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Time-resolved ultrafast EUV magnetic scattering was used to test a recent prediction of >10 km/s domain wall speeds by optically exciting a magnetic sample with a nanoscale labyrinthine domain pattern. Ultrafast distortion of the diffraction pattern was observed at markedly different timescales compared to the magnetization quenching. The diffraction pattern distortion shows a threshold-dependence with laser fluence, not seen for magnetization quenching, consistent with a picture of domain wall motion with pinning sites. Supported by simulations, we show that a speed of $\approx$ 66 km/s for highly curved domain walls can explain the experimental data. While our data agree with the prediction of extreme, non-equilibrium wall speeds locally, it differs from the details of the theory, suggesting that additional mechanisms are required to fully understand these effects., 5 pages, 4 figures; Supplemental Material: 9 pages, 9 figures

The advent of free electron lasers (FELs) in the soft and hard X-ray spectral region has opened the possibility to probe electronic, magnetic and structural dynamics, in both diluted and condensed matter samples, with femtosecond time resolution. In particular, FELs strongly enhanced the capabilities of several analytical techniques, which took advantage of the high degree of transverse coherence provided. FELs based on the harmonic up-conversion of an external seed laser are characterised also by a high degree of longitudinal coherence, since electrons inherit the coherence properties of the seed. At the present state of the art, the shortest wavelength delivered to user experiments by an externally seeded FEL light source is about 4 nm. We show here that pulses with a high longitudinal degree of coherence (first and second order) covering the water window and with photon energy extending up to 790 eV can be generated by exploiting the so-called nonlinear harmonic regime, which allows generation of radiation at harmonics of the resonant FEL wavelength. Moreover, we report the results of two proof-of-principle experiments: one measuring the oxygen K-edge absorption in water ($\sim$ 530 eV), the other analysing the spin dynamics of Fe and Co through magnetic small angle x-ray scattering at their L-edges (707 eV and 780 eV)

Time-resolved X-ray Emission/Absorption Spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires X-ray pulses with both a narrow bandwidth and sub-picosecond pulse duration, a combination that in principle finds its optimum with Fourier transform-limited pulses. In this work, we explore an alternative xperimental approach, capable of simultaneously retrieving information about unoccupied (XAS) and occupied (XES) states from the stochastic fluctuations of broadband extreme ultraviolet pulses of a free-electron laser. We used this method, in combination with singular value decomposition and Tikhonov regularization procedures, to determine the XAS/XES response from a crystalline silicon sample at the L2,3-edge, with an energy resolution of a few tens of meV. Finally, we combined this spectroscopic method with a pump-probe approach to measure structural and electronic dynamics of a silicon membrane. Tr-XAS/XES data obtained after photoexcitation with an optical laser pulse at 390 nm allowed us to observe perturbations of the band structure, which are compatible with the formation of the predicted precursor state of a non-thermal solid-liquid phase transition associated with a bond softening phenomenon.

High-resolution emission/absorption spectroscopy with picosecond time resolution appears to be strategic in fundamental matter physics investigation as well as in functional materials characterization. Such a method typically requires a pulsed radiation source and high energy resolution, along with a large data statistic. In this work we demonstrate the possibility to retrieve high resolution absorption and emission spectra with picosecond time resolution, by exploiting the stochastic nature of the wide-band self-amplified FEL radiation provided by FERMI. In this work we get advantage of the two spectrometers present on the TIMEX beamline to reconstruct a 2D emission/absorption spectrum of a Si sample. To do so, we applied the singular value decomposition on the single-pulse incoming and outgoing spectra; by applying Tikhonov regularization, we were able to obtain spectra with an energy resolution of few tens of meV. In addition, we performed a time resolved characterization of the Si L23-edge and Si emission line at 99.3 eV by pumping the Si sample with visible laser below damage threshold. The result of this measurement allow us to claim for a bond softening phenomenon on the picosecond time-scale.

