Ultrabroadband self-phase-stabilized near-IR pulses have been generated by difference-frequency generation of a filament broadened supercontinuum followed by two-stage optical parametric amplification. Pulses with energy up to $1.2\mathrm{mJ}$ and duration down to $17\mathrm{fs}$ are demonstrated. These characteristics make such a source suited as a driver for high-order harmonic generation and isolated attosecond pulse production.

High-order harmonics were generated in a two-color scheme exploiting an infrared parametric source with self-stabilization of the carrier-envelope phase. A significant cutoff extension was observed with respect to single color, 800 nm driving pulses at comparable peak intensities. Exploiting the wavelength tuning of the parametric source in the $1.5–1.6\mu \text{m}$ range, a continuous xuv spectrum extending from 36 to 70 eV was generated in krypton. A broader xuv continuum, extending beyond 100 eV, was observed in argon. These results represent a step forward in the extension of attosecond science toward the soft x-rays region and open new perspectives in the investigation of quantum effects in atoms and molecules.

We investigated the giant resonance in xenon by high-order harmonic generation spectroscopy driven by a two-color field. The addition of a nonperturbative second harmonic component parallel to the driving field breaks the symmetry between neighboring subcycles resulting in the appearance of spectral caustics at two distinct cutoff energies. By controlling the phase delay between the two color components it is possible to tailor the harmonic emission in order to amplify and isolate the spectral feature of interest. In this Letter we demonstrate how this control scheme can be used to investigate the role of electron correlations that give birth to the giant resonance in xenon. The collective excitations of the giant dipole resonance in xenon combined with the spectral manipulation associated with the two-color driving field allow us to see features that are normally not accessible and to obtain a good agreement between the experimental results and the theoretical predictions.

Over the last few decades, the investigation of ultrafast phenomena occurring in atoms, molecules and solid-state systems under a strong-field regime of light-matter interaction has attracted great attention. The increasing request for a suitable optical technology is significantly boosting the development of powerful ultrafast laser sources. In this framework, Optical Parametric Amplification (OPA) is currently becoming a leading solution for applications in high-power ultra-broadband light burst generation. The main advantage provided by the OPA scheme consists of the possibility of exploring spectral ranges that are inaccessible by other laser technologies, as the InfraRed (IR) window. In this paper, we will give an overview on recent progress in the development of high-power few-optical-cycle parametric amplifiers in the near-IR and in the mid-IR spectral domain. In particular, the design of the most advanced OPA implementations is provided, containing a discussion on the key technical aspects. In addition, a review on their application to the study of strong-field ultrafast physical processes is reported.

The light-induced ultrafast switching between molecular isomers norbornadiene and quadricyclane can reversibly store and release a substantial amount of chemical energy. Prior work observed signatures of ultrafast molecular dynamics in both isomers upon ultraviolet excitation but could not follow the electronic relaxation all the way back to the ground state experimentally. Here we study the electronic relaxation of quadricyclane after exciting in the ultraviolet (201 nanometres) using time-resolved gas-phase extreme ultraviolet photoelectron spectroscopy combined with non-adiabatic molecular dynamics simulations. We identify two competing pathways by which electronically excited quadricyclane molecules relax to the electronic ground state. The fast pathway (<100 femtoseconds) is distinguished by effective coupling to valence electronic states, while the slow pathway involves initial motions across Rydberg states and takes several hundred femtoseconds. Both pathways facilitate interconversion between the two isomers, albeit on different timescales, and we predict that the branching ratio of norbornadiene/quadricyclane products immediately after returning to the electronic ground state is approximately 3:2.