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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.

An open-source database containing metrology data for X-ray mirrors is presented. It makes available metrology data (mirror heights and slopes profiles) that can be used with simulation tools for calculating the effects of optical surface errors in the performances of an optical instrument, such as a synchrotron beamline. A typical case is the degradation of the intensity profile at the focal position in a beamline due to mirror surface errors. This database for metrology (DABAM) aims to provide to the users of simulation tools the data of real mirrors. The data included in the database are described in this paper, with details of how the mirror parameters are stored. An accompanying software is provided to allow simple access and processing of these data, calculate the most usual statistical parameters, and also include the option of creating input files for most used simulation codes. Some optics simulations are presented and discussed to illustrate the real use of the profiles from the database.

An open-source database containing metrology data for X-ray mirrors is presented. It makes available metrology data (mirror heights and slopes profiles) that can be used with simulation tools for calculating the effects of optical surface errors in the performances of an optical instrument, such as a synchrotron beamline. A typical case is the degradation of the intensity profile at the focal position in a beamline due to mirror surface errors. This database for metrology (DABAM) aims to provide to the users of simulation tools the data of real mirrors. The data included in the database are described in this paper, with details of how the mirror parameters are stored. An accompanying software is provided to allow simple access and processing of these data, calculate the most usual statistical parameters, and also include the option of creating input files for most used simulation codes. Some optics simulations are presented and discussed to illustrate the real use of the profiles from the database.

Soft X-ray monochromators for synchrotron radiation sources have been continuously developed over the years, improving energy resolution and stability. Great effort has been made in improving the surface quality of the optics involved, reaching values permitting diffraction-limited images. Still, one problem has not been solved, nor fully understood, yet: groove placing errors. Nowadays, these are one of the major factors responsible for resolving the power reduction of diffraction-gratings-based X-ray monochromators. Despite decades of use of gratings, there is not yet a universally established method for predicting and simulating the effect of groove placing errors on monochromator performance. This is especially important in the new scenario of high-coherent X-ray sources, i.e. diffraction-limited storage rings and free-electron lasers. To address this problem, in this article an approach based on WISER (Wavefront propagatIon Simulation codE libRary) is presented. WISER is a physical optics simulation package, also available in the user-friendly Orange Synchrotron Radiation Suite - OASYS. Even though it was originally conceived to assess the focusing performance of X-ray mirrors in the presence of height defects, it perfectly simulates the performance of a periodic (or quasi-periodic) structure like a diffraction grating. In this article, the way to use WISER and its application to a specific case, e.g. the design of a monochromator for the upgrade of a beamline at the Advanced Light Source, are shown. A simple rule for estimating how well the grooves are placed on a grating, based on calculation of the Strehl ratio, is also presented. [ABSTRACT FROM AUTHOR]

The scope of this paper is to outline the main marks and performances of the MagneDyn beamline, which was designed and built to perform ultrafast magnetodynamic studies in solids. Open to users since 2019, MagneDyn operates with variable circular and linear polarized femtosecond pulses delivered by the externally laser-seeded FERMI free-electron laser (FEL). The very high degree of polarization, the high pulse-to-pulse stability, and the photon energy tunability in the 50–300 eV range allow performing advanced time-resolved magnetic dichroic experiments at the K-edge of light elements, e.g., carbon and at the M- and N-edge of the 3d-transition-metals and rare earth elements, respectively. To this end, two experimental end-stations are available. The first is equipped with an in situ dedicated electromagnet, a cryostat, and an extreme ultraviolet Wollaston-like polarimeter. The second, designed for carry-in user instruments, hosts also a spectrometer for pump-probe resonant x-ray emission and inelastic spectroscopy experiments with a sub-eV energy resolution. A Kirkpatrick-Baez active optics system provides a minimum focus of ∼ 20 × 20 μ m2 FWHM at the sample. A pump laser setup, synchronized with the FEL-laser seeding system, delivers sub-picosecond pulses with photon energies ranging from the mid-IR to near-UV for optical pump-FEL probe experiments with a minimal pump-probe jitter of few femtoseconds. The overall combination of these features renders MagneDyn a unique state-of-the-art tool for studying ultrafast magnetic and resonant emission phenomena in solids. [ABSTRACT FROM AUTHOR]

