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Pulses of light that are both ultrashort and ultraintense are often generated using optical parametric amplifiers (OPA). These are capable of driving highly non-linear interactions with matter, which are interesting when studying the fundamental laws of our universe. Furthermore, they are also used in many scientific and industrial applications, such as particle accelerators, inertial-confinement nuclear fusion, and medical diagnostics and treatment. This thesis explores the diagnostic and optimization of pulses of light with extreme properties and utilizes them to drive electron acceleration.

The applied light pulses with very short duration (<5 fs) and high peak power (>10 TW) are sensitive to develop spatio-temporal aberrations. These are color-dependent distortions that can significantly degrade the pulse properties, like peak-intensity, and affect their applicability. Furthermore, in most cases they are not easy to correctly diagnose, with current tools failing to provide widely applicable solutions. In this thesis, we describe a new type of spatio-temporal coupling that is especially relevant for optical parametric synthesizers (OPS), systems that coherently combine multiple OPA stages. To do this, we have contributed to the development of two methods for the characterization of such aberrations, the so-called simplified-INSIGHT and HASO multispectral. These enabled us to further improve the structure of our OPS and laser systems.

We also explored the applicability of light pulses to drive relativistic electron acceleration in vacuum. To this end, an injection system using nanotips is presented, capable of inserting electrons spatially in the focus and temporally in the most intense light-cycle. This way, vacuum laser accelerated electrons of up to 14 MeV were detected using a tight focusing configuration (f#1) and their properties characterized. Furthermore, we investigated the dependence of the acceleration process when the focusing geometry is relaxed (f#3). This resulted in the unexpected outcome of similar electron energies in both cases, although the intensity was ten times reduced. This indicates that the decrease in accelerating field strength is compensated by longer acceleration lengths, which is not predicted by currently existing analytical models.