Coherent light-matter interactions mediated by opto-magnetic phenomena like the inverse Faraday effect (IFE) are expected to provide a non-thermal pathway for ultrafast manipulation of magnetism on timescales as short as the excitation pulse itself. As the IFE scales with the spin-orbit coupling strength of the involved electronic states, photo-exciting the strongly spin-orbit coupled core-level electrons in magnetic materials appears as an appealing method to transiently generate large opto-magnetic moments. Here, we investigate this scenario in a ferrimagnetic GdFeCo alloy by using intense and circularly polarized pulses of extreme ultraviolet radiation. Our results reveal ultrafast and strong helicity-dependent magnetic effects which are in line with the characteristic fingerprints of an IFE, corroborated by ab initio opto-magnetic IFE theory and atomistic spin dynamics simulations.

Free-electron lasers (FELs) are currently the most advanced class of light sources, by virtue of their unique capability to lase high-brightness and ultrashort pulses characterized by wavelengths spanning the Extreme-Ultraviolet (EUV), the Soft (SXR) and Hard (HXR) X-Ray spectral domains, alongside with temporal duration lying in the femtosecond (fs) timescale [1]. Specifically, the advent of FELs light sources has recently allowed to perform, in a time-resolved fashion approach, both established spectroscopies, daily employed at synchrotron light sources, and novel non-linear optical methods, mostly combining FELs and laser pulses. Nonetheless, the next step to push the ultrafast X-Ray science standards is widely recognized to be linked to go beyond the current time-resolved schemes, so performing experiments engaging exclusively EUV, SXR and HXR pulses. Indeed, exciting (and probing) matter at its (or nearby) electronic resonance is largely speculated to be one of the key for discriminating and revealing the microscopic mechanisms hiding behind some of the most exotic phases of physical, chemical, and biological systems. Such a challenge calls the design of optical devices capable to both split and delay (in time) FELs pulses, without impacting on their coherence properties, and fully user-friendly in terms of preserving the perfect overlap of the resulting focal spots, even in the few microns spatial domain, a well-known trademark for focusing EUV, SXR and HXR pulses at FELs light sources [2]. At the seeded FERMI FEL (Trieste, Italy) this goal is committed by the novel optical device known as AC/DC, which stands for the Auto Correlator/Delay Creator. AC/DC is purposely designed to double the incoming FEL photon beam into two exact pulse replicas, splitting it by inserting a grazing incidence flat mirror, and further delaying in time, in a controlled way, one of the two pulses, with an intrinsic temporal resolution of approximately 360 attoseconds. A detailed description of AC/DC is highlighted here. Specifically, strong emphasis is dedicated to the opto-mechanical design and the laser-based feedback system, purposely designed and implemented to compensate in real-time any potential drift and pointing mismatch affecting the FEL optical trajectory, ascribable to both mechanical imperfections and residual paraxial errors appearing during a temporal delay scan [3]. [1] Bostedt C., Boutet S., Fritz D.M., Huang Z., Lee H.J., Lemke H.T., Robert A., Schlotter W.F., Turner J.J., Williams G.J., Linac Coherent Light Source: The first five years. Rev. Mod. Phys.88, 015007 (2016) [2] Manfredda M., Fava C., Gobessi R., Mahne N., Raimondi L., Simoncig A., Zangrando M., The evolution of KAOS, a multipurpose active optics system for EUV/Soft X-rays, Synchrotron Radiation News, 0, 0, (2022) DOI: 10.1080/08940886.2022.2066432 . [3] Simoncig A., Manfredda M., Gaio G., Mahne N., Raimondi M., Fava C., Gerusina S., Gobessi R., Abrami A., Capotondi F., De Angelis D., Menk R., Pancaldi M., Pedersoli E., Zangrando M., AC/DC: The FERMI FEL Split and Delay Optical Device for Ultrafast X-rays Science, Photonics, 9(5), 314, 2022

The recently discovered topological fluctuation state provides a fascinating new perspective on the ultrafast emergence of topology in condensed matter systems. However, rather little is known about the physics of this state and the origin of the topological fluctuations. Using time-resolved small-angle x-ray scattering, we observe that topological fluctuation states appear after laser excitation even if the final state does not host stable skyrmions. Simulations support these findings and reveal that the fluctuations originate from the competition between spontaneous nucleation and decay of skyrmions, consistent with Arrhenius-like activation over a potential barrier. Stable skyrmions can freeze out of such fluctuations when the effective temperature of the system relaxes faster than the decay time of the skyrmions. Our results reveal a robust scenario for the generation of topological fluctuation states, potentially enabling their study in a wide variety of magnetic systems.