Free-electron lasers (FELs) are the most advanced class of light-sources, by virtue of their unique capability to lase high-brightness pulses characterized by wavelengths spanning the extreme-ultraviolet, the soft and hard X-ray spectral domains, as well as by temporal lengths lying in the femtosecond (fs) timescale. The next step to push the current standards in ultrafast X-ray science is strongly linked to the possibility of engineering and exploiting time-resolved experiments exclusively for FELs pulses, ideally having different colors tunable at specific electronic resonance of the chemical elements. At the seeded FERMI FEL (Trieste, Italy) this goal is committed to the optical device known as AC/DC, which stands for the auto correlator/delay creator. AC/DC is designed to double the incoming FEL pulse splitting the photon beam by inserting a grazing incidence flat mirror, thus preserving the spectral and temporal properties, and further delaying one of these two pulses in time. It can independently tune the FEL pulses fluence on the two optical paths by means of solid-state filters, too. Here, we present a detailed description about this optical device. Strong emphasis is dedicated to the AC/DC opto-mechanical design and to the laser-based feedback systems implemented to compensate for any mismatch affecting the FEL optical trajectory, ascribable to both mechanical imperfections and paraxial errors rising during a temporal delay scan. [ABSTRACT FROM AUTHOR]

The transient dynamics of carbon monoxide (CO) molecules on a Ru(0001) surface following femtosecond optical laser pump excitation has been studied by monitoring changes in the unoccupied electronic structure using an ultrafast X-ray free-electron laser (FEL) probe. The particular symmetry of perpendicularly chemisorbed CO on the surface is exploited to investigate how the molecular orientation changes with time by varying the polarization of the FEL pulses. The time evolution of spectral features corresponding to the desorption precursor state was well distinguished due to the narrow line-width of the C K-edge in the X-ray absorption (XA) spectrum, illustrating that CO molecules in the precursor state rotated freely and resided on the surface for several picoseconds. Most of the CO molecules trapped in the precursor state ultimately cooled back down to the chemisorbed state, while we estimate that ∼14.5 ± 4.9% of the molecules in the precursor state desorbed into the gas phase. It was also observed that chemisorbed CO molecules diffused over the metal surface from on-top sites toward highly coordinated sites. In addition, a new "vibrationally hot precursor" state was identified in the polarization-dependent XA spectra. [ABSTRACT FROM AUTHOR]

FERMI is the first and only seeded EUV‐SXR free‐electron laser (FEL) facility available to users; it operates at Elettra – Sincrotrone Trieste (Italy) and it presents five operating endstations. Three of them, namely LDM (Low Density Matter), DiProI (Diffraction and Projection Imaging) and MagneDyn (Magneto‐Dynamical studies), use a Kirkpatrick–Baez (KB) active X‐ray optics system to focus the FEL pulses into the experimental chambers. The present work reports on the final results of the upgraded KB Active Optics Systems (KAOS), which have been mechanically modified in order to improve stability and repeatability with respect to the original design. The results have been obtained on both the FERMI FEL lines, FEL1 and FEL2, and are particularly relevant for the latter as it is the low‐wavelength line recently opened to users. After a thorough description of the new mechanical layout of the system and the aspects that have been improved after the refurbishment, a set of simulations of the optical performances are presented. The code used to simulate the behavior of KAOS is WISEr, a physical‐optics‐based tool, which is freely accessible, and integrated into the Oasys platform, that takes into account the specific surface metrology characterization of the beamline mirrors, including figure errors and microroughness power spectral density. The results of WISEr are then used as a reference for the actual optimization of the optical system. This procedure relies heavily on a wavefront sensor (WFS) mounted out of focus to optimize the refocusing mirrors alignment as well as their curvature bending (by minimization of the coefficients of the Zernike wavefront expansion). Moreover, the WFS data are used to reconstruct the focal spot parameters by means of a back‐propagation of the electric field. Finally, these results are compared with those obtained after the FEL ablation of a PMMA layer positioned on the focal plane, and analyzed ex situ in a post‐mortem fashion. The mechanically refurbished optical system and the multi‐technique alignment approach, aimed at optimizing the mirrors' curvature, pitch and roll angles, allowed a focal spot of 1.8 µm × 2.4 µm at 4.14 nm wavelength (FEL2) to be inferred, confirmed by the PMMA ablation imprints. [ABSTRACT FROM AUTHOR]

