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We utilize coherent femtosecond extreme ultraviolet (EUV) pulses derived from a free electron laser (FEL) to generate transient periodic magnetization patterns with periods as short as 44 nm. Combining spatially periodic excitation with resonant probing at the dichroic M-edge of cobalt allows us to create and probe transient gratings of electronic and magnetic excitations in a CoGd alloy. In a demagnetized sample, we observe an electronic excitation with 50 fs rise time close to the FEL pulse duration and ~0.5 ps decay time within the range for the electron-phonon relaxation in metals. When the experiment is performed on a sample magnetized to saturation in an external field, we observe a magnetization grating, which appears on a sub-picosecond time scale as the sample is demagnetized at the maxima of the EUV intensity and then decays on the time scale of tens of picoseconds via thermal diffusion. The described approach opens prospects for studying dynamics of ultrafast magnetic phenomena on nanometer length scales.

Physical review / A 105(5), 053524 (2022). doi:10.1103/PhysRevA.105.053524, The advent of free-electron lasers (FELs) in the soft- and hard-x-ray spectral regions has introduced the possibility to probe electronic, magnetic, and structural dynamics, in both diluted and condensed matter samples, with femtosecond time resolution. In particular, FELs have strongly enhanced the capabilities of several analytical techniques, which have taken advantage of the high degree of transverse coherence provided. Free-electron lasers based on the harmonic up-conversion of an external coherent source (seed) are characterized also by a high degree of longitudinal coherence, since electrons inherit the coherence properties of the seed. For the state of the art, the shortest wavelength delivered to user experiments by an externally seeded FEL light source is about 4 nm. In this paper we demonstrate 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. In order to show the suitability of the nonlinear harmonics generated by a seeded FEL for research in the water window and beyond, we report the results of two proof-of-principle experiments: one measuring the oxygen $K$-edge absorption in water (∼$530$ eV) and the other analyzing the spin dynamics of Fe and Co through magnetic small-angle x-ray scattering at their $L$ edges (707 and 780 eV, respectively)., Published by Inst., Woodbury, NY

Collective lattice dynamics determine essential aspects of condensed matter, such as elastic and thermal properties. These exhibit strong dependence on the length-scale, reflecting the marked wavevector dependence of lattice excitations. The extreme ultraviolet transient grating (EUV TG) approach has demonstrated the potential of accessing a wavevector range corresponding to the 10s of nm length-scale, representing a spatial scale of the highest relevance for fundamental physics and forefront technology, previously inaccessible by optical TG and other inelastic scattering methods. In this manuscript we report on the capabilities of this technique in the context of probing thermoelastic properties of matter, both in the bulk and at the surface, as well as discussing future developments and practical considerations.

In recent years, femtosecond extreme-ultraviolet (XUV) and x-ray pulses from free-electron lasers have developed into important probes to monitor processes and dynamics in matter on femtosecond-time and angstrom-length scales. With the rapid progress of versatile ultrafast x-ray spectroscopy techniques and more sophisticated data analysis tools, accurate single-pulse information on the arrival time, duration, and shape of the probing x-ray and XUV pulses becomes essential. Here, we demonstrate that XUV pulses can be converted into terahertz electromagnetic pulses using a spintronic terahertz emitter. We observe that the duration, arrival time, and energy of each individual XUV pulse is encoded in the waveform of the associated terahertz pulses, and thus can be readily deduced from single-shot terahertz time-domain detection.

Charge transport processes at interfaces play a crucial role in many processes. Here, the first soft x-ray second harmonic generation (SXR SHG) interfacial spectrum of a buried interface (boron-Parylene N) is reported. SXR SHG shows distinct spectral features that are not observed in x-ray absorption spectra, demonstrating its extraordinary interfacial sensitivity. Comparison to electronic structure calculations indicates a boron-organic separation distance of 1.9Å, with changes of less than 1Å resulting in easily detectable SXR SHG spectral shifts (ca. hundreds of milli-electron volts).