We demonstrate the measurement of ultrafast dynamics using ghost spectroscopy and a pump-probe approach with an optical pump and a short-wavelength radiation probe. The ghost spectroscopy approach is used to overcome the challenge of the strong intensity and spectrum fluctuations at free-electron lasers and to provide high -spectral resolution, which enables the measurement of small energy shifts in the absorption spectrum. We exploit the high resolution to explore the dynamics of the charge carrier excitations and relaxations and their impact on the photoinduced structural changes in silicon by measuring the variation of the absorption spectrum of a Si(100) membrane near the silicon L2,3 edge and the accompanying edge shifts in response to the optical illumination.

Supporting information

We use a pump-probe scheme to measure the time evolution of the C K-edge X-ray absorption spectrum (XAS) from CO/Ru(0001) after excitation by an ultrashort high-intensity optical laser pulse. Due to the short duration of the X-ray probe pulse and precise control of the pulse delay, the excitation-induced dynamics during the first ps after the pump can be resolved with unprecedented time resolution. By comparing with theoretical (DFT) 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 ps 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 non-thermalized electron-hole pairs is responsible for the ultrafast initial excitation of the modes., Comment: 16 pages, 16 figures. To be published in Physical Review Letters: https://journals.aps.org/prl/accepted/c1070Y74M8b18063d9cd0221b000631d50ef7a249

While chiral spin structures stabilized by Dzyaloshinskii-Moriya interaction (DMI) are candidates as novel information carriers, their dynamics on the fs-ps timescale is little known. Since with the bulk Heisenberg exchange and the interfacial DMI two distinct exchange mechanisms are at play, the ultra-fast dynamics of the chiral order needs to be ascertained and compared to the dynamics of the conventional collinear order. Using an XUV free-electron laser we determine the fs-ps temporal evolution of the chiral order in domain walls in a magnetic thin film sample by an IR pump-X-ray magnetic scattering probe experiment. Upon demagnetisation we observe that the dichroic (CL-CR) signal from the chiral order in the domain walls recovers significantly faster than the (CL+CR) sum signal from the average collinear domain magnetisation. We explore possible explanations based on spin structure dynamics and reduced transversal magnetisation fluctuations inside the domain walls and find that the latter can explain the experimental data leading to distinctly different dynamics for collinear magnetic order and chiral magnetic order.

In chemistry, biology and materials science, the ability to access interatomic interactions and their dynamical evolution has become possible with the advent of femtosecond lasers. In particular, the observation of vibrational wave packets via optical (UV-visible-IR) spectroscopies has been a major achievement as it can track the motion of nuclei within the system. However, optical spectroscopies only detect the effect of the interatomic vibrations on the global electronic surfaces. New tuneable, pulsed and polarized sources of short-wavelength radiation, such as X-Ray Free electron lasers, can overcome this limitation, allowing for chemical and, of primary importance in biochemistry, enantiomeric selectivity. This selectivity may be complemented by taking into account the chemical shifts of atoms belonging to different molecular moieties

While chiral spin structures stabilized by Dzyaloshinskii-Moriya interaction (DMI) are candidates as novel information carriers, their dynamics on the fs-ps timescale is little known. Since with the bulk Heisenberg exchange and the interfacial DMI two distinct exchange mechanisms are at play, the ultra-fast dynamics of the chiral order needs to be ascertained and compared to the dynamics of the conventional collinear order. Using an XUV free-electron laser we determine the fs-ps temporal evolution of the chiral order in domain walls in a magnetic thin film sample by an IR pump - X-ray magnetic scattering probe experiment. Upon demagnetisation we observe that the dichroic (CL-CR) signal connected with the chiral order correlator $m_z m_x$ in the domain walls recovers significantly faster than the (CL+CR) sum signal representing the average collinear domain magnetisation $m_z^2 + m_x^2$. We explore possible explanations based on spin structure dynamics and reduced transversal magnetisation fluctuations inside the domain walls and find that the latter can explain the experimental data leading to different dynamics for collinear magnetic order and chiral magnetic order., 28 pages, 14 figures

