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AbstractAbstract
[en] Atomic and molecular processes can nowadays be directly followed in the time domain. This is a core technique for a better understanding of the involved fundamental physics, thus auguring new applications in the future as well. Usually the so-called pump-probe technique making use of two synchronized ultrashort light pulses is utilized to obtain this time-resolved data. In this work, the development and characterization of a synchronization system enabling such pump-probe studies at the storage ring PETRA III in combination with an external, then synchronized fs-laser system is described. The synchronization is based on an extended PLL approach with three interconnected feedback loops allowing to monitor short-time losses of the lock and thus prevent them. This way, the jitter between the laser PHAROS and the PETRA III reference signal is reduced to σ <5 ps. Thus the system allows to conduct experiments at a repetition rate of 130 kHz with a temporal resolution limited only by the X-ray pulse length. A major emphasis in the fundamental introductory chapters is an intuitive explanation of the basic principles of phase locked loops and the different aspects of phase noise to allow a deeper understanding of the synchronization. Furthermore, first pump-probe experiments conducted at different beamlines at PETRA III are presented, demonstrating the usability of the laser system in a scientific environment as well. In first characterizing experiments the pulse duration of PETRA III X-ray pulses has been measured to be 90 ps FWHM. In particular, there have been time resolved X-ray absorption spectroscopy experiments on Gaq3 and Znq2 conducted at beamline P11. First results show dynamics of the electronic excitation on the timescale of a few hundred pico seconds up to a few nano seconds and provide a basic understanding for further research on those molecules. For Gaq3 this data is analyzed in detail and compared with visible fluorescence measurements suggesting at least two excited and probed states with different decay constants. Time resolved electron-ion coincidence spectroscopy conducted at P04 shows the flexibility of the system to be usable at different beamlines and to obtain spatial and temporal overlap in vacuum as well.
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Sep 2013; 186 p; ISSN 1435-8085;
; Diss.

Record Type
Report
Literature Type
Thesis/Dissertation
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ABSORPTION SPECTROSCOPY, COINCIDENCE SPECTROMETRY, DE-EXCITATION, ELECTRON SPECTROSCOPY, EXCITED STATES, FEEDBACK, GALLIUM COMPOUNDS, ION SPECTROSCOPY, LASERS, LIFETIME, MOLECULES, OPTICAL PUMPING, ORGANOMETALLIC COMPOUNDS, PETRA STORAGE RING, PULSE TECHNIQUES, SYNCHRONIZATION, TIME DEPENDENCE, TIME RESOLUTION, X-RAY SPECTROSCOPY, ZINC COMPOUNDS
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