Search

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.

Expanding the activity of wide bandgap semiconductors from the UV into the visible range has become a central goal for their application in green solar photocatalysis. The hybrid plasmonic/semiconductor system, based on silver nanoparticles (Ag NPs) embedded in a film of CeO2, is an example of a functional material developed with this aim. In this work, we take advantage of the chemical sensitivity of free electron laser (FEL) time-resolved soft X-ray absorption spectroscopy (TRXAS) to investigate the electron transfer process from the Ag NPs to the CeO2 film generated by the NPs plasmonic resonance photoexcitation. Ultrafast changes (

We use femtosecond extreme ultraviolet pulses derived from a free electron laser to excite and probe surface acoustic waves (SAWs) on the (001) surface of single crystal SrTiO3. SAWs are generated by a pair of 39.9 nm pulses crossed at the sample with the crossing angle defining the SAW wavelength at 84 nm. Detection of SAWs is performed via diffraction of a time-delayed 13.3 nm probe pulse by SAW-induced surface ripples. Despite the low reflectivity of the sample in the extreme ultraviolet range, the reflection mode detection is found to be efficient because of an increase in the diffraction efficiency for shorter wavelengths. We describe a methodology for extracting the SAW attenuation in the presence of a thermal grating, which is based on measuring the decay of oscillations at twice the SAW frequency. The proposed approach can be used to study ultrahigh frequency SAWs in a broad range of materials and will bridge the wave vector gap in surface phonon spectroscopy between Brillouin scattering and He atom scattering.

Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We demonstrate for the first time TG excitation in the hard X-ray range at 7.1 keV. In Bismuth Germanate (BGO), the nonresonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods., Comment: 11 pages, 4 figures

Ultrafast time-resolved extreme ultraviolet (EUV) reflectivity measurements of optically pumped amorphous carbon (a-C) have been performed with the FERMI free electron laser (FEL). This work extends the energy range used in previous reflectivity studies and adds polarization dependence. The EUV probe is known to be sensitive to lattice dynamics, since in this range the reflectivity is essentially unaffected by the photo-excited surface plasma. The exploitation of both s- and p-polarized EUV radiation permits variation of the penetration depth of the probe; a significant increase in the characteristic time is observed upon increasing the probing depth (1 vs. 5 ps) due to hydrodynamic expansion and consequent destruction of the excited region, implying that there is only a short window during which the probed region is in the isochoric regime. A weak wavelength dependence of the reflectivity is found, consistent with previous measurements and implying a maximum electronic temperature of 0.8 eV ± 0.4.

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.

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.

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.

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

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.

We investigate the excitation of coherent acoustic and optical phonons by ultrashort extreme ultraviolet (EUV) pulses produced by a free electron laser. Two crossed femtosecond EUV (wavelength 12.7 nm) pulses are used to excite coherent phonons at a wavelength of 280 nm, which are detected via diffraction of an optical probe beam. Longitudinal and surface acoustic waves are measured in BK-7 glass, diamond, and Bi4Ge3O12; in the latter material, the excitation of a coherent optical phonon mode is also observed. We discuss probing different acoustic modes in reflection and transmission geometries and frequency mixing of surface and bulk acoustic waves in the signal. The use of extreme ultraviolet radiation will allow the creation of tunable GHz to THz acoustic sources in any material without the need to fabricate transducer structures. The contribution by the MIT group was supported by the U.S. Department of Energy, Office of Basic Energy Sciences under Award No. DE-FG02-00ER15087. The JILA group graciously acknowledges support from the Department of Energy BES Award No. DE-FG02-99ER14982 and the Gordon and Betty Moore Foundation's EPiQS Initiative through Grant No. GBMF: 4538, and J.K. acknowledges support from an SRC Fellowship. The Elettra group acknowledges the European Research Council Grant No. 202804-TIMER. A.C. and T.F. acknowledge the Swiss NSF through the NCCR-MUST.

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.

The development of free electron laser (FEL) sources, which provide extreme ultraviolet (XUV) and soft x-ray radiation of unprecedented coherence and almost transform-limited pulse structure, has opened up the realm of XUV/x-ray non-linear optics. In particular, XUV four-wave-mixing (XFWM) experiments may allow, e.g., to probe correlations among low-energy excitations and core states, and to access the "mesoscopic" wavevector range (0.1-1 nm-1), inaccessible so far and fundamental to investigate nanostructures and disordered systems. In this manuscript we report on the latest advances and future developments of the TIMER setup at FERMI (Elettra, Italy), specifically conceived for XFWM experiments. In particular, we discuss the improvements on the XUV-probe and on the pump transport. Moreover, TIMER and mini-TIMER (a test setup available at the DiProI end station) are also suitable for time-resolved second order nonlinear experiments, which are intrinsically surface sensitive due to symmetry restrictions. We hereby discuss the foreseen extension to the XUV of interface specific probing of electronic processes, for example charge and energy transfer, with chemical specificity.

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.

Time resolved extreme ultraviolet (EUV) transient reflectivity measurements on non-equilibrium amorphous carbon (a-C) have been carried out by combining optical and free electron laser (FEL) sources. The EUV probing was specifically sensitive to lattice dynamics, since the EUV reflectivity is essentially unaffected by the photo-excited surface plasma. Data have been interpreted in terms of the dynamics of an expanding surface, i.e., a density gradient rapidly forming along the normal surface. This allowed us to determine the characteristic time ( τ ≲ 1 ps) for hydrodynamic expansion in photo-excited a-C. This finding suggests an extremely narrow time window during which the system can be assumed to be in the isochoric regime, a situation that may complicate the study of photo-induced metastable phases of carbon. Data also showed a weak dependence on the probing EUV wavelength, which was used to estimate the electronic temperature ( T e ≈ 0.8 eV) of the excited sample. This experimental finding compares fairly well with the results of calculations, while a comparison of our data and calculations with previous transient optical reflectivity measurements highlights the complementarities between optical and EUV probing.