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Herrwerth, Oliver (2011): Atomic and molecular ionization dynamics in strong IR and XUV fields probed by time-resolved coincidence spectroscopy. Dissertation, LMU München: Fakultät für Physik



In the work for this thesis, a split-mirror-setup was designed and build, which was used to split the XUV laser-pulse of FELs (Free Electron Laser) into two identical pulses from which one can be delayed. With this setup the laser pulses of FLASH, Hamburg and SCSS, Harima(Japan) where characterized temporally, to determine the temporal pulse-structure for subsequent experiments. The intermolecular dynamics of the homonuclear diatomic molecules nitrogen and oxygen were examined and the experimental results were reproduced by classical simulations. In the measurement with oxygen for an energy band of the coincident singly charged ions, an ionization probability was found that depends on the delay between the two XUV-pulses. This can most probably be explained by the autoionization of an excited singly charged molecular state. Subsequently the investigation of the two photon double ionization (TPDI) of deuterium is presented. In the single pulse experiments simulations within the Born-Oppenheimer approximation made it possible to distinguish between the direct and sequential TPDI. In the pump-probe experiments light was shed onto the dynamics of the TPDI. In addition, experiments with strong few-cycle near-infrared (NIR) pulses are presented that examined the carrier envelope phase (CEP) dependence of the non-sequential double ionization of argon. Implementing single-shot CEP-tagging in conjunction with coincidence spectroscopy allowed to achieve unprecedented accuracy in measuring correlated electron dynamics.