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Nonlinear light-matter interactions in the extreme ultraviolet (XUV) are a prerequisite to perform XUV-pump/XUV-probe spectroscopy of core electrons. Such interactions are now routinely investigated at free-electron laser (FEL) facilities. Yet, electron dynamics are often too fast to be captured with the femtosecond resolution of state-of-the-art FELs. Attosecond pulses from laser-driven XUV-sources offer the necessary temporal resolution. However, intense attosecond pulses supporting nonlinear processes have only been available for photon energy below 50 eV, precluding XUV-pump/XUV-probe investigation of typical inner-shell processes. Here, we surpass this limitation by demonstrating two-photon absorption from inner electronic shells of xenon at photon energies around 93 eV and 115 eV. This advance opens the door for attosecond real-time observation of nonlinear electron dynamics deep inside atoms.

We demonstrate multiphoton ionization of inner-shell electrons in Xenon with 100-eV attosecond pulses. This was achieved with a novel XUV source based on high-harmonic generation in the gas phase driven with multi-TW few-cycle laser pulses.

Vacuum laser acceleration (VLA) is a paradigm that utilizes the strong fields of focused laser light to accelerate electrons in vacuum. Despite its conceptual simplicity and a large existing collection of theoretical studies, realizing VLA in practice has proven remarkably challenging due to the difficulties associated with efficient injection: the electrons to be accelerated must be pre-energized and temporally compressed below an optical half-cycle before timely entering the rapidly oscillating fields of the laser. Therefore, only a handful of experiments have been published up to date, and a knowledge gap remains [1-3].

Acceleration of electrons in vacuum directly by intense laser fields holds great promise for the generation of high-charge, ultrashort, relativistic electron bunches. While the energy gain is expected to be higher with tighter focusing, this does not account for the reduced acceleration range, which is limited by diffraction. Here, we present the results of an experimental investigation that exposed nanotips to relativistic few-cycle laser pulses. We demonstrate the vacuum laser acceleration of electron beams with 100s pC charge and 15 MeV energy. Two different focusing geometries, with normalized vector potential a0 of 9.8 and 3.8, produced comparable overall charge and electron spectra, despite a factor of almost ten difference in peak intensity. Our results are in good agreement with 3D particle-in-cell simulations, which indicate the importance of dephasing.

Optical parametric amplification (OPA) is a powerful tool for the generation of ultrashort light pulses. However, under certain circumstances, it develops spatio-spectral couplings, color dependent aberrations that degrade the pulse properties. In this work, we present a spatio-spectral coupling generated by a non-collimated pump beam and resulting in the change of direction of the amplified signal with respect to the input seed. We experimentally characterize the effect, introduce a theoretical model to explain it as well as reproduce it through numerical simulations. It affects high-gain non-collinear OPA configurations and becomes especially relevant in sequential optical parametric synthesizers. In collinear configuration, however, beyond the direction change, also angular and spatial chirp is produced. We obtain with a synthesizer about 40% decrease in peak intensity in the experiments and local elongation of the pulse duration by more than 25% within the spatial full width at half maximum at the focus. Finally, we present strategies to correct or mitigate the coupling and demonstrate them in two different systems. Our work is important for the development of OPA-based systems as well as few-cycle sequential synthesizers.

We report on the detection of spatio-temporal couplings in a 700-1000 nm NOPA using an optimized characterization method. The technique is performed during normal focus observation and requires little additional hardware.

Optical parametric chirped-pulse amplification (OPCPA) [1] is an established light amplification technique with many beneficial properties, like high single pass gain, scalability, large spectral bandwidth, tunability and good conversion efficiency. Different methods have been proposed for optimization of conversion [2] - [4] mainly altering the pump or the crystal properties. However, seed manipulation to increase the OPCPA conversion efficiency has been only described in a general spatiotemporal field optimization theory so far [5]. Here, we show numerical and experimental results of a novel method to improve the gain saturation in an ultra-broadband OPCPA, hence conversion efficiency, by applying an adaptive spectral filter function to the seed pulses.

