The long-standing scientific quest of real-time tracing electronic motion and dynamics in all states of matter has been remarkably benefited by the development of intense laser-based pulsed sources with a temporal resolution in the attosecond [1 attosecond = 10⁻¹⁸ s] time scale. Nowadays, attosecond pulses are routinely produced in laboratories by the synthesis of the frequency components of broadband coherent extreme ultraviolet (XUV) radiation generated by the interaction of matter with intense femtosecond (fs) pulses. Attosecond pulse metrology aims at the accurate and complete determination of the temporal and phase characteristics of attosecond pulses and is one of the most innovative challenges in the broad field of ultrashort pulse metrology. For more than two decades since coherent high-brilliance broadband XUV sources have become available, fascinating advances in attosecond pulse metrology have led to the development of remarkable techniques for pulse duration measurements as well as the complete reconstruction of those pulses. Nonetheless, new challenges born from diverse fields call upon for additional efforts and continuously innovative ideas in the field. In this perspective article, we follow the history of ultrashort pulse technology tracing attosecond pulse production and characterization approaches, focus on the operation principles of the most commonly used techniques in the region where they interact with matter, address their limitations, and discuss future prospects as well as endeavors of the field to encounter contemporary scientific progress.

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.

We report the application of the time gated ion microscopy technique in accessing online the position of the source of harmonics generated in atomic gas media. This is achieved by mapping the spatial extreme-ultraviolet (XUV)-intensity distribution of the harmonic source onto a spatial ion distribution, produced in a separate focal volume of the generated XUV beam through single photon ionization of atoms. It is found that the position of the harmonic source depends on the relative position of the harmonic generation gas medium and the focus of the driving infrared (IR) beam. In particular, by translating the gas medium with respect to the IR beam focus different “virtual” source positions are obtained online. Access to such online source positioning allows better control and provides increased possibilities in experiments where selection of electron trajectory is important. The present study gives also access to quantitative information which is connected to the divergence, the coherence properties and the photon flux of the harmonics. Finally, it constitutes a precise direct method for providing complementary experimental info to different attosecond metrology techniques.

We report on high-order harmonic (HHG) two-source interferometry (TSI) in molecular gases. We used a 0-\(\pi\) phase plate to create two bright spots at the focus of a lens by converting a Gaussian laser beam into a TEM please define \(_{01}\) Transverse Electromagnetic Mode. The two bright foci produce two synchronized HHG sources. One of them is used to probe on-going dynamics in the generating medium, while the other serves to heterodyne the signal. The interference of the emissions in the far–field gives access to the phase difference between the two sources. In self–probing HHG phase spectroscopy, one of the two sources is used as a reference while the other one probes some on goin dynamics in the generating medium. We first compute overlap integrals to investigate the mode conversion efficiency. We then establish a clear relation between the laser phase-front curvature and the far-field overlap of the two HHG beams. Both Fresnel diffraction calculations and an experimental lens position scan are used to reveal variations of the phase front inclination in each source. We show that this arrangement offers \(\frac{\lambda_{XUV}}{100}\) precision, enabling extremely sensitive phase measurements. Finally, we use this compact setup for TSI and measure phase variations across the molecular alignment revival of nitrogen and in vibrating sulfur hexafluoride. In both gases, the phase variations change sign around the ionization threshold of the investigated molecule.