Temporal probing of a number of fundamental dynamical processes requires intense pulses at femtosecond or even attosecond (1 as = 10(-18) s) timescales. A frequency 'comb' of extreme-ultraviolet odd harmonics can easily be generated in the interaction of subpicosecond laser pulses with rare gases: if the spectral components within this comb possess an appropriate phase relationship to one another, their Fourier synthesis results in an attosecond pulse train. Laser pulses spanning many optical cycles have been used for the production of such light bunching, but in the limit of few-cycle pulses the same process produces isolated attosecond bursts. If these bursts are intense enough to induce a nonlinear process in a target system, they can be used for subfemtosecond pump-probe studies of ultrafast processes. To date, all methods for the quantitative investigation of attosecond light localization and ultrafast dynamics rely on modelling of the cross-correlation process between the extreme-ultraviolet pulses and the fundamental laser field used in their generation. Here we report the direct determination of the temporal characteristics of pulses in the subfemtosecond regime, by measuring the second-order autocorrelation trace of a train of attosecond pulses. The method exhibits distinct capabilities for the characterization and utilization of attosecond pulses for a host of applications in attoscience.

Ultrafast-dynamics studies and femtosecond-pulse metrology both rely on the nonlinear processes induced solely by an incident light pulse. Extending these approaches to the extreme-ultraviolet (XUV) spectral region would open up a new route to attosecond-scale dynamics. However, this has been hindered by the limited intensities available in coherent XUV continua. In the present work, we realized conditions at which simultaneous ejection of two bound electrons by two-XUVphoton absorption becomes more efficient than their removal one-by-one. In this regime we have succeeded in tracing atomic coherences evolving at the 1-fs scale with simultaneous determination of the average XUV-pulse duration. The rich and dense structure of the autoionizing manifold demonstrates the applicability of the approach to complex systems. This initiates the era of XUV-pump-XUV-probe experiments at the boundary between femto-and attosecond scales.A large variety of ultrafast phenomena, including electronic motion in atoms, molecules, condensed matter and plasmas, dynamic electron-electron correlations, charge migration, ultrafast dissociation and reaction processes, occur on the few-femtosecond to attosecond temporal scale. Attosecond (as) pulses 1 provide access to these temporal regimes in different states of matter [2][3][4][5][6] . Nonlinear (NL) XUV processes constitute the ideal tool for the study of such dynamics. Attosecond pulse trains 7-9 have reached intensities sufficient to induce two-XUV-photon processes [10][11][12][13][14] . However, isolated attosecond pulses, requisite for XUV-pump-XUV-probe experiments, have not yet attained the required parameters for an observable two-XUV-photon process. As a consequence, attosecond pulse metrology and time-domain applications have been widely based on infrared (IR)-XUV cross-correlation approaches, which entail assumptions for the analysis 15 .The present work succeeds for the first time in observing two-XUV-photon processes induced by energetic XUV continua, in part temporally confined in isolated pulses with durations on the order of 1 fs. These processes are in turn exploited in XUVpump-XUV-probe ultrafast evolving atomic coherences, as well as in determining the duration of the XUV bursts. A structured part of the single continuum of the xenon atom is excited by the first pulse, forming an electronic wave packet that undergoes rapid and complex motion before it decays. This evolution can be traced, thanks to the XUV parameters reached, at which a second pulse ejects a second electron before the first one leaves the atom carrying with it all the information on the temporal evolution of the system (coherence decay). Unconventionally, the two electrons leave the atom together and, thus, the doubly ionized Xe yield as a function of the delay between the two pulses carries the fingerprint of the wave packet motion and the XUV pulse duration. As the pulse duration and the decay The intense XUV radiation is generated by frequency upconversion of many-cycle high-peak-power laser fields...

Laser-driven coherent extreme-ultraviolet (XUV) sources provide pulses lasting a few hundred attoseconds 1,2 , enabling real-time access to dynamic changes of the electronic structure of matter 3,4 , the fastest processes outside the atomic nucleus. These pulses, however, are typically rather weak. Exploiting the ultrahigh brilliance of accelerator-based XUV sources 5 and the unique time structure of their laser-based counterparts would open intriguing opportunities in ultrafast X-ray and high-field science, extending powerful nonlinear optical and pump-probe techniques towards X-ray frequencies, and paving the way towards unequalled radiation intensities. Relativistic laser-plasma interactions have been identified as a promising approach to achieve this goal 6-13 . Recent experiments confirmed that relativistically driven overdense plasmas are able to convert infrared laser light into harmonic XUV radiation with unparalleled efficiency, and demonstrated the scalability of the generation technique towards hard X-rays 14-19 . Here we show that the phases of the XUV harmonics emanating from the interaction processes are synchronized, and therefore enable attosecond temporal bunching. Along with the previous findings concerning energy conversion and recent advances in high-power laser technology, our experiment demonstrates the feasibility of confining unprecedented amounts of light energy to within less than one femtosecond.The nonlinear response of matter exposed to intense femtosecond laser pulses gives rise to the emission of highfrequency radiation at harmonics of the laser oscillation frequency. If the harmonics are phase-locked, their superposition results in a train of attosecond bursts 20 . The concept has been so far successfully implemented in atomic gases 21 , and culminated in isolated attosecond pulses by using few-cycle laser drivers 1,2 . The low generation efficiency of harmonic radiation from atoms has motivated research into alternative concepts. Dense, femtosecond-laser-produced plasmas hold promise of converting laser light into coherent harmonics with much higher efficiency and of exploiting much higher laser intensities, because the plasma medium-in contrast to the atomic emitters-imposes no restriction on the strength of the laser field driving the harmonics [6][7][8][9][10][11][12][13] . Recent experimental studies of harmonics produced from overdense plasmas impressively corroborate several theoretical predictions: the high conversion efficiency 19 , the favourable scalability of the generation technique towards high photon energies 14,16,19 and excellent divergence due to the spatial coherence of the generated harmonics 19,22 . Whether the high-order harmonics that are produced in overdense plasmas • gold-coated off-axis parabolic mirror with the same focal length as the laser focusing parabola. The recollimating mirror is mounted on a flipper stage for easy withdrawal, thus enabling the spectral characterization of the emitted XUV light. Thin metal filters (typically 150 nm Al, In or Sn)...

This review presents the technological infrastructure that will be available at the Extreme Light Infrastructure Attosecond Light Pulse Source (ELI-ALPS) international facility. ELI-ALPS will offer to the international scientific community ultrashort pulses in the femtosecond and attosecond domain for time-resolved investigations with unprecedented levels of high quality characteristics. The laser sources and the attosecond beamlines available at the facility will make attosecond technology accessible for scientists lacking access to these novel tools. Time-resolved