The advent of extreme ultraviolet (EUV) and soft x-ray free electron lasers (FELs) has enabled nonlinear optical experiments at wavelengths shorter than the visible-UV range. An important class of experiments is those based on the four-wave-mixing (FWM) approach, which are often based on interactions between pulses at different wavelengths. The exploitation of multiple EUV/soft x-ray wavelengths is not straightforward, but it can significantly expand the range of applications. In this manuscript we report on an experimental approach, based on the concomitant use of a non-collinear split-delay-and-recombination unit (“mini-Timer”) and on a two-color seeded FEL emission scheme (“twin-seed mode”). We used a diamond sample for demonstrating the capability of this setup of generating and detecting a FWM signal stimulated by two-color EUV FEL pulses. This approach can be further exploited for developing experimental methods based on non-linear EUV/x-ray optics.

Understanding and controlling the thermal transport at nanoscale is a key ingredient for the development of future nanoelectronical devices. In this study of thin silicon carbide (SiC) membrane we demonstrate the potential of free electron laser extreme ultraviolet (EUV) transient grating (TG) technique as contactless probe for thermoelastic response at length scales of 84 nm, where the Fourier heat diffusion law is no longer valid. The results have revealed that the mechanical behavior of the system can be fully described in the framework of Lamb waves. Moreover, by use of a bidimensional spatial detector to measure the TG signal, a new feature is the observed, time dependence in the emission angle of the transient diffraction, correlated to the transient grating signal intensity.

The development of ultra-bright extreme ultraviolet (EUV) and X-ray free electron laser (FEL) sources has enabled the extension of wave-mixing approaches into the short wavelength regime. Such a class of experiments relies upon nonlinear interactions among multiple light pulses offering a unique tool for exploring the dynamics of ultrafast processes and correlations between selected excitations at relevant length and time scales adding elemental and site selectivity as well. Besides the availability of a suitable photon source, the implementation of wave mixing methodology requires efforts in developing the instrumental set-up. We have realized at the FERMI FEL two dedicated set-ups to handle multiple FEL beams with preselected parameters in a non-collinear fashion and control their interaction sequence at the target. These unique apparatuses, combined with the exceptional characteristics of the seeded FERMI FEL, have allowed us to make the first steps into this field and further advances are foreseen in the near future.

A liquid carbon ($l$-C) sample is generated through constant volume heating exposing an amorphous carbon foil to an intense ultrashort laser pulse. Time-resolved x-ray absorption spectroscopy at the C $K$ edge is used to monitor the dynamics of the melting process revealing a subpicosecond rearrangement of the electronic structure associated with a sudden change of the C bonding hybridization. The obtained $l$-C sample, resulting from a nonthermal melting mechanism, reaches a transient equilibrium condition with a temperature of about 14 200 K and pressure in the order of 0.5 Mbar in about 0.3 ps, prior to hydrodynamic expansion. A detailed analysis of the atomic and electronic structure in solid-density $l$-C based on time-resolved x-ray absorption spectroscopy and theoretical simulations is presented. The method can be fruitfully used for extending the experimental investigation of the C phase diagram in a vast unexplored region covering the ${10}^{3}--{10}^{4}\text{ }\text{ }\mathrm{K}$ temperature range with pressures up to 1 Mbar.

We demonstrate an all-optical approach for measuring spectrograms of individual FEL pulses by measuring a spectrally-resolved EUV-EUV-optical four-wave-mixing signal. We experimentally demonstrate that this is phase-sensitive can be applied to structured and unstable pulse trains.

The rapid development of extreme ultraviolet (EUV) and x-ray ultrafast coherent light sources such as free electron lasers (FELs) has triggered the extension of wave-mixing techniques to short wavelengths. This class of experiments, based on the interaction of matter with multiple light pulses through the Nth order susceptibility, holds the promise of combining intrinsic ultrafast time resolution and background-free signal detection with nanometer spatial resolution and chemical specificity. A successful approach in this direction has been the combination of the unique characteristics of the seeded FEL FERMI with dedicated four-wave-mixing (FWM) setups, which leads to the demonstration of EUV-based transient grating (TG) spectroscopy. In this perspective paper, we discuss how the TG approach can be extended toward more general FWM spectroscopies by exploring the intrinsic multiparameter nature of nonlinear processes, which derives from the ability of controlling the properties of each field independently.

