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Abstract

Within this thesis, a new experimental setup has been developed to investigate the quantum
dynamics of molecular ions and charged clusters. An Electrostatic Ion Beam Trap (EIBT) stores
a fast target beam at keV energies in oscillatory motion. By crossing it with a projectile beam, e.g.
an IR laser, molecular reactions can be induced. We implemented a Reaction Microscope (REMI)
in the field-free region of the EIBT to perform coincidence spectroscopy on the resulting reaction
products. In contrast to prior experiments, this unique combination of techniques allows to measure
the 3D momentum vectors of ions, electrons and neutrals as reaction products in coincidence.
At the same time, the EIBT allows for advanced target preparation techniques, e.g. relaxation of
hot molecules during storage times up to seconds, autoresonance cooling and recycling of target
species which are difficult to prepare. The TrapREMI setup can be connected to a variety of
projectile sources, e.g. atomic gas jets, large-scale radiation facilities and ultrashort laser pulses
which enable even time-resolved studies. Here, we describe the setup development and first,
IR-induced photodissociation experiments on O⁺
₂ and CH⁺
₄, providing a proof-of-principle for
ion-neutral coincidence detection in the TrapREMI.