Optical parametric chirped-pulse amplification (OPCPA) is a light amplification technique that provides the combination of broad spectral gain bandwidth and large energy, directly supporting few-cycle pulses with multi-terawatt (TW) peak powers. Saturation in an OPCPA increases the stability and conversion efficiency of the system. However, distinct spectral components experience different gain and do not saturate under the same conditions, which reduces performance. Here, we describe a simple and robust approach to control the saturation for all spectral components. The demonstrated optimal saturation increases the overall gain, conversion efficiency and spectral bandwidth. We experimentally obtain an improvement of the pulse energy by more than 18%. This technique is easily implemented in any existing OPCPA system with a pulse shaper to maximize its output.

We report on details of a peak-power upgrade of a sub-5-fs Optical Parametric Synthesizer towards 100TW. System design, pump pulse delaying and relay imaging system arepresented. A tailored second and third harmonic generation reaches conversion efficiencies of 80% and 60% with 80ps pump pulses.

Non-linear interactions between light and matter have nowadays a broad range of applications. They are used for frequency doubling in simple laser pointers as well as for a variety of purposes in complex laser systems like the one presented in this thesis. For the study of ultrafast phenomena, those non-linear interactions are crucial to trigger and observe events at the fastest timescale, which is currently the attosecond regime (10^-15 – 10^-18 s). As the duration of a single optical cycle of a visible light wave is longer than this timescale, these investigations necessitate the application of XUV and X-ray pulses. However, the generation of isolated attosecond light pulses sufficiently intense to initiate non-linear interactions with matter is restricted to photon energies below 50 eV. The aim of this thesis is to establish a new light source, which pushes this boundary further and thereby enables the observation of up to now unrevealed electron dynamics.

The presented new light source provides attosecond pulses with approximately hundred times more pulse energy than typical systems (up to 55 nJ in the spectral range from approximately 65 eV to 140 eV). This facilitates non-linear measurements at these photon energies. The achieved high energy stability (5 %) of this light source allows precise and time efficient measurements. These parameters are obtained via energy-upscaling of high-harmonic generation in gas medium. For the generation of well isolated attosecond pulses a unique laser, like the Light Wave Synthesizer 20, is necessary. This laser uses optical parametric synthesis to produce the most intense sub-5 fs, sub two-cycle laser pulses in the world (80 mJ, 4.5 fs).

Furthermore, an optimal focus of the XUV pulses is crucial to provide the necessary intensity for non-linear interactions. Therefore, different methods for focusing the XUV pulses are investigated. Moreover, the construction and characterization of a robust split and delay stage is presented, which is essential for time resolved measurements.

The detection of the non-linear interaction is realized via a spatially resolved ion time-of-flight detector, the ion microscope. This allows for a quantitative measurement of different ionization states. With the combination of this detector and the new light source the non-linear generation of Xe⁴⁺ and Xe⁵⁺ at photon energies around 100 eV is demonstrated. This enables the determination of the two-photon ionization cross-sections, which could up to now only be measured with much longer pulses at large scientific infrastructures. This paves the way towards time-resolved XUV pump – XUV probe measurements at 100 eV.

The Fourier-transform limit achieved by a linear spectral phase is the typical optimum by the generation of ultrashort light pulses. It provides the highest possible intensity, however, not the shortest full width at half maximum of the pulse duration, which is relevant for many experiments. The approach for achieving shorter pulses than the original Fourier limit is termed temporal superresolution. We demonstrate this approach by shaping the spectral phase of light from an optical parametric chirped pulse amplifier and generate sub-Fourier limited pulses. We also realize it in a simpler way by controlling only the amplitude of the spectrum, producing a shorter Fourier-limited duration. Furthermore, we apply this technique to an optical parametric synthesizer and generate multi-TW sub-4-fs light pulses. This light source is a promising tool for generating intense and isolated attosecond light and electron pulses.

For many applications of extreme ultraviolet (XUV) and X-ray pulses, a small focus size is crucial to reach the required intensity or spatial resolution. In this article, we present a simple way to characterize an XUV focus with a resolution of 1.85 µm. Furthermore, this technique was applied for the measurement and optimization of the focus of an ellipsoidal mirror for photon energies ranging from 18 to 150 eV generated by high-order harmonics. We envisage a broad range of applications of this approach with sub-micrometer resolution from high-harmonic sources via synchrotrons to free-electron lasers.