In many experimental facilities there is a rising interest by users and beamline scientists to take part in the experiment control software development process. This necessity arises from the flexibility and adaptability of many beamlines, that can run very different experiments, requiring changes in the software even during beamtimes. On the other side, we still need a professional and controlled approach in order to be able to maintain the software efficiently. Our proposed solution is to exploit the object oriented nature of programming languages to create a library that provides a uniform interface both to the different controlled devices (e.g. motors) and to experimental procedures (e.g. scans). Every component and procedure can be represented as an object, a building block for experiment control scripts. We can thus provide the scientists with a powerful tool for implementing highly flexible control software to run experiments. Furthermore, a library makes the development of experiment control scripts easier and quicker for software developers. In any case we are able to protect the most sensitive structures (e.g. control systems) beneath a strong and trusted software layer., Proceedings of the 17th International Conference on Accelerator and Large Experimental Physics Control Systems, ICALEPCS2019, New York, NY, USA

Non-collinear spin textures in ferromagnetic ultrathin films are attracting a renewed interest fueled by possible fine engineering of several magnetic interactions, notably the interfacial Dzyaloshinskii-Moriya interaction. This allows the stabilization of complex chiral spin textures such as chiral magnetic domain walls (DWs), spin spirals, and magnetic skyrmions. We report here on the ultrafast behavior of chiral DWs after optical pumping in perpendicularly magnetized asymmetric multilayers, probed using time-resolved circular dichroism in x-ray resonant magnetic scattering (CD-XRMS). We observe a picosecond transient reduction of the CD-XRMS, which is attributed to the spin current-induced coherent and incoherent torques within the continuously dependent spin texture of the DWs. We argue that a specific demagnetization of the inner structure of the DW induces a flow of hot spins from the interior of the neighboring magnetic domains. We identify this time-varying change of the DW textures shortly after the laser pulse as a distortion of the homochiral N'eel shape toward a transient mixed Bloch-N��el-Bloch textures along a direction transverse to the DW. Our study highlights how time-resolved CD-XRMS can be a unique tool for studying the time evolution in other systems showing a non-collinear electric/magnetic ordering such as skyrmion lattices, conical/helical phases, as well as the recently observed antiskyrmion lattices, in metallic or insulating materials.

We report on ultrafast magnetisation dynamics in ferro-magnetic cobalt/platinum multilayers upon pumping by near and mid to far infrared radiation, utilizing sub-100 femtosecond free-electron laser pulses. The evolution of the excited magnetic state is studied on femtosecond timescales with nanometre spatial resolution and element selectivity, employing time-resolved magnetic small-angle X-ray scattering. The obtained results contribute to the ongoing discussion to what extent either coupling of the electromagnetic field or rather quasi-instantaneous heating of the electron-system is the driving force for phenomena like ultrafast demagnetization or all-optical helicity-dependent switching., Proceedings of the 39th Free Electron Laser Conference, FEL2019, Hamburg, Germany

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., Two-colour X-ray free electron laser is a powerful tool for pump–probe measurements, but currently constrained by limited tunability. Here, Ferrari et al. develop a configuration that allows tuning both the pump and the probe to specific electronic excitations, providing element selectivity.

It has been suggested that the extended intensity profiles surrounding Bragg reflections that arise when a series of finite crystals of varying size and shape are illuminated by the intense, coherent illumination of an x-ray free-electron laser may enable the crystal’s unit-cell electron density to be obtained ab initio via well-established iterative phasing algorithms. Such a technique could have a significant impact on the field of biological structure determination since it avoids the need for a priori information from similar known structures, multiple measurements near resonant atomic absorption energies, isomorphic derivative crystals, or atomic-resolution data. Here, we demonstrate this phasing technique on diffraction patterns recorded from artificial two-dimensional microcrystals using the seeded soft x-ray free-electron laser FERMI. We show that the technique is effective when the illuminating wavefront has nonuniform phase and amplitude, and when the diffraction intensities cannot be measured uniformly throughout reciprocal space because of a limited signal-to-noise ratio.