Time-resolved transient grating (TG) spectroscopy facilitates detailed studies of electron dynamics and transport phenomena by means of a periodic excitation of matter with coherent ultrashort light pulses. Several current and next generation free-electron laser (FEL) facilities provide fully coherent pulses with few femtosecond pulse durations and extreme ultraviolet (XUV) photon energies. Thus, they allow for transient grating experiments with periodicities as small as tens of nanometers and with element specific photon energies. Here, we demonstrate the element specificity of XUV TG (X-TG) experiments by tuning the photon energy across the Si L2,3-edge of Si3N4. We observe a shortening of the signal decay when increasing the XUV photon energy above the absorption edge. The analysis of the wavelength dependent signal shows that the faster decay is driven by the increase in the charge carrier density. From the decay constants the interband Auger coefficient at elevated temperatures and high electron densities has been determined.Time-resolved transient grating (TG) spectroscopy facilitates detailed studies of electron dynamics and transport phenomena by means of a periodic excitation of matter with coherent ultrashort light pulses. Several current and next generation free-electron laser (FEL) facilities provide fully coherent pulses with few femtosecond pulse durations and extreme ultraviolet (XUV) photon energies. Thus, they allow for transient grating experiments with periodicities as small as tens of nanometers and with element specific photon energies. Here, we demonstrate the element specificity of XUV TG (X-TG) experiments by tuning the photon energy across the Si L2,3-edge of Si3N4. We observe a shortening of the signal decay when increasing the XUV photon energy above the absorption edge. The analysis of the wavelength dependent signal shows that the faster decay is driven by the increase in the charge carrier density. From the decay constants the interband Auger coefficient at elevated temperatures and high electron dens...

Recent advances in ultrafast extreme ultraviolet (EUV) and x-ray light sources provide direct access to fundamental time and length scales for biology, chemistry, and materials physics. However, such light pulses are challenging to measure due to the need for femtosecond time resolution at difficult-to-detect wavelengths. Also, single-shot measurements are needed because severe pulse-to-pulse fluctuations are common. Here we demonstrate single-shot, complete field measurements by applying a novel version of frequency resolved optical gating. An EUV free electron laser beam creates a transient grating containing the pulse’s electric field information, which is read out with a 400 nm probe pulse. By varying the time delay between two copies of the EUV pump, rather than between the pump and the probe, we separate the needed coherent wave mixing from the slow incoherent response. Because this approach uses photoionization, it should be applicable from the vacuum ultraviolet to hard x rays.

We hereby report on a set of transient optical reflectivity and transmissivity measurements performed on silicon nitride thin membranes excited by extreme ultraviolet (EUV) radiation from a free electron laser (FEL). Experimental data were acquired as a function of the membrane thickness, FEL fluence and probe polarization. The time dependence of the refractive index, retrieved using Jones matrix formalism, encodes the dynamics of electron and lattice excitation following the FEL interaction. The observed dynamics are interpreted in the framework of a two temperature model, which permits to extract the relevant time scales and magnitudes of the processes. We also found that in order to explain the experimental data thermo-optical effects and inter-band filling must be phenomenologically added to the model.

The extension of nonlinear optical techniques to the extreme-ultraviolet (EUV), soft and hard x-ray regime represents one of the open challenges of modern science since it would combine chemical specificity with background-free detection and ultrafast time resolution. We report on the first observation of a four-wave-mixing (FWM) response from solid-state samples stimulated exclusively by EUV pulses. The all-EUV FWM signal was generated by the diffraction of high-order harmonics of the FERMI free-electron laser (FEL) from the standing wave resulting from the interference of two crossed FEL pulses at the fundamental wavelength. From the intensity of the FWM signal, we are able to extract the first-ever estimate of an effective value of $\ensuremath{\sim}6\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}24}\text{ }\text{ }\text{ }{\mathrm{m}}^{2}\text{ }{\mathrm{V}}^{\ensuremath{-}2}$ for the third-order nonlinear susceptibility in the EUV regime. This proof of principle experiment represents a significant advance in the field of nonlinear optics and sets the starting point for a manifold of techniques, including frequency and phase-resolved FWM methods, that are unprecedented in this photon-energy regime.