In this work the longitudinal shifts of the focal plane of an ellipsoidal mirror induced by longitudinal shifts of the source and by the optical figure error of the mirror itself are investigated. The case of an ideal mirror illuminated by a Gaussian beam is considered first, deriving an analytical formula predicting the source‐to‐focus shift. Then the realistic case of a mirror affected by surface shape defects is examined, by taking into account metrological data and numerically solving the Huygens–Fresnel integral. The analytical and numerical solutions in the ideal and real cases are compared. Finally, it is shown that an additional dependence of the focal shift is introduced on the wavelength and the pointing angle of the source. Both effects are investigated by numerical computations. We limit the treatment in the XUV spectral range, choosing as a test bench the Kirkpatrick–Baez mirror system of the DiProI and LDM end‐stations and at the FERMI seeded free‐electron laser (FEL). The work is primarily aimed at disentangling the different causes of focal shift at FEL light sources, where source position, wavelength and pointing angle are either tunable or rapidly fluctuating. The method can be easily extended to parabolic reflectors and refractors (lenses) with other kinds of illuminating sources and wavelengths. [ABSTRACT FROM AUTHOR]

Laser‐slicing at a diffraction‐limited storage ring light source in the soft X‐ray region is investigated with theoretical and numerical modelling. It turns out that the slicing efficiency is favoured by the ultra‐low beam emittance, and that slicing can be implemented without interference to the standard multi‐bunch operation. Spatial and spectral separation of the sub‐picosecond radiation pulse from a hundreds of picosecond‐long background is achieved by virtue of 1:1 imaging of the radiation source. The spectral separation is enhanced when the radiator is a transverse gradient undulator. The proposed configuration applied to the Elettra 2.0 six‐bend achromatic lattice envisages total slicing efficiency as high as 10−7, one order of magnitude larger than the demonstrated state‐of‐the‐art, at the expense of pulse durations as long as 0.4 ps FWHM and average laser power as high as ∼40 W. [ABSTRACT FROM AUTHOR]

Free-electron lasers (FELs) in the extreme ultraviolet (XUV) and X-ray regime opened up the possibility for experiments at high power densities, in particular allowing for fluencedependent absorption and scattering experiments to reveal non-linear light-matter interactions at ever shorter wavelengths. Findings of such non-linear effects are met with tremendous interest, but prove difficult to understand and model due to the inherent shot-toshot fluctuations in photon intensity and the often structured, non-Gaussian spatial intensity profile of a focused FEL beam. Presently, the focused beam is characterized and optimized separately from the actual experiment. Here, we present the simultaneous measurement of XUV diffraction signals from solid samples in tandem with the corresponding single-shot spatial fluence distribution on the actual sample. Our in situ characterization scheme enables direct monitoring of the sample illumination, providing a basis to optimize and quantitatively understand FEL experiments. [ABSTRACT FROM AUTHOR]

