on the vibrational degrees of freedom of the molecule or of the molecules in a cluster and may result
in fragmentation. Here, the fragmentation is statistical and favors the lowest-energy dissociation channels which are losses
of intact molecules from clusters, H- and C2H2-losses from isolated PAHs, and C2-loss from fullerene monomers. We will
also discuss the possibility of formation of molecular H2 direct from native PAHs which reach high enough energies when
interacting with ions, electrons, or photons.
For the experiments at lower center of mass collision energies (~100 eV) a single atom may be knocked out in close
atom-atom interaction. Such non-statistical fragmentation are due to nuclear stopping processes and gives highly reactive
fragments which may form covalent bonds with other molecules in a cluster on very short time scales (picoseconds). This
process may be important when considering the formation of new species. For collision between 12 keV Ar2+ and clusters
of pyrene (C16H10) molecules, new molecules, e.g. C17H10+, C30H18+, C31H19+, etc are detected. We also observe molecular
fusion processes for He and Ar ions colliding with clusters of C60 molecules. These and related molecular fusion processes
may play a key role for understanding molecular growth processes under certain astrophysical conditions.