Four wave mixing (FWM) processes, based on third-order non-linear light-matter interactions, can combine ultrafast time resolution with energy and wavevector selectivity, and enables to explore dynamics inaccessible by linear methods. [1][2][3][4][5][6][7] The coherent and multi-wave nature of FWM approach has been crucial in the development of cutting edge technologies, such as silicon photonics, 8 sub-wavelength imaging 9 and quantum communications. 10 All these technologies operate with optical wavelengths, which limit the spatial resolution and do not allow probing excitations with energy in the eV range. The extension to shorter wavelengths, that is the extreme ultraviolet (EUV) and soft-x-ray (SXR) range, will allow to improve the spatial resolution and to expand the excitation energy range, as well as to achieve elemental selectivity by exploiting core resonances. [5][6][7][11][12][13][14] So far FWM applications at these wavelengths have been prevented by the absence of coherent sources of sufficient brightness and suitable experimental setups. Our results show how transient gratings, generated by the interference of coherent EUV pulses delivered by the FERMI free electron laser (FEL), 15 can be used to stimulate FWM processes at sub-optical wavelengths. Furthermore, we have demonstrated the possibility to read the time evolution of the FWM signal, which embodies the dynamics of coherent excitations as molecular vibrations. This result opens the perspective for FWM with nanometer spatial resolution and elemental selectivity,

Exploring the dynamics of matter driven to extreme non-equilibrium states by an intense ultrashort X-ray pulse is becoming reality, thanks to the advent of free-electron laser technology that allows development of different schemes for probing the response at variable time delay with a second pulse. Here we report the generation of two-colour extreme ultraviolet pulses of controlled wavelengths, intensity and timing by seeding of high-gain harmonic generation free-electron laser with multiple independent laser pulses. The potential of this new scheme is demonstrated by the time evolution of a titanium-grating diffraction pattern, tuning the two coherent pulses to the titanium M-resonance and varying their intensities. This reveals that an intense pulse induces abrupt pattern changes on a time scale shorter than