Broadband Coherent X-ray Diffractive Imaging and Developments towards a High Repetition Rate mid-IR Driven keV High Harmonic Source

Abstract : Soft X-ray sources based on high harmonic generation are up to now unique tools to probe dynamics in matter on femto- to attosecond timescales. High harmonic generation is a process in which an intense femtosecond laser pulse is frequency upconverted to the UV and soft X-ray region through a highly nonlinear interaction in a gas. Thanks to their excellent spatial coherence, they can be used for lensless imaging, which has already led to impressive results. To use these sources to the fullest of their potential, a number of challenges needs to be met: their brightness and maximum photon energy need to be increased and the lensless imaging techniques need to be modified to cope with the large bandwidth of these sources. For the latter, a novel approach is presented, in which broadband diffraction patterns are rendered monochromatic through a numerical treatment based solely on the spectrum and the assumption of a spatially non-dispersive sample. This approach is validated through a broadband lensless imaging experiment on a supercontinuum source in the visible, in which a binary sample was properly reconstructed through phase retrieval for a source bandwidth of 11 %. Through simulations, the numerical monochromatization method is shown to work for hard X-rays as well, with a simplified semiconductor lithography mask as sample. A potential application of lithography mask inspection on an inverse Compton scattering source is proposed, although the conclusion of the analysis is that the current source lacks brightness for the proposal to be realistic. Simulations with sufficient brightness show that the sample is well reconstructed up to 10 % spectral bandwidth at 8 keV. In an extension of these simulations, an extended lithography mask sample is reconstructed through ptychography, showing that the monochromatization method can be applied in combination with different lensless imaging techniques. Through two synchrotron experiments an experimental validation with hard X-rays was attempted, of which the resulting diffraction patterns after numerical monochromatization look promising. The phase retrieval process and data treatment however require additional efforts.An important part of the thesis is dedicated to the extension of high harmonic sources to higher photon energies and increased brightness. This exploratory work is performed towards the realization of a compact high harmonic source on a high repetition rate mid-IR OPCPA laser system, which sustains higher average power and longer wavelengths compared to ubiquitous Ti:Sapphire laser systems. High repetition rates are desirable for numerous applications involving the study of rare events. The use of mid-IR wavelengths (3.1 μm in this work) promises extension of the generated photon energies to the kilo-electronvolt level, allowing shorter pulses, covering more X-ray absorption edges and improving the attainable spatial resolution for imaging. However, high repetition rates come with low pulse energies, which constrains the generation process. The generation with longer wavelengths is challenging due to the significantly lower dipole response of the gas. To cope with these challenges a number of experimental configurations is explored theoretically and experimentally: free-focusing in a gas-jet; free-focusing in a gas cell; soliton compression and high harmonic generation combined in a photonic crystal fiber; separated soliton compression in a photonic crystal fiber and high harmonic generation in a gas cell. First results on soliton compression down to 26 fs and lower harmonics up to the seventh order are presented.Together, these results represent a step towards ultrafast lensless X-ray imaging on table-top sources and towards an extension of the capabilities of these sources.
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Julius Huijts. Broadband Coherent X-ray Diffractive Imaging and Developments towards a High Repetition Rate mid-IR Driven keV High Harmonic Source. Optics [physics.optics]. Université Paris-Saclay, 2019. English. ⟨NNT : 2019SACLS154⟩. ⟨tel-02183193⟩

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