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X-ray free-electron lasers (FELs), which amplify light emitted by a relativistic electron beam, are extending nonlinear optical techniques to shorter wavelengths, adding element specificity by exciting and probing electronic transitions from core levels. These techniques would benefit tremendously from having a stable FEL source, generating spectrally pure and wavelength-tunable pulses. We show that such requirements can be met by operating the FEL in the so-called echo-enabled harmonic generation (EEHG) configuration. Here, two external conventional lasers are used to precisely tailor the longitudinal phase space of the electron beam before emission of X-rays. We demonstrate high-gain EEHG lasing producing stable, intense, nearly fully coherent pulses at wavelengths as short as 5.9 nm (~211 eV) at the FERMI FEL user facility. Low sensitivity to electron-beam imperfections and observation of stable, narrow-band, coherent emission down to 2.6 nm (~474 eV) make the technique a prime candidate for generating laser-like pulses in the X-ray spectral region, opening the door to multidimensional coherent spectroscopies at short wavelengths.Echo-enabled harmonic generation in a free-electron laser enables 45th harmonic pulses from a 264 nm wavelength seed, yielding 5.9 nm wavelength coherent output.

Photons have fixed spin and unbounded orbital angular momentum (OAM). While the former is manifested in the polarization of light, the latter corresponds to the spatial phase distribution of its wavefront1. The distinctive way in which the photon spin dictates the electron motion upon light–matter interaction is the basis for numerous well-established spectroscopies. By contrast, imprinting OAM on a matter wave, specifically on a propagating electron, is generally considered very challenging and the anticipated effect undetectable2. In refs. 3,4, the authors provided evidence of OAM-dependent absorption of light by a bound electron. Here, we seek to observe an OAM-dependent dichroic photoelectric effect, using a sample of He atoms. Surprisingly, we find that the OAM of an optical field can be imprinted coherently onto a propagating electron wave. Our results reveal new aspects of light–matter interaction and point to a new kind of single-photon electron spectroscopy.The findings that the spatial distribution of an optical field with vortex phase profile can be imprinted coherently onto a propagating electron wave reveal new aspects of light–matter interactions and will help develop future single-photon electron spectroscopy.

Exploiting acceleration gradients that are up to three orders of magnitude higher than those achievable using conventional radiofrequency-based devices, plasma-based devices promise a revolution in particle acceleration, enabling particles to reach high energies over much shorter distances than existing accelerators [...]

The two single-pass, externally seeded free-electron lasers (FELs) of the FERMI user facility are designed around Apple-II-type undulators that can operate at arbitrary polarization in the vacuum ultraviolet-to-soft x-ray spectral range. Furthermore, within each FEL tuning range, any output wavelength and polarization can be set in less than a minute of routine operations. We report the first demonstration of the full output polarization capabilities of FERMI FEL-1 in a campaign of experiments where the wavelength and nominal polarization are set to a series of representative values, and the polarization of the emitted intense pulses is thoroughly characterized by three independent instruments and methods, expressly developed for the task. The measured radiation polarization is consistently >90% and is not significantly spoiled by the transport optics; differing, relative transport losses for horizontal and vertical polarization become more prominent at longer wavelengths and lead to a non-negligible ellipticity for an originally circularly polarized state. The results from the different polarimeter setups validate each other, allow a cross-calibration of the instruments, and constitute a benchmark for user experiments.

Experimental characterization of the structural, electronic and dynamic properties of dilute systems in aqueous solvents, such as nanoparticles, molecules and proteins, are nowadays an open challenge. X-ray absorption spectroscopy (XAS) is probably one of the most established approaches to this aim as it is element-specific. However, typical dilute systems of interest are often composed of light elements that require extreme-ultraviolet to soft X-ray photons. In this spectral regime, water and other solvents are rather opaque, thus demanding radical reduction of the solvent volume and removal of the liquid to minimize background absorption. Here, we present an experimental endstation designed to operate a liquid flat jet of sub-micrometre thickness in a vacuum environment compatible with extreme ultraviolet/soft XAS measurements in transmission geometry. The apparatus developed can be easily connected to synchrotron and free-electron-laser user-facility beamlines dedicated to XAS experiments. The conditions for stable generation and control of the liquid flat jet are analyzed and discussed. Preliminary soft XAS measurements on some test solutions are shown.