Experimental approaches based on nonlinear optical processes (wave-mixing) have allowed major breakthroughs in diverse fields of science and technology. Nevertheless, these concepts were restricted to the optical regime due to the lack of coherent photon sources of sufficient peak brightness at sub-optical wavelengths. Nowadays, while the development of free electron lasers (FELs) potentially allows extreme ultraviolet (EUV) and X-ray wave-mixing, their full exploitation still requires efforts in instrumentation developments. The need to control (both in the spatial and temporal coordinates) multiple FEL input pulses, which may have different photon frequencies and polarizations, calls for the developments of instruments with a higher degree of complexity with respect to those typically used at synchrotron and FEL beamlines. Here we report on the progresses in the development of such kind of instrumentation at the FERMI FEL facility. Our FEL-based wave-mixing setups rely upon the transient grating (TG) approach, which represents a relevant benchmark for the development of advanced EUV/soft x-ray four-wave-mixing (FWM) experiments, as for instance coherent Raman scattering and multi-dimensional spectroscopy. © 2018 Elsevier B.V.

© 2018 American Physical Society. Nonlinear optical processes at soft x-ray wavelengths have remained largely unexplored due to the lack of available light sources with the requisite intensity and coherence. Here we report the observation of soft x-ray second harmonic generation near the carbon K edge (∼284 eV) in graphite thin films generated by high intensity, coherent soft x-ray pulses at the FERMI free electron laser. Our experimental results and accompanying first-principles theoretical analysis highlight the effect of resonant enhancement above the carbon K edge and show the technique to be interfacially sensitive in a centrosymmetric sample with second harmonic intensity arising primarily from the first atomic layer at the open surface. This technique and the associated theoretical framework demonstrate the ability to selectively probe interfaces, including those that are buried, with elemental specificity, providing a new tool for a range of scientific problems.

We have examined the transmission of soft X-ray pulses from the FERMI free electron laser through carbon films of varying thickness, quantifying nonlinear effects of pulses above and below the carbon K-edge. At typical of soft X-ray free electron laser intensities, pulses exhibit linear absorption at photon energies above and below the K-edge, ∼308 and ∼260 eV, respectively; whereas two-photon absorption becomes significant slightly below the K-edge, ∼284.2 eV. The measured two-photon absorption cross section at 284.18 eV (∼6 × 10−48 cm4 s) is 7 orders of magnitude above what is expected from a simple theory based on hydrogen-like atoms – a result of resonance effects.

The characterization of the time structure of ultrafast photon pulses in the extreme-ultraviolet (EUV) and soft X-ray spectral ranges is of high relevance for a number of scientific applications and photon diagnostics. Such measurements can be performed following different strategies and often require large setups and rather high pulse energies. Here, high-quality measurements carried out by exploiting the transient grating process, i.e. a third-order non-linear process sensitive to the time-overlap between two crossed EUV pulses, is reported. From such measurements it is possible to obtain information on both the second-order intensity autocorrelation function and on the coherence length of the pulses. It was found that the pulse energy density needed to carry out such measurements on solid state samples can be as low as a few mJ cm−2. Furthermore, the possibility to control the arrival time of the crossed pulses independently might permit the development of a number of coherent spectroscopies in the EUV and soft X-ray regime, such as, for example, photon echo and two-dimensional spectroscopy.

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.A description of the novel timing methodologies developed at the FERMI FEL facility is given.

The use of lasers to generate acoustic waves revolutionized the field of ultrasound and enabled numerous key developments in both fundamental research and applications. In the past decade, remarkable progress has been achieved in developing coherent sources of radiation operating in the extreme ultraviolet (EUV) and x-ray ranges, such as free electron lasers, which already yielded many breakthroughs in different fields of science. We expect that the field of ultrasonics will also greatly benefit from the availability of coherent EUV and x-ray sources. So far, a number of studies explored the use of coherent EUV and x-ray radiation for detection of acoustic waves. In this report, we describe the first experiment on the generation of surface and bulk acoustic waves in the tens of GHz range by EUV light.