Time-resolved investigations have begun a new era of chemistry and physics, enabling the monitoring in real time of the dynamics of chemical reactions and matter. Induced transient optical absorption is a basic ultrafast electronic effect, originated by a partial depletion of the valence band, that can be triggered by exposing insulators and semiconductors to sub-picosecond extreme-ultraviolet pulses. Besides its scientific and fundamental implications, this process is very important as it is routinely applied in free-electron laser (FEL) facilities to achieve the temporal superposition between FEL and optical laser pulses with tens of femtoseconds accuracy. Here, a set of methodologies developed at the FERMI facility based on ultrafast effects in condensed materials and employed to effectively determine the FEL/laser cross correlation are presented. [ABSTRACT FROM AUTHOR]

The control of polarization state in soft and hard X-ray light is of crucial interest to probe structural and symmetry properties of matter. Thanks to their Apple-II type undulators, the FERMI-Free Electron Lasers are able to provide elliptical, circular or linearly polarized light within the extreme ultraviolet and soft X-ray range. In this paper, we report the characterization of the polarization state of FERMI FEL-2 down to 5 nm. The results show a high degree of polarization of the FEL pulses, typically above 95%. The campaign of measurements was performed at the Low Density Matter beamline using an electron Time-Of-Flight based polarimeter. [ABSTRACT FROM AUTHOR]

It was shown recently that the Fe magnetization reversal in the Fe/MnAs/GaAs(001) epitaxial system, attained by temperature control of the regular stripe pattern of the MnAs α-and β-phases, can also be driven by an ultrashort optical laser pulse. In the present time-resolved scattering experiment, we address the dynamics of the MnAs α-β self-organized stripe pattern induced by a 100 fs optical laser pulse, using as a probe the XUV radiation from the FERMI free-electron laser. We observe a loss in the diffraction intensity from the ordered α-β stripes that occurs at two characteristic timescales in the range of ~10-12 and ~10-10. We associate the first intensity drop with ultrafast electron-lattice energy exchange processes within the laser-MnAs interaction volume and the second with thermal diffusion towards the MnAs/GaAs interface. With the support of model calculations, the observed dynamics are interpreted in terms of the formation of a laterally homogeneous MnAs overlayer, the thickness of which evolves in time, correlating the MnAs microstructure dynamics with the Fe magnetization response. [ABSTRACT FROM AUTHOR]

The potential of the two-color mode implemented at the FERMI free-electron laser (FEL) source for pumping and probing selectively different atomic species has been demonstrated by time-resolved scattering experiments with permalloy (FeNi alloy) and NiFe2O4 samples. We monitored the ultra-fast demagnetization of Ni induced by the pump FEL pulse, by tuning the linearly-polarized FEL probe pulse to the Ni-3p resonance and measuring the scattered intensity in the transverse magneto-optical Kerr effect geometry. The measurements were performed by varying the intensity of the FEL pump pulse, tuning its wavelength to and off of the Fe-3p resonance, and by spanning the FEL probe pulse delays across the 300-900 fs range. The obtained results have evidenced that for the case of NiFe2O4, there is a sensible difference in the magnetic response at the Ni site when the pump pulse causes electronic excitations at the Fe site. [ABSTRACT FROM AUTHOR]

A new high-performance method for the free-electron laser (FEL) focused beam diagnosis has been successfully tested at the FERMI FEL in Trieste, Italy. The novel pixelated phosphor detector (PPD) consists of micrometric pixels produced by classical UV lithography and dry etching technique, fabricated on a silicon substrate, arranged in a hexagonal geometry and filled with suitable phosphors. It has been demonstrated that the overall resolution of the system has increased by reducing the diffusion of the light in the phosphors. Various types of PPD have been produced and tested, demonstrating a high resolution in the beam profile and the ability to measure the actual spot size shot-to-shot with an unprecedented resolution. For these reasons, the proposed detector could become a reference technique in the FEL diagnosis field. [ABSTRACT FROM AUTHOR]

