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.

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.

Ramsey-like schemes have been recently introduced in combination with high-order laser harmonic sources for high-resolution spectroscopic studies in the extreme ultraviolet (XUV). Here we demonstrate a novel method, combining measurements only in a limited subset of randomly chosen time-sampling intervals, which lead us to perform the first high-resolution XUV spectroscopy of atomic argon with a simple split-pulse setup. Providing an experimentally simple and convenient solution to the problem of performing high-resolution absolute frequency measurements in the XUV, our approach will help paving new roads into this challenging spectral territory.