High-order harmonic generation has become a standard technique for producing attosecond extreme ultraviolet (XUV) pulses in the laboratory, yet the high flux necessary for nonlinear XUV photoionization remains accessible to only a few research groups. Here, we introduce the SYLOS Compact high-harmonic beamline at the Extreme Light Infrastructure Attosecond Light Pulse Source, specifically designed to provide the flux required for nonlinear optics in the XUV. We present a detailed characterization of the beam line demonstrating its capability to generate and utilize both intense attosecond pulse trains and isolated attosecond pulses. We further showcase the 2-XUV–photon double ionization of neon (Ne) and argon (Ar), achieved in a user campaign. The results underscore the beamline’s capability to support cutting-edge attosecond experiments and investigations of ultrafast electron dynamics on the attosecond scale.

Semiconductor crystals driven by strong mid-infrared pulses offer advantages for studying many-body physics and ultrafast optoelectronics via high-harmonic generation. While the process has been used to study solids in the presence strong mid-infrared fields, its potential as an attosecond light source is largely underexplored. We demonstrate that high-harmonics emitted from zinc-oxide crystals produce attosecond pulses, measured through spectroscopy of alkali metals. Using a cross-correlation approach, we photoionize Cesium atoms with vacuum-ultraviolet high-harmonics in the presence of a mid-infrared laser field. We observe oscillations in the photoelectron yield, originating from the instantaneous polarization of atoms by the laser field. The phase of these oscillations encodes the attosecond synchronization of the high-harmonics and is used for attosecond pulse metrology. This source opens new spectral windows for attosecond spectroscopy, enabling studies of bound-state dynamics in natural systems with low ionization energies, while facilitating the generation of non-classical entangled light states in the visible-VUV.

Strongly laser-driven semiconductor crystals offer substantial advantages for the study of many-body physics and ultrafast optoelectronics via the high harmonic generation process. While this phenomenon has been employed to investigate the dynamics of solids in the presence of strong laser fields, its potential to be utilized as an attosecond light source has remained unexploited. Here, we demonstrate that the high harmonics generated through the interaction of mid–infrared pulses with a ZnO crystal leads to the production of attosecond pulses, that can be used to trace the ultrafast ionization dynamics of alkali metals. In a cross–correlation approach, we photoionize Cesium atoms with the vacuum-ultraviolet (VUV) high-harmonics in the presence of a mid-infrared laser field. We observe strong oscillations of the photoelectron yield originating from the instantaneous polarization of the atoms by the laser field. The phase of the oscillations encodes the attosecond synchronization of the ionizing high-harmonics and is used for attosecond pulse metrology. This light source opens a new spectral window for attosecond spectroscopy, paving the way for studies of systems with low ionization potentials including neutral atoms, molecules and solids. Additionally, our results highlight the significance of the source for generating non–classical massively entangled light states in the visible–VUV spectral region.

In recent years laser driven attosecond sources based on loose geometry high order harmonic generation reach focused intensities as high as to induce multi-photon multiple ionization or even strong-field effects in the extreme ultraviolet spectral range. In this chapter, we review four such sources developed through collaborative efforts between FORTH, ELI-ALPS and the University of Lund together with recent results obtained in the above mentioned topics utilizing these sources.

Advancements in light engineering have led to the creation of pulsed laser sources capable of delivering high-repetition-rate, high-power few-cycle laser pulses across a wide spectral range, enabling exploration of many fascinating nonlinear processes occurring in all states of matter. High-harmonic generation, one such process, which converts the low-frequency photons of the driver laser field into soft x-rays, has revolutionized atomic, molecular, and optical physics, leading to progress in attosecond science and ultrafast optoelectronics. The Extreme Light Infrastructure, Attosecond Light Pulse Source (ELI ALPS) facility pioneers state-of-the-art tools for research in these areas. This paper outlines the design rationale, capabilities, and applications of plasma- and gas-based high-repetition-rate (1 kHz to 100 kHz) attosecond extreme ultraviolet (XUV) beamlines developed at ELI ALPS, highlighting their potential for advancing various research fields.

In the present work we report on the current progress of the recently constructed GW attosecond extreme ultraviolet (XUV) source developed at the Institute of Electronic Structure and Laser of the Foundation for Research and Technology-Hellas (I.E.S.L-FO.R.T.H.). By the implementation of a compact-collinear polarization gating arrangement, the generation of a broadband, coherent XUV quasi-continuum produced by the interaction of a many-cycle infrared field with a gas phase medium is achieved. The spectral width of the XUV emission generated in Xenon, is spanning in the range of 17-32 eV and can support isolated pulses of duration in the range from 0.4 fs to 1.3 fs and pulse energy in the 1 μJ level.Theoretical calculations, taking into account the experimental conditions of this work, are supporting the observations, offering also an insight regarding the temporal profile of the emitted radiation. Finally, the high intensity of the produced XUV pulses has been confirmed by investigating the two-XUV-photon double ionization process of Argon atoms. The demonstrated results inaugurate the capability of the beamline to produce intense isolated attosecond pulses towards their exploitation in studies of non-linear XUV processes, attosecond pulse metrology and XUV pump XUV probe experiments.

