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Development of a coherent ultrafast transmission electron microscope based on a laser-driven cold field emission source

Abstract : The investigation of the physics of nanoscale systems ideally requires atomic spatial resolution and femtosecond time-resolution. Ultrafast Transmission Electron Microscopy (UTEM) combining subpicosecond temporal resolution and nanometer spatial resolution has recently emerged as a unique tool with unprecedented spatio-temporal resolutions. However, the performances of the first UTEMs were limited by the brightness of the photocathodes used as ultrafast electron source. In this context, it was soon realized that UTEMs relying on laser-driven electron sources based on nanoscale emitters would overcome this limitation. The aim of this thesis is to report the development of an ultrafast Transmission Electron Microscope based on a cold field emission source, which can operate either in DC or ultrafast mode. Electron emission from a tungsten nanotip is triggered by femtosecond laser pulses, which are tightly focused by optical components integrated inside a cold-field emission source close to the cathode. The measured brightness is the largest reported so far for UTEMs. Combining this new high brightness source with an injection/Cathodoluminescence system, composed of a parabolic mirror placed above the sample holder, the UTEM can be used to perform time-resolved ultrafast pump-probe TEM experiments. The possibilities of such an instrument for ultrafast imaging, diffraction, electron holography and spectroscopy are presented. Particular attention has been paid on applications in nano-optics. In particular, Electron Energy Gain Spectroscopy (EEGS) allows to investigate the optical excitations of nanosystems in the energy domain. The ability to easily synchronize ultrashort free electron pulses with the optical excitation of the sample in UTEMs is essential for the observation of strongly nonlinear electron/photon interactions. These experiments will enable us to characterize the spectro-temporal properties of the ultrashort electron beam. Off-axis electron holography performed with ultrafast electron pulses are finally discussed. The electron dose in the specimen plane is considerably reduced due to the low repetition rate of the electron pulse train. This peculiar property of ultrafast FE-TEMs implies that ultrafast holograms are acquired in low-dose-like conditions. As a consequence, the experimental parameters commonly used for the acquisition of off-axis electron holograms with conventional TEMs cannot be directly implemented in the ultrafast mode. Experimental studies were performed to find the optimum conditions for ultrafast off-axis electron holography. Influence of the dose, the coherence length of the source, the illumination condition and the instrument instabilities have been addressed.
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Giuseppe Mario Caruso. Development of a coherent ultrafast transmission electron microscope based on a laser-driven cold field emission source. Physics [physics]. Université Paul Sabatier - Toulouse III, 2019. English. ⟨NNT : 2019TOU30140⟩. ⟨tel-02879050⟩



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