The future Magneto Dynamics (MagneDyn) beamline will be devoted to study the electronic states and the local magnetic properties of excited and transient states of complex systems by means of the time-resolved X-ray absorption spectroscopy technique. The beamline will use FERMI's high-energy source covering the wavelength range from 60 nm down to 1.3 nm. An on-line photon energy spectrometer will allow spectra to be measured with high resolution while delivering most of the beam to the end-stations. Downstream the beam will be possibly split and delayed, by means of a delay line, and then focused with a set of active Kirkpatrick-Baez mirrors. These mirrors will be able to focus the radiation in one of the two MagneDyn experimental chambers: the electromagnet end-station and the resonant inelastic X-ray scattering end-station. After an introduction of the MagneDyn scientific case, the layout will be discussed showing the expected performances of the beamline. [ABSTRACT FROM AUTHOR]

Measurement of the emission wavelength and the spectral content of the photon radiation is essential information for both machine and experimental physicists at a free-electron laser (FEL) user facility. Knowledge of the photon beam spectral properties is needed during the machine optimization and for performing machine studies ( i.e. monitoring the change of the FEL output as a function of the machine parameters). The experimentalists, on the other hand, need to know the photon beam spectral distribution of the source, shot to shot, to discriminate the acquired data. Consequently, the main requirement for the instrument, supposed to obtain this information, is the capability of working on-line and shot-to-shot, with minimal perturbation of the beam delivered to the experimental stations. Starting from the grating fundamental equations, the conceptual design of the FERMI Pulse-Resolved Energy Spectrometer: Transparent and On-line (PRESTO) is presented, explaining the optical design in detail. The performance of PRESTO, in terms of resolving power, efficiency and spectral response, is also discussed. Finally, some useful features beyond the usual measurement of the energy spectrum are reported, as they have been routinely used by both machine and experimental physicists. [ABSTRACT FROM AUTHOR]

TeraFERMI is the new terahertz (THz) beamline for pump-probe studies on the femtosecond time-scale, under construction at the FERMI free-electron laser (FEL) facility in Trieste, Italy. The beamline will take advantage of the coherent radiation emitted by the spent electrons from the FEL undulators, before being dumped. This will result in short, coherent, high-power THz pulses to be used as a pump beam, in order to modulate structural properties of matter, thereby inducing phase transitions. The TeraFERMI beamline collects THz radiation in the undulator hall and guides it along a beam pipe which is approximately 30 m long, extending across the safety hutch and two shielding walls. Here the optical design, which will allow the efficient transport of the emitted THz radiation in the experimental hall, is presented. [ABSTRACT FROM AUTHOR]

The Low Density Matter (LDM) beamline has been built as part of the FERMI free-electron laser (FEL) facility to serve the atomic, molecular and cluster physics community. After the commissioning phase, it received the first external users at the end of 2012. The design and characterization of the LDM photon transport system is described, detailing the optical components of the beamline. [ABSTRACT FROM AUTHOR]

The Photon Analysis Delivery and REduction System of FERMI (PADReS) has been routinely used during the machine commissioning and operations of FERMI since 2011. It has also served the needs of several user runs at the facility from late 2012. The system is endowed with online and shot-to-shot diagnostics giving information about intensity, spatial-angular distribution, spectral content, as well as other diagnostics to determine coherence, pulse length etc. Moreover, PADReS is capable of manipulating the beam in terms of intensity and optical parameters. Regarding the optics, besides a standard refocusing system based on an ellipsoidal mirror, the Kirkpatrick-Baez active optics systems are key elements and have been used intensively to meet users' requirements. A general description of the system is given, together with some selected results from the commissioning/operations/user beam time. [ABSTRACT FROM AUTHOR]