FERMI is the seeded FEL user facility in Trieste, Italy, producing photons from the VUV to the soft X-rays with a high degree of coherence and spectral stability. Both FEL lines, FEL-1 and FEL-2, are available for users, down to the shortest wavelength of 4 nm. We report on the completion of the commissioning of the high energy FEL line, FEL-2, on the most recent progress obtained on FEL-1 and on the operational experience for users, in particular those requiring specific FEL configurations, such as two-colour experiments. We will also give a perspective on the improvements and upgrades which have been triggered based on our experience, aiming to maintain as well as to constantly improve the performance of the facility for our user community., Proceedings of the 37th International Free Electron Laser Conference, FEL2015, Daejeon, Republic of Korea

The quantum efficiency (QE) of Cu(111) is measured for different impinging light angles with photon energies just above the work function. We observe that the vectorial photoelectric effect, an enhancement of the QE due to illumination with light with an electric vector perpendicular to the sample surface, is stronger in the more surface sensitive regime. This can be explained by a contribution to photoemission due to the variation in the electromagnetic potential at the surface. The contributions of bulk and surface electrons can then be determined.

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements, where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Here, we report on an experiment using a dedicated optical element and the two-color emission of the FERMI XUV free-electron laser to follow the charge and spin dynamics in composite materials at two distinct absorption edges, simultaneously. The sample, consisting of ferromagnetic Fe and Ni layers, separated by a Cu layer, is pumped by an infrared laser and probed by a two-color XUV pulse with photon energies tuned to the M-shell resonances of these two transition metals. The experimental geometry intrinsically avoids any timing uncertainty between the two elements and unambiguously reveals an approximately 100 fs delay of the magnetic response with respect to the electronic excitation for both Fe and Ni. This delay shows that the electronic and spin degrees of freedom are decoupled during the demagnetization process. We furthermore observe that the electronic dynamics of Ni and Fe show pronounced differences when probed at their resonance, while the demagnetization dynamics are similar. These observations underline the importance of simultaneous investigation of the temporal response of both charge and spin in multi-component materials. In a more general scenario, the experimental approach can be extended to continuous energy ranges, promising the development of jitter-free transient absorption spectroscopy in the XUV and soft X-ray regimes.

Scientific reports 11(1), 5203 (1-10) (2021). doi:10.1038/s41598-021-84677-w, Spatially encoded measurements of transient optical transmissivity became a standard tool for temporal diagnostics of free-electron-laser (FEL) pulses, as well as for the arrival time measurements in X-ray pump and optical probe experiments. The modern experimental techniques can measure changes in optical coefficients with a temporal resolution better than 10 fs. This, in an ideal case, would imply a similar resolution for the temporal pulse properties and the arrival time jitter between the FEL and optical laser pulses. However, carrier transport within the material and out of its surface, as well as carrier recombination may, in addition, significantly decrease the number of carriers. This would strongly affect the transient optical properties, making the diagnostic measurement inaccurate. Below we analyze in detail the effects of those processes on the optical properties of XUV and soft X-ray irradiated Si$_3$N$_4$, on sub-picosecond timescales. Si$_3$N$_4$ is a wide-gap insulating material widely used for FEL pulse diagnostics. Theoretical predictions are compared with the published results of two experiments at FERMI and LCLS facilities, and with our own recent measurement. The comparison indicates that three body Auger recombination strongly affects the optical response of Si$_3$N$_4$ after its collisional ionization stops. By deconvolving the contribution of Auger recombination, in future applications one could regain a high temporal resolution for the reconstruction of the FEL pulse properties measured with a Si$_3$N$_4$-based diagnostics tool., Published by Macmillan Publishers Limited, part of Springer Nature, [London]

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 alpha- and beta-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 alpha-beta 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 alpha-beta stripes that occurs at two characteristic timescales in the range of similar to 10(-12) and similar to 10(-10) s. 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.

Physical review letters 127(1), 016802 (2021). doi:10.1103/PhysRevLett.127.016802, 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., Published by APS, College Park, Md.

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 similar to 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.

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. © 2016 International Union of Crystallography.

International audience; 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.

We report on new opportunities for ultrafast science thanks to the use of two-colour extreme ultraviolet (XUV) pulses at the FERMI free electron laser (FEL) facility. The two pulses have been employed to carry out a pioneering FEL-pump/FEL-probe diffraction experiment using a Ti target and tuning the FEL pulses to the M2/3-edge in order to explore the dependence of the dielectric constant on the excitation fluence. The future impact that the use of such a two-colour FEL emission will have on the development of ultrafast wave-mixing methods in the XUV/soft X-ray range is addressed and discussed.