High repetition rate gas targets constitute an essential component in intense laser matter interaction studies. The technology becomes challenging as the repetition rate approaches kHz regime. In this regime, cantilever based gas valves are employed, which can open and close in tens of microseconds, resulting in a unique kind of gas characteristics in both spatial and temporal domain. Here we characterize piezo cantilever based kHz pulsed gas valves in the low density regime, where it provides sufficient peak gas density for High Harmonic Generation while releasing significantly less amount of gas reducing the vacuum load within the interaction chamber, suitable for high vacuum applications. In order to obtain reliable information of the gas density in the target jet space-time resolved characterization is performed. The gas jet system is validated by conducting interferometric gas density estimations and high harmonic generation measurements at the Extreme Light Infrastructure Attosecond Light Pulse Source (ELI ALPS) facility. Our results demonstrate that while employing such targets for optimal high harmonic generation, the high intensity interaction should be confined to a suitable time window, after the cantilever opening. The measured gas density evolution correlates well with the integrated high harmonic flux and state of the art 3D simulation results, establishing the importance of such metrology.

Two XUV-photon double ionization of Ne, induced by an intense few-pulse attosecond train with a 4 fs envelope duration is investigated experimentally and theoretically. The experiment is performed at ELI-ALPS utilizing the recently constructed 10 Hz gas phase high-order harmonic generation SYLOS GHHG-COMPACT beamline. A total pulse energy up to 1 μJ generated in Argon in conjunction with high reflectivity optics in the XUV region, allowed the observation of the doubly charged state of Ne induced by 40 eV central XUV photon energies. The interaction of the intense attosecond pulse train with Ne is also theoretically studied via a second-order time dependent perturbation theory equations-of-motion. The results of this work, combined with the feasibility of conducting XUV-pump-XUV-probe experiments, constitute a powerful tool for many potential applications. Those include attosecond pulse metrology as well as time resolved investigations of the dynamics underlying direct and sequential double ionization and their electron correlation effects.

Two-XUV-photon double ionization of Ne, induced by an intense few-pulse attosecond train with a -4 fs envelope duration is investigated experimentally and theoretically. The experiment is performed at ELI-ALPS (Extreme Light Infrastructure Attosecond Light Pulse Source) utilizing the recently constructed 10 Hz gas phase high-order harmonic generation SYLOS GHHG-COMPACT beamline. A total pulse energy up to -1 mu J generated in argon in conjunction with high-reflectivity optics in the XUV region allowed the observation of the doubly charged state of Ne induced by 40 eV central XUV-photon energies. The interaction of the intense attosecond pulse train with Ne is also theoretically studied via second-order time-dependent perturbation theory equations of motion. The results of this work, combined with the feasibility of conducting XUV-pump-XUV-probe experiments, constitute a powerful tool for many potential applications. Those include attosecond pulse metrology as well as time-resolved investigations of the dynamics underlying direct and sequential double ionization and their electron correlation effects.

Above-threshold ionization spectra from cesium are measured as a function of the carrier-envelope phase (CEP) using laser pulses centered at 3.1  μm wavelength. The directional asymmetry in the energy spectra of backscattered electrons oscillates three times, rather than once, as the CEP is changed from 0 to 2π. Using the improved strong-field approximation, we show that the unusual behavior arises from the interference of few quantum orbits. We discuss the conditions for observing the high-order CEP dependence, and draw an analogy with time-domain holography with electron wave packets.

The interpretation of experimental data from novel mid-infrared few-cycle laser sources requires an understanding of ionization mechanisms and knowledge about related ion yields. Experimental studies have indicated sequential double ionization as the dominant process above 1014 W cm−2. These results contradict a recent prediction that in this spectral region, non-sequential processes dominate the double ionization of xenon up to intensities of about 1015 W cm−2. In either case, the ratio of doubly to singly charged xenon yield reported in previous studies has been limited to a few percent, indicating a regime well below the onset of saturation of the double ionization process. We present an experimental study of double ionization of xenon and krypton atoms exposed to intense near four-cycle pulses at 3.2 μm. Our experiments rely on the ion microscopy technique, which facilitates the detection of ions originating from a restricted region within the interaction volume, thereby reducing the impact of focal averaging. Our measurements suggest that at intensities of close to 1.2 × 1014 W cm−2, double ionization of xenon and krypton is already significantly saturated. In particular, we find a doubly to singly charged yield ratio of about 75 percent for xenon and 25 percent for krypton. We compare our results with the predictions of different models accounting for the effects of volume averaging and focal geometry. We find that in the deeply saturated regime of our experiment, the Perelomov–Popov–Terentyev theory significantly underestimates the observed double ionization yield.