The Diffraction and Projection Imaging (DiProI) beamline at FERMI, the Elettra free-electron laser (FEL), hosts a multi-purpose station that has been opened to users since the end of 2012. This paper describes the core capabilities of the station, designed to make use of the unique features of the FERMI-FEL for performing a wide range of static and dynamic scattering experiments. The various schemes for time-resolved experiments, employing both soft X-ray FEL and seed laser IR radiation are presented by using selected recent results. The ongoing upgrade is adding a reflection geometry setup for scattering experiments, expanding the application fields by providing both high lateral and depth resolution. [ABSTRACT FROM AUTHOR]

Abstract: X-ray mirrors with high focusing performances are in use in both mirror modules for X-ray telescopes and in synchrotron and FEL (Free Electron Laser) beamlines. A degradation of the focus sharpness arises in general from geometrical deformations and surface roughness, the former usually described by geometrical optics and the latter by physical optics. In general, technological developments are aimed at a very tight focusing, which requires the mirror profile to comply with the nominal shape as much as possible and to keep the roughness at a negligible level. However, a deliberate deformation of the mirror can be made to endow the focus with a desired size and distribution, via piezo actuators as done at the EIS-TIMEX beamline of FERMI@Elettra. The resulting profile can be characterized with a Long Trace Profilometer and correlated with the expected optical quality via a wavefront propagation code. However, if the roughness contribution can be neglected, the computation can be performed via a ray-tracing routine, and, under opportune assumptions, the focal spot profile (the Point Spread Function, PSF) can even be predicted analytically. The advantage of this approach is that the analytical relation can be reversed; i.e., from the desired PSF the required mirror profile can be computed easily, thereby avoiding the use of complex and time-consuming numerical codes. The method can also be suited in the case of spatially inhomogeneous beam intensities, as commonly experienced at synchrotrons and FELs. In this work we expose the analytical method and the application to the beam shaping problem. [Copyright &y& Elsevier]

Abstract: To enhance the reflectivity of X-ray mirrors beyond the critical angle, multilayer coatings are required. Interface imperfections in the multilayer growth process are known to cause non-specular scattering and degrade the mirror optical performance; therefore, it is important to predict the amount of X-ray scattering from the rough topography of the outer surface of the coating, which can be directly measured, e.g., with an Atomic Force Microscope (AFM). This kind of characterization, combined with X-ray reflectivity measurements to assess the deep multilayer stack structure, can be used to model the layer roughening during the growth process via a well-known roughness evolution model. In this work, X-ray scattering measurements are performed and compared with simulations obtained from the modeled interfacial Power Spectral Densities (PSDs) and the modeled Crossed Spectral Densities for all the couples of interfaces. We already used this approach in a previous work for periodic multilayers; we now show how this method can be extended to graded multilayers. The upgraded code is validated for both periodic and graded multilayers, with a good accord between experimental data and model findings. Doing this, different kinds of defects observed in AFM scans are included in the PSD analysis. The subsequent data-model comparison enables us to recognize them as surface contamination or interfacial defects that contribute to the X-ray scattering of the multilayer. [Copyright &y& Elsevier]

Wave packet interferometry with vacuum ultraviolet light has been used to probe a complex region of the electronic spectrum of molecular nitrogen, N2. Wave packets of Rydberg and valence states were excited by using double pulses of vacuum ultraviolet (VUV), free-electron-laser (FEL) light. These wave packets were composed of contributions from multiple electronic states with a moderate principal quantum number (n ∼ 4-9) and a range of vibrational and rotational quantum numbers. The phase relationship of the two FEL pulses varied in time, but as demonstrated previously, a shot-by-shot analysis allows the spectra to be sorted according to the phase between the two pulses. The wave packets were probed by angle-resolved photoionization using an infrared pulse with a variable delay after the pair of excitation pulses. The photoelectron branching fractions and angular distributions display oscillations that depend on both the time delays and the relative phases of the VUV pulses. The combination of frequency, time delay, and phase selection provides significant control over the ionization process and ultimately improves the ability to analyze and assign complex molecular spectra., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