Revealing the structure of complex biological macromolecules, such as proteins, is an essential step for understanding the chemical mechanisms that determine the diversity of their functions. Synchrotron based X-ray crystallography and cryo-electron microscopy have made major contributions in determining thousands of protein structures even from micro-sized crystals. They suffer from some limitations that have not been overcome, such as radiation damage, the natural inability to crystallize a number of proteins, and experimental conditions for structure determination that are incompatible with the physiological environment. Today, the ultra-short and ultra-bright pulses of X-ray free-electron lasers have made attainable the dream to determine protein structures before radiation damage starts to destroy the samples. However, the signal-to-noise ratio remains a great challenge to obtain usable diffraction patterns from a single protein molecule. With the perspective to overcome these challenges, we describe here a new methodology that has the potential to overcome the signal-to-noise-ratio and protein crystallization limits. Using a multidisciplinary approach, we propose to create ordered, two dimensional protein arrays with defined orientation attached on a self-assembled-monolayer. We develop a literature-based flexible toolbox capable of assembling different kinds of proteins on a functionalized surface and consider using a graphene cover layer that will allow performing experiments with proteins in physiological conditions.

Conference on X-Ray Lasers and Coherent X-ray Sources - Development and Applications, Prague, CZECH REPUBLIC, APR 24-26, 2017; International audience; Stimulated emission is a fundamental process in nature that deserves to be investigated and understood in the EUV and X-ray regimes. Today this is definitely possible through high energy density FEL beams. In this context, we show evidence for soft x-ray stimulated emission from a MgO solid target pumped by extreme ultraviolet FEL pulses formed in the regime of travelling-wave amplified spontaneous emission in backward geometry. Our results combine two effects separately reported in previous works: emission in a privileged direction and existence of a material-dependent threshold, for the stimulated emission. We have developed a theoretical framework, based on coupled rate and transport equations taking into account the solid density plasma state of the target. Our model, accounts for both observed mechanisms that are the privileged direction for the stimulated emission of the Mg L-2,L-3 characteristic emission and the pumping threshold.

Among the fourth-generation light sources, the Italian free-electron laser (FEL) FERMI is the only one operating in the high-gain harmonic generation (HGHG) seeding mode. FERMI delivers pulses characterized by a quasi transform limited temporal structure, photon energies lying in the extreme ultra-violet (EUV) region, supreme transversal and longitudinal coherences, high peak brilliance, and full control of the polarization. Such state of the art performances recently opened the doors to a new class of time-resolved spectroscopies, difficult or even impossible to be performed using self-amplified spontaneous sources (SASE) light sources. FERMI is currently equipped with three operating beamlines opened to external users (DiProI, LDM and EIS), while two more are under commissioning (MagneDYN and TeraFERMI). Here, we present the recent highlights of the EIS (Elastic and Inelastic Scattering) beamline, which has been purposely designed to take full advantage from the coherence, the intensity, the harmonics content, and the temporal duration of the pulses. EIS is a flexible experimental facility for time-resolved EUV scattering experiments on condensed matter systems, consisting of two independent end-stations. The first one (EIS-TIMEX) aims to study materials in metastable and warm dense matter (WDM) conditions, while the second end-station (EIS-TIMER) is fully oriented to the extension of four-wave mixing (FWM) spectroscopies towards the EUV spectral regions, trying to reveal the behavior of matter in portions of the mesoscopic regime of exchanged momentum impossible to be probed using conventional light sources.

Extreme-ultraviolet vortices may be exploited to steer the magnetic properties of nanoparticles, increase the resolution in microscopy, and gain insight into local symmetry and chirality of a material; they might even be used to increase the bandwidth in long-distance space communications. However, in contrast to the generation of vortex beams in the infrared and visible spectral regions, production of intense, extreme-ultraviolet and x-ray optical vortices still remains a challenge. Here, we present an in-situ and an ex-situ technique for generating intense, femtosecond, coherent optical vortices at a free-electron laser in the extreme ultraviolet. The first method takes advantage of nonlinear harmonic generation in a helical undulator, producing vortex beams at the second harmonic without the need for additional optical elements, while the latter one relies on the use of a spiral zone plate to generate a focused, micron-size optical vortex with a peak intensity approaching 10^{14} W/cm^{2}, paving the way to nonlinear optical experiments with vortex beams at short wavelengths.