Chirped pulse amplification in optical lasers is a revolutionary technique, which allows the generation of extremely powerful femtosecond pulses in the infrared and visible spectral ranges. Such pulses are nowadays an indispensable tool for a myriad of applications, both in fundamental and applied research. In recent years, a strong need emerged for light sources producing ultra-short and intense laser-like X-ray pulses, to be used for experiments in a variety of disciplines, ranging from physics and chemistry to biology and material sciences. This demand was satisfied by the advent of short-wavelength free-electron lasers. However, for any given free-electron laser setup, a limit presently exists in the generation of ultra-short pulses carrying substantial energy. Here we present the experimental implementation of chirped pulse amplification on a seeded free-electron laser in the extreme-ultraviolet, paving the way to the generation of fully coherent sub-femtosecond gigawatt pulses in the water window (2.3–4.4 nm). Short laser pulses of femtosecond time scales are in high demand in order to explore the fast electron dynamics in light-matter interactions. Here, the authors demonstrated the compression of free electron laser pulses in the extreme ultraviolet range by using a chirped pulse amplification technique.

The calibration activities of the COmpact SPectrometer—COSP for the FERMI Free-Electron Laser (FEL) facility at the Elettra Synchrotron (Italy) are presented. COSP is an in-house built grating spectrometer designed to be used during the optimization of the FERMI parameters and to control the relative stability between different FEL harmonics in the multi-harmonic emission mode. The spectrometer is designed to work in single-shot mode at a repetition rate of 50 Hz providing medium resolution in a wide spectral range in order to either measure the separate intensities of the harmonics being mixed in a multi-color experiment or to quantify the amount of possible spurious harmonics. These activities are of key importance in the new class of experiments based on the wave mixing paradigm tested at the seeded FEL FERMI.

The development of novel coherent and brilliant sources, such as soft X-ray free electron laser (FEL) and high harmonic generation (HHG), enables new ultrafast analysis of the electronic and structural dynamics of a wide variety of materials. Soft X-ray FEL delivers high-brilliance beams with a short pulse duration, high spatial coherence and photon energy tunability. In comparison with FELs, HHG X-ray sources are characterized by a wide spectral bandwidth and few- to sub-femtosecond pulses. The approach will lead to the time-resolved reconstruction of molecular dynamics, shedding light on different photochemical pathways. The high peak brilliance of soft X-ray FELs facilitates investigations in a nonlinear regime, while the broader spectral bandwidth of the HHG sources may provide the simultaneous probing of multiple components. Significant technical breakthroughs in these novel sources are under way to improve brilliance, pulse duration, and to control spectral bandwidth, spot size, and energy resolution. Therefore, in the next few years, the new generation of soft X-ray sources combined with novel experimental techniques, new detectors, and computing capabilities will allow for the study of several extremely fast dynamics, such as vibronic dynamics. In the present review, we discuss recent developments in experiments, performed with soft X-ray FELs and HHG sources, operating near the carbon K-absorption edge, being a key atomic component in biosystems and soft materials. Different spectroscopy methods such as time-resolved pump-probe techniques, nonlinear spectroscopies and photoelectron spectroscopy studies have been addressed in an attempt to better understand fundamental physico-chemical processes.

EuPRAXIA@SPARC_LAB is a new Free Electron Laser (FEL) facility that is currently under construction at the Laboratori Nazionali di Frascati of the INFN. The electron beam driving the FEL will be delivered by an X-band normal conducting LINAC followed by a plasma wakefield acceleration stage. It will be characterized by a small footprint and will deliver ultra-bright photon pulses for experiments in the water window to the user community. In addition to the soft-X-rays beamline already planned in the project, we propose the installation of a second photon beamline with seeded FEL pulses in the range between 50 and 180 nm. Here, we will present the FEL generation scheme, the layout of the dedicated beamline and the potential applications of the FEL radiation source in this low energy range.

The metrology of attosecond pulse trains is based on a cross-correlation technique between a comb of extreme ultraviolet harmonics generated by the high-order harmonic generation process and a synchronised infrared field. The approach, usually referred to as reconstruction of attosecond beating by interference of two-photon transitions (RABBIT), allows one to recover the relative phase between the comb of consecutive odd harmonics, thus providing access to the attosecond temporal structure of the radiation. Seeded free-electron lasers have recently demonstrated the generation of combs consisting of even and odd harmonics of the seeding radiation. In this scheme, each harmonic is generated by an independent undulator (or set thereof), providing an additional degree of freedom in selecting the specific harmonics that make up the extreme ultraviolet comb. Here, we present results on the generation and temporal characterisation of a comb consisting of non-consecutive harmonics. The single-shot correlation analysis of the photoelectron spectra and the reordering of the single-shot data using an attosecond timing tool allow the reconstruction of the group delay dispersion of the harmonic comb and the temporal reconstruction of the attosecond pulse train. Attosecond pulse trains, crucial for ultrafast science, traditionally consist of only odd harmonics due to symmetry constraints in high-order harmonic generation. Here, the authors extend the RABBIT technique to analyze non-consecutive harmonics, enabling the temporal reconstruction of attosecond pulse trains and advancing metrology in extreme ultraviolet spectroscopy.