The electronic excitation occurring on adsorbates at ultrafast timescales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of x-ray absorption spectroscopy (XAS) and x-ray emission spectroscopy (XES) of a simple well-known adsorbate prototype system, namely carbon (C) atoms adsorbed on a nickel [Ni(100)] surface, following intense laser optical pumping at 400 nm. We observe ultrafast (∼100  fs) changes in both XAS and XES showing clear signatures of the formation of a hot electron-hole pair distribution on the adsorbate. This is followed by slower changes on a few picoseconds timescale, shown to be consistent with thermalization of the complete C/Ni system. Density functional theory spectrum simulations support this interpretation.

We report on carbon monoxide desorption and oxidation induced by 400 nm femtosecond laser excitation on the O/Ru(0001) surface probed by time-resolved x-ray absorption spectroscopy (TR-XAS) at the carbon K-edge. The experiments were performed under constant background pressures of CO (6 × 10 -8 Torr) and O 2 (3 × 10 -8 Torr). Under these conditions, we detect two transient CO species with narrow 2π* peaks, suggesting little 2π* interaction with the surface. Based on polarization measurements, we find that these two species have opposing orientations: (1) CO favoring a more perpendicular orientation and (2) CO favoring a more parallel orientation with respect to the surface. We also directly detect gas-phase CO 2 using a mass spectrometer and observe weak signatures of bent adsorbed CO 2 at slightly higher x-ray energies than the 2π* region. These results are compared to previously reported TR-XAS results at the O K-edge, where the CO background pressure was three times lower (2 × 10 -8 Torr) while maintaining the same O 2 pressure. At the lower CO pressure, in the CO 2π* region, we observed adsorbed CO and a distribution of OC-O bond lengths close to the CO oxidation transition state, with little indication of gas-like CO. The shift toward "gas-like" CO species may be explained by the higher CO exposure, which blocks O adsorption, decreasing O coverage and increasing CO coverage. These effects decrease the CO desorption barrier through dipole-dipole interaction while simultaneously increasing the CO oxidation barrier.

Performing experiments at free-electron lasers (FELs) requires an exhaustive knowledge of the pulse temporal and spectral profile, as well as the focal spot shape and size. Operating FELs in the extreme ultraviolet (EUV) and soft X-ray (SXR) spectral regions calls for designing ad-hoc optical layouts to transport and characterize the EUV/SXR beam, as well as tailoring its spatial dimensions at the focal plane down to sizes in the few micrometers range. At the FERMI FEL (Trieste, Italy) this task is carried out by the Photon Analysis Delivery and Reduction System (PADReS). In particular, to meet the different experimental requests on the focal spot shape and size, a proper tuning of the optical systems is required, and this should be monitored by means of dedicated techniques. Here, we present and compare two reconstruction methods for spot characterization: single-shot imprints captured via ablation on a poly(methyl methacrylate) sample (PMMA) and pulse profiles retrieved by means of a Hartmann wavefront sensor (WFS). By recording complementary datasets at and nearby the focal plane, we exploit the tomography of the pulse profile along the beam propagation axis, as well as a qualitative and quantitative comparison between these two reconstruction methods.

We use a pump-probe scheme to measure the time evolution of the C K-edge x-ray absorption spectrum from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Because of the short duration of the x-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first picosecond after the pump can be resolved with unprecedented time resolution. By comparing with density functional theory spectrum calculations, we find high excitation of the internal stretch and frustrated rotation modes occurring within 200 fs of laser excitation, as well as thermalization of the system in the picosecond regime. The ∼100  fs initial excitation of these CO vibrational modes is not readily rationalized by traditional theories of nonadiabatic coupling of adsorbates to metal surfaces, e.g., electronic frictions based on first order electron-phonon coupling or transient population of adsorbate resonances. We suggest that coupling of the adsorbate to nonthermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes.

