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| Report/Dissertation / PhD Thesis | DESY-2014-02322 |
2014
Report No.: DESY-THESIS-2014-005
Abstract: This thesis reports on the development and application of two different but complementary ultrafast electron diffraction setups built at the Max Planck Research Department for Structural Dynamics. One is an ultra-compact femtosecond electron diffraction (FED) setup (Egun300), which is currently operational (with a maximum electron energy of 150 keV) and provides ultrashort (~300 fs) and bright (~10 e/um^(2)) electron bunches. The other one, named as Relativistic Electron Gun for Atomic Exploration (REGAE) is a radio frequency driven 2 to 5 MeV FED setup built in collaboration with different groups from DESY. REGAE was developed as a facility that will provide high quality diffraction with sufficient coherence to even address structural protein dynamics and with electron pulses as short as 20 fs (FWHM). As one of the first students in Prof. R.J. Dwayne Miller’s group, I led the femtosecond (fs) laser sub-group at REGAE being responsible for the construction of different key optical elements required to drive both of aforementioned FED systems. A third harmonic generation (THG) and a nonlinear optical parametric amplifier (NOPA) have been used for the photo-generation of ultrashort electron bursts as well as sample laser excitation. Different diagnostic tools have been constructed to monitor the performance of the fs optical system. A fast autocorrelator was developed to provide on the fly pulse duration correction. A transient-grating frequency-resolved optical gating (TG-FROG) was built to obtain detail information about the characteristics of fs optical pulse, i.e. phase and amplitude of its spectral components. In addition to these optical setups, I developed a fs optical pump-probe system, which supports broadband probe pulses. This setup was successfully applied to investigate the semiconductor-to-metal photoinduced phase transition in vanadium dioxide and the ultrafast photo-reduction mechanism of graphene oxide.In regard to FED setups, I have been deeply involved in their development. I performed the first study in our compact FED system. I studied the optical and structural response of alkali halides to intense UV excitation conditions, i.e. above the damage threshold of the samples which required the application of a single-shot scheme. In order to gain a better understanding of the ablation process that follows fs optical excitation in alkali halides, I applied a variety of different techniques. Optical reflectivity, femtosecond electron diffraction, ion detection and crater measurements revealed the existence of a cold ablation process that occurs well below the threshold for plasma formation and even that for the melting point of the salts. This atypical cold explosion owes to the presence of highly localized excitonic states and reflects the repulsive nature of initial electronic correlations at play.In the case of REGAE, we performed the first time-resolved experiment following the fs laser heating dynamics and partial melting of polycrystalline gold films. This experiment was crucial to test the overall synchronization of our REGAE machine. We were able to observe a clear dynamics under single-shot photo-excitation conditions and found time zero within 1 picosecond. Further electron pulse characterization will involve the implementation of ponderomotive scattering. I have already constructed the required modular setup and performed all preliminary ASTRA N-body simulations.
Keyword(s): Dissertation
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