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Gliserin, Alexander (2014): Towards attosecond 4D imaging of atomic-scale dynamics by single-electron diffraction. Dissertation, LMU München: Faculty of Physics



Many physical and chemical processes which define our daily life take place on atomic scales in space and time. Time-resolved electron diffraction is an excellent tool for investigation of atomic-scale structural dynamics (4D imaging) due to the short de Broglie wavelength of fast electrons. This requires electron pulses with durations on the order of femtoseconds or below. Challenges arise from Coulomb repulsion and dispersion of non-relativistic electron wave packets in vacuum, which currently limits the temporal resolution of diffraction experiments to some hundreds of femtoseconds. In order to eventually advance the temporal resolution of electron diffraction into the few-femtosecond range or below, four new concepts are investigated and combined in this work: First, Coulomb repulsion is avoided by using only a single electron per pulse, which does not repel itself but interferes with itself when being diffracted from atoms. Secondly, dispersion control for electron pulses is implemented with time-dependent electric fields at microwave frequencies, compressing the duration of single-electron pulses at the expense of simultaneous energy broadening. Thirdly, a microwave signal used for electron pulse compression is derived from an ultrashort laser pulse train. Optical enhancement allows a temporal synchronization between the microwave field and the laser pulses with a precision below one femtosecond. Fourthly, a cross-correlation between laser and electron pulses is measured in this work with the purpose of determining the possible temporal resolution of diffraction experiments employing compressed single-electron pulses. This novel characterization method uses the principles of a streak camera with optical fields and potentially offers attosecond temporal resolution. These four concepts show a clear path towards improving the temporal resolution of electron diffraction into the few-femtosecond domain or below, which opens the possibility of observing electron densities in motion. In this work, a compressed electron pulse's duration of 28±5 fs full width at half maximum (12±2 fs standard deviation) at a de Broglie wavelength of 0.08 Å is achieved. Currently, this constitutes the shortest electron pulses suitable for diffraction, about sixfold shorter than in previous work. Ultrafast electron diffraction now meets the requirements for investigating the fastest primary processes in molecules and solids with atomic resolution in space and time.