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Cluster Dynamics
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des MPI fuer Dynamik und Selbstorganisation |
Photodissociation
and fragmentation of molecules in different cluster environments
(Farnik) Single molecules can be generated, depending
on the production method (adiabatic expansion or pick-up), either
embedded inside or sitting on the surface of a large host cluster.
Experiments have been carried out for HBr molecules and argon
clusters which were dissociated by laser radiation of 193 nm
and 243 nm. The formed H-atoms are detected by multi-photon
ionization in a time-of-flight mass spectrometer and their kinetic
energy is measured as a function of cluster size. In this way the
different dissociation channels as well as their angular
dependence and their branching ratios are determined. The
influence of the cluster environment, e.g. the cage effect,
manifests itself in totally slowed down H-atoms. The systems under
investigation are HBr, HI, and HCl molecules, and small HBr
clusters adsorbed on the surface or embedded in different rare gas
clusters.The cage effect depends critically on the site of the
molecule and on the mass of the cage. In addition, interesting
energy transfer effects in different vibrational states are
observed resulting from collisions of fast H atoms with neighbored
molecules. We observed an unusual behavior for Ne and Xe host
clusters. In the case of Ne, the outer shell turned out to be
liquid. For Xe, the time-of-flight distributions exhibited an
asymmetric behaviour. This is attributed to the formation of HXeI
and HXeCCH. molecules, which were recently observed in
matrices. We detect them by their orientation in coupled weak
electric and strong laser fields and by their subsequent
photodissociation observing the outgoing H atom. In the meantime
the experiments were continued with systems which are
important in atmospheric chemistry solvated in or adsorbed on the
surface of water clusters. First experiments of HCl on ice
particles have already been carried out. HCl dissociates at the
surface of the water clusters and after electronic excitation the
radical H3O is formed. Furthermore pyrrole, imidazol,
and acetylene were investigated. The experimental arrangement has
also been used for measuring the fragmentation probabilities by
electron impact ionization. In this way the heavy rare gases
and methyl lactate as well as pyrrole clusters have
been investigated.
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