Recent developments in extreme ultraviolet (XUV) and x-ray radiation sources have pushed pulse energies and durations to unprecedented levels that opened up the era of non-linear XUV and x-ray optics. In this quest, laser driven high order harmonic generation sources providing attosecond resolution in the XUV spectral region enabled XUV-pump-XUV-probe experiments, while Free Electron Laser research infrastructures offer unique x-ray brilliances for highly non-linear interactions and since recently, they too entered the sub-fs temporal regime. This topical review discusses the conceptual intricacies of non-linear XUV and x-ray processes, addresses experimental particularities and highlights recent applications of such processes with emphasis to laser driven XUV-attosecond source related research.

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.

High-harmonic generation (HHG) in crystals offers a simple, affordable and easily accessible route to carrier-envelope phase (CEP) measurements, which scales favorably towards longer wavelengths. We present measurements of HHG in ZnO using few-cycle pulses at 3.1µm. Thanks to the broad bandwidth of the driving laser pulses, spectral overlap between adjacent harmonic orders is achieved. The resulting spectral interference pattern provides access to the relative harmonic phase, and hence, the CEP.

Attoscience is the emerging field that accesses the fastest electronic processes occurring at the atomic and molecular length scales with attosecond (1 as = 10−18 s) time resolution having wide ranging physical, chemical, material science and biological applications. The quintessential and one of the most fundamental processes in this domain is the generation of phase locked XUV attosecond pulses. The theoretical approach to understand the process incorporates a fully quantum or semi classical or relativistic description of coherent charge dynamics in intense ultrashort electromagnetic fields driving a quantum system (an atom, a molecule, solid band gap materials or surface plasmas). Modelling of such physical and dynamical systems in science and also in many other branches often leads to equations represented in terms of complex multi-dimensional integrals. These integrals can often be solved using the stationary phase approximation, which leads to a series of equations identifying the points in the multi-dimensional space, having most significant contributions in their evaluation. These points are usually indicated as saddle points. The description of the dynamics of quantum mechanical or relativistic systems that results from such an approach enables near to classical physics intuitive perceptions of the processes under investigation. Thus, the saddle point methods are very powerful and valuable general theoretical tools to obtain asymptotic expressions of such solutions and help also to gain physical insights on the underlying phenomena. Such techniques developed in the past have been adapted to study the emission of as pulses by different physical systems and have been widely employed in calculating and estimating the response of matter to intense electromagnetic pulses on ultrafast time scales. Here we provide an extensive disposition of the saddle point approaches unifying their ubiquitous applications within the domain of attoscience valid for simple atomic to more complex condensed matter systems undergoing ultrafast dynamics and present current trends and advancements in the field. In this review we would delineate the methodology, present a synthesis of seminal works and describe the state of the art applications. Finally we also address ultrashort time dynamics of novel materials that have gained much attention recently, namely lower dimensional material systems and micro-plasma systems.

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.

Get PDF Email Share Share with Facebook Tweet This Post on reddit Share with LinkedIn Add to CiteULike Add to Mendeley Add to BibSonomy Get Citation Copy Citation Text M. Dumergue, S. Köhn, A. Nayak, E. Skantzakis, J. Makos, J. Orfanos, D. Charalambidis, and P. Tzallas, "Towards generation of ultrahigh energy XUV pulses," in High-Brightness Sources and Light-driven Interactions, OSA Technical Digest (online) (Optica Publishing Group, 2018), paper EW2B.3. Export Citation BibTex Endnote (RIS) HTML Plain Text Citation alert Save article

Ultrashort extreme ultraviolet (EUV) laser pulses with a controllable polarization state are highly desirable for time-resolved studies and applications involving chirality, circular dichroism, spin dynamics and magnetism in the gas phase or condensed matter. A convenient method to generate such radiation is higher-order harmonic generation (HHG) as applied in numerous laboratories worldwide. Unless special techniques are employed, however, this process will produce predominantly linearly polarized EUV radiation as imposed by the symmetry of the generating field-medium system. To overcome this fundamental limitation, intense research activity has focused on shaping the time-dependent field vector of the generating light pulse [1]. In the current contribution we present an alternative method to generate EUV pulses with a widely controllable polarization state utilizing field-free aligned molecules as an anisotropically shaped medium for HHG.

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.