We have used the FERMI free-electron laser to perform time-resolved photoelectron imaging experiments on a complex group of resonances near 15.38 eV in the absorption spectrum of molecular nitrogen, N 2 , under jet-cooled conditions. The new data complement and extend the earlier work of Fushitani et al. [Opt. Express 27, 19702-19711 (2019)], who recorded time-resolved photoelectron spectra for this same group of resonances. Time-dependent oscillations are observed in both the photoelectron yields and the photoelectron angular distributions, providing insight into the interactions among the resonant intermediate states. In addition, for most states, we observe an exponential decay of the photoelectron yield that depends on the ionic final state. This observation can be rationalized by the different lifetimes for the intermediate states contributing to a particular ionization channel. Although there are nine resonances within the group, we show that by detecting individual photoelectron final states and their angular dependence, we can identify and differentiate quantum pathways within this complex system.

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).

The advent of free-electron laser (FEL) sources delivering two synchronized pulses of different wavelengths (or colours) has made available a whole range of novel pump-probe experiments. This communication describes a major step forward using a new configuration of the FERMI FEL-seeded source to deliver two pulses with different wavelengths, each tunable independently over a broad spectral range with adjustable time delay. The FEL scheme makes use of two seed laser beams of different wavelengths and of a split radiator section to generate two extreme ultraviolet pulses from distinct portions of the same electron bunch. The tunability range of this new two-colour source meets the requirements of double-resonant FEL pump/FEL probe time-resolved studies. We demonstrate its performance in a proof-of-principle magnetic scattering experiment in Fe-Ni compounds, by tuning the FEL wavelengths to the Fe and Ni 3p resonances.

The recent advent of free-electron laser (FEL) sources is driving the scientific community to extend table-top laser research to shorter wavelengths adding elemental selectivity and chemical state specificity. Both a compact setup (mini-TIMER) and a separate instrument (EIS-TIMER) dedicated to four-wave-mixing (FWM) experiments has been designed and constructed, to be operated as a branch of the Elastic and Inelastic Scattering beamline: EIS. The FWM experiments that are planned at EIS-TIMER are based on the transient grating approach, where two crossed FEL pulses create a controlled modulation of the sample excitations while a third time-delayed pulse is used to monitor the dynamics of the excited state. This manuscript describes such experimental facilities, showing the preliminary results of the commissioning of the EIS-TIMER beamline, and discusses original experimental strategies being developed to study the dynamics of matter at the fs-nm time-length scales. In the near future such experimental tools will allow more sophisticated FEL-based FWM applications, that also include the use of multiple and multi-color FEL pulses.

The Elastic and Inelastic Scattering (EIS) beamline at the free-electron laser FERMI is presented. It consists of two separate end-stations: EIS-TIMEX, dedicated to ultrafast time-resolved studies of matter under extreme and metastable conditions, and EIS-TIMER, dedicated to time-resolved spectroscopy of mesoscopic dynamics in condensed matter. The scientific objectives are discussed and the instrument layout illustrated, together with the results from first exemplifying experiments.

Knowledge of the sequence of different conformational states of a protein molecule is key to better understanding its biological function. A diffraction pattern from a single conformational state can be captured with an ultrafast X-ray Free-Electron Laser (XFEL) before the target is completely annihilated by the radiation. In this paper, we report the first experimental demonstration of conformation sequence recovery using diffraction patterns from randomly ordered conformations of a non-periodic object using the dimensional reduction technique Isomap and coherent diffraction imaging.

We present the experimental demonstration of a method for generating two spectrally and temporally separated pulses by an externally seeded, single-pass free-electron laser operating in the extreme-ultraviolet spectral range. Our results, collected on the FERMI@Elettra facility and confirmed by numerical simulations, demonstrate the possibility of controlling both the spectral and temporal features of the generated pulses. A free-electron laser operated in this mode becomes a suitable light source for jitter-free, two-colour pump-probe experiments.