The full comprehension of magnetic phenomena at the femtosecond (fs) time scale is of high demand for current material science and technology. Here we report the observation of coherent collective modes in the antiferromagnetic insulator nickel oxide (NiO) identified by a frequency of 0.86 THz, which matches the expected out-of-plane single-mode magnon resonance. Such collective excitations are inelastically stimulated by extreme ultraviolet (EUV) pulses delivered by a seeded free-electron laser (FEL) and subsequently revealed probing the transient optical activity of NiO looking at the Faraday effect. Moreover, the unique capability of the employed FEL source to deliver circularly polarized pulses allows us to demonstrate optomagnetic control of such collective modes at EUV photon energies. These results may set a starting point for future investigations of magnetic materials at time scales comparable or faster than those typical of exchange interactions.

Scientific reports 6, 38796 (2016). doi:10.1038/srep38796, In the past few years, we have been witnessing an increased interest for studying materials properties under non-equilibrium conditions. Several well established spectroscopies for experiments in the energy domain have been successfully adapted to the time domain with sub-picosecond time resolution. Here we show the realization of high resolution resonant inelastic X-ray scattering (RIXS) with a stable ultrashort X-ray source such as an externally seeded free electron laser (FEL). We have designed and constructed a RIXS experimental endstation that allowed us to successfully measure the d-d excitations in KCoF3 single crystals at the cobalt M$_{2,3}$-edge at FERMI FEL (Elettra-Sincrotrone Trieste, Italy). The FEL-RIXS spectra show an excellent agreement with the ones obtained from the same samples at the MERIXS endstation of the MERLIN beamline at the Advanced Light Source storage ring (Berkeley, USA). We established experimental protocols for performing time resolved RIXS experiments at a FEL source to avoid X ray-induced sample damage, while retaining comparable acquisition time to the synchrotron based measurements. Finally, we measured and modelled the influence of the FEL mixed electromagnetic modes, also present in externally seeded FELs, and the beam transport with ~120 meV experimental resolution achieved in the presented RIXS setup., Published by Nature Publishing Group, London

Free-electron lasers (FELs) currently represent a step forward on time-resolved investigations on any phase of matter through pump-probe methods involving FELs and laser beams. That class of experiments requires an accurate spatial and temporal superposition of pump and probe beams on the sample, which at present is still a critical procedure. More efficient approaches are demanded to quickly achieve the superposition and synchronization of the beams. Here, we present what we believe is a novel technique based on an integrated device allowing the simultaneous characterization and the fast spatial and temporal overlapping of the beams, reducing the alignment procedure from hours to minutes. (C) 2016 Optical Society of America

The development of free electron laser (FEL) sources has provided an unprecedented bridge between the scientific communities working with ultrafast lasers and extreme ultraviolet (XUV) and X-ray radiation. Indeed, in recent years an increasing number of FEL-based applications have exploited methods and concepts typical of advanced optical approaches. In this context, we recently used a seeded FEL to demonstrate a four-wave-mixing (FWM) process stimulated by coherent XUV radiation, namely the XUV transient grating (X-TG). We hereby report on X-TG measurements carried out on a sample of silicon nitride (Si3N4). The recorded data bears evidence for two distinct signal decay mechanisms: one occurring on a sub-ps timescale and one following slower dynamics extending throughout and beyond the probed timescale range (100 ps). The latter is compatible with a slower relaxation (time decay > ns), that may be interpreted as the signature of thermal diffusion modes. From the peak intensity of the X-TG signal we could estimate a value of the effective third-order susceptibility which is substantially larger than that found in SiO2, so far the only sample with available X-TG data. Furthermore, the intensity of the time-coincidence peak shows a linear dependence on the intensity of the three input beams, indicating that the measurements were performed in the weak field regime. However, the timescale of the ultrafast relaxation exhibits a dependence on the intensity of the XUV radiation. We interpreted the observed behaviour as the generation of a population grating of free-electrons and holes that, on the sub-ps timescale, relaxes to generate lattice excitations. The background free detection inherent to the X-TG approach allowed the determination of FEL-induced electron dynamics with a sensitivity largely exceeding that of transient reflectivity and transmissivity measurements, usually employed for this purpose. This journal is © The Royal Society of Chemistry.