The spectral phase and amplitude of a multi-TW laser with a Fourier transform limit of 4.6 fs was optimized to obtain 3.9 fs pulses with >5TW, providing the most energetic sub-4-fs pulses in the world.

When a pulsed, few-cycle electromagnetic wave is focused by optics with f-number smaller than two, the frequency components it contains are focused to different regions of space, building up a complex electromagnetic field structure. Accurate numerical computation of this structure is essential for many applications such as the analysis, diagnostics, and control of high-intensity laser-matter interactions. However, straightforward use of finite-difference methods can impose unacceptably high demands on computational resources, owing to the necessity of resolving far-field and near-field zones at sufficiently high resolution to overcome numerical dispersion effects. Here, we present a procedure for fast computation of tight focusing by mapping a spherically curved far-field region to periodic space, where the field can be advanced by a dispersion-free spectral solver. In many cases of interest, the mapping reduces both run time and memory requirements by a factor of order 10, making it possible to carry out simulations on a desktop machine or a single node of a supercomputer. We provide an open-source C++ implementation with Python bindings and demonstrate its use for a desktop machine, where the routine provides the opportunity to use the resolution sufficient for handling the pulses with spectra spanning over several octaves. The described approach can facilitate the stability analysis of theoretical proposals, the studies based on statistical inferences, as well as the overall development and analysis of experiments with tightly-focused short laser pulses.

Temporal-intensity contrast is crucial in intense laser-matter interaction to circumvent the undesirable expansion of steep high-density plasma prior to the interaction with the main pulse. Nonlinear elliptical polarization rotation in an argon filled hollow-core fiber is used here for cleaning pedestals/satellite pulses of a chirped-pulse-amplifier based Ti: Sapphire laser. This source provides similar to 35 mu J energy and sub-4-fs duration, and the process has >50% internal efficiency, more than the most commonly used pulse cleaning methods. Further, the contrast is improved by 3 orders of magnitude when measured after amplifying the pulses to 16 TW using non-collinear optical parametric chirped pulse amplification with a prospect to even further enhancement.

Temporal filtering and spectral broadening are simultaneously achieved, allowing the compression of 20 fs laser pulses down to sub-4 fs duration through the method of nonlinear elliptical polarization rotation in an argon filled hollow-core fiber. The sub-4 fs source provides ~ 35-µJ energy with an internal efficiency >50%, which is more than from the most commonly used pulse-cleaning methods. Further, the contrast is improved by 3 orders of magnitude when measured after amplifying the pulses to 16 TW using non-collinear optical parametric chirped pulse amplification with a prospect to even further enhancement.

We investigate the temporal contrast of the Light Wave Synthesizer 20 (LWS-20): a powerful, few-cycle source based on the optical parametric synthesizer principle. Saturation effects in the RF amplifier driving the acousto-optic programmable dispersive filter (AOPDF) were found to degrade the coherent contrast for non-monotonic group delay corrections. We subsequently present a new dispersion scheme and design a novel transmission grism-based stretcher optimized for LWS-20. The resulting temporal contrast of the amplified, compressed output pulses is improved by 2-4 orders of magnitude compared to the former design.

The development of ultra-short intense laser sources in the visible and extreme ultraviolet (XUV) spectral range has led to fascinating studies in laser-matter interactions and attosecond science. In the majority of these studies, the system under investigation interacts with a focused light beam, which ionizes the system. The ionization products are usually measured by devices, which spatiotemporally integrate the ionization signal originating from the entire focal area, discarding in this way valuable information about the ionization dynamics that take place in the interaction volume. Here, we review a recently developed approach in measuring the spatially resolved photoionization yields resulting from the interaction of infrared (IR)/XUV ultra-short light pulses in gas phase media. We show how this approach enables (a) the in situ focus diagnostic, (b) quantitative studies of linear and non-linear ionization processes in the IR/XUV regime, (c) single-shot XUV-pump-XUV-probe studies and (d) single-shot 2nd-order XUV autocorrelation measurements.