We report the observation of multiple ionization of argon through multi-XUV-photon absorption induced by an unprecedentedly powerful laser driven high-order harmonic generation source. Comparing the measured intensity dependence of the yield of the different argon charge states with numerical calculations we can infer the different channels—direct and sequential—underlying the interaction. While such studies were feasible so far only with free electron laser (FEL) sources, this paper connects highly nonlinear XUV processes with the ultrashort time scales inherent to the harmonic pulses and highlights the advanced perspectives of emerging large scale laser research infrastructures.

Real-time observation of ultrafast dynamics in the microcosm is a fundamental approach for understanding the internal evolution of physical, chemical and biological systems. Tools for tracing such dynamics are flashes of light with duration comparable to or shorter than the characteristic evolution times of the system under investigation. While femtosecond (fs) pulses are successfully used to investigate vibrational dynamics in molecular systems, real time observation of electron motion in all states of matter requires temporal resolution in the attosecond (1 attosecond (asec) = 10⁻¹⁸ s) time scale. During the last decades, continuous efforts in ultra-short pulse engineering led to the development of table-top sources which can produce asec pulses. These pulses have been synthesized by using broadband coherent radiation in the extreme ultraviolet (XUV) spectral region generated by the interaction of matter with intense fs pulses. Here, we will review asec pulses generated by the interaction of gas phase media and solid surfaces with intense fs IR laser fields. After a brief overview of the fundamental process underlying the XUV emission form these media, we will review the current technology, specifications and the ongoing developments of such asec sources.

The quantum mechanical motion of electrons and nuclei in systems spatially confined to the molecular dimensions occurs on the sub-femtosecond to the femtosecond timescales respectively. Consequently, the study of ultrafast electronic and, in specific cases, nuclear dynamics requires the availability of light pulses with attosecond (asec) duration and of sufficient intensity to induce two-photon processes, essential for probing the intrinsic system dynamics. The majority of atoms, molecules and solids absorb in the extreme-ultraviolet (XUV) spectral region, in which the synthesis of the required attosecond pulses is feasible. Therefore, the XUV spectral region optimally serves the study of such ultrafast phenomena. Here, we present a detailed review of the first 10-GW class XUV attosecond source based on laser driven high harmonic generation in rare gases. The pulse energy of this source largely exceeds other laser driven attosecond sources and is comparable to the pulse energy of femtosecond Free-Electron-Laser (FEL) XUV sources. The measured pulse duration in the attosecond pulse train is 650 ± 80 asec. The uniqueness of the combined high intensity and short pulse duration of the source is evidenced in non-linear XUV-optics experiments. It further advances the implementation of XUV-pump-XUV-probe experiments and enables the investigation of strong field effects in the XUV spectral region.

The present work reports on the generation of short-pulse coherent extreme ultraviolet radiation of controlled polarization. The proposed strategy is based on high-order harmonics generated in pre-aligned molecules. Field-free molecular alignment produced by a short linearly-polarized infrared laser pulse is used to break the isotropy of a gas medium. Driving the aligned molecules by a circularly-polarized infrared pulse allows to transfer the anisotropy of the medium to the polarization of the generated harmonic light. The ellipticity of the latter is controlled by adjusting the angular distribution of the molecules at the time they interact with the driving pulse. Extreme ultraviolet radiation produced with high degree of ellipticity (close to circular) is demonstrated.

We propose a method for the measurement of attosecond beating structures that result from the superposition of harmonics of laser radiation. It utilizes the phase control of the excitation probability of atoms through different interfering channels. The channels consist of multiphoton excitation by the fundamental frequency and single-photon excitation by the superposition of the harmonic fields, or alternatively, by each harmonic or frequency interval within the bandwidth of each harmonic. The method is sensitive to the relative phase of the harmonics, including phases introduced by chirp, and thus allows evaluation of the temporal structure of the superimposed harmonic fields. An experimental setup for the implementation of the method based on freestanding transmission grating is suggested as well.