In this manuscript we report on a compact experimental set-up (“mini-TIMER”) conceived for transient grating (TG) experiments based on free electron laser (FEL) radiation. This set-up has been tested at the seeded FEL facility FERMI (Elettra, Trieste, Italy) and allowed us to observe the first FEL-stimulated TG signal. This experimental result is of the greatest relevance in the context of developing coherent non-linear optical methods into the extreme ultraviolet (EUV) and soft X-ray (SXR) range. Such a challenging task will be addressed in the next future at FERMI by using the present set-up and the forthcoming EIS-TIMER beamline, which is being installed at FERMI and will start the commissioning phase in the second semester 2015. The possibility to use TGs generated by FEL radiation at sub-optical wavelengths would allow developing EUV/SXR four-wave-mixing (FWM) applications, so far considered only theoretically and widely believed to be potentially able to provide major breakthroughs in several fields of science.

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.

FERMI is the first user dedicated seeded free-electron-laser (FEL) working in the extreme ultraviolet (XUV) and soft x-ray range. The EIS-TIMEX experimental end-station was availabe to external users since from the beginning of the user operation of the facility, in Dicember 2012. EIS-TIMEX has been conceived to exploit the unique properties of the FERMI source to study matter under extreme and metastable thermodynamic conditions. We hereby report on its basic parameters and applications, which includes very low jitter (i.e., high time resolution) pump-probe measurements.

X-ray/optical cross-correlation methods are attracting increasing interest for exploring transient states of matter using ultrashort free-electron laser (FEL) pulses. Our paper shows that in such studies the difference in the penetration depth of the FEL-pump and the infrared (IR) probe pulses become important, in particular, when exploring the changes in the optical properties of solid targets. We discuss the role of interference effects, using a phenomenological model with excited and unperturbed slabs. The reliability of this model was experimentally verified by measuring the transient optical response of free-standing and silicon (Si) supported silicon nitride (Si3N4) films, simultaneously in reflection and transmission, using s- and p-polarized IR light. The changes in the Si3N4 optical refractive index, induced by the FEL pulses, have fully been described in the frame of the proposed model. The experimental results confirm that the differences, observed in the FEL-induced transient reflectance and transmittance of the Si3N4 targets with different thicknesses, arise from multilayer-like interferometric phenomena.

We interpreted the recent construction of free electron laser (FELs) facilities worldwide as an unprecedented opportunity to bring concepts and methods from the scientific community working with optical lasers into the domain of x-ray science. This motivated our efforts towards the realization of FEL-based wave-mixing applications. In this article we present new extreme ultraviolet transient grating (X-TG) data from vitreous SiO2, collected using two crossed FEL pulses (photon frequency 38 eV) to generate the X-TG and a phase matched optical probing pulse (photon frequency 3.1 eV). This experiment extends our previous investigation, which was carried out on a nominally identical sample using a different FEL photon frequency (45 eV) to excite the X-TG. The present data are featured by a peak intensity of the X-TG signal substantially larger than that previously reported and by slower modulations of the X-TG signal at positive delays. These differences could be ascribed to the different FEL photon energy used in the two experiments or to differences in the sample properties. A systematic X-TG study on the same sample as a function of the FEL wavelength is needed to draw a consistent conclusion. We also discuss how the advances in the performance of the FELs, in terms of generation of fully coherent photon pulses and multi-color FEL emission, may push the development of original experimental strategies to study matter at the femtosecond-nanometer time-length scales, with the unique option of element and chemical state specificity. This would allow the development of advanced experimental tools based on wave-mixing processes, which may have a tremendous impact in the study of a large array of phenomena, ranging from nano-dynamics in complex materials to charge and energy transfer processes.

X-ray free electron lasers (FEL) coupled with optical lasers have opened unprecedented opportunities for studying ultrafast dynamics in matter. The major challenge in pump-probe experiments using FEL and optical lasers is synchronizing the arrival time of the two pulses. Here we report a technique that benefits from the seeded-FEL scheme and uses the optical seed laser for nearly jitter-free pump-probe experiments. Timing jitter as small as 6 fs has been achieved and confirmed by measurements of FEL-induced transient reflectivity changes of Si3N4 using both collinear and non-collinear geometries. Planned improvements of the experimental set-up are expected to further reduce the timing jitter between the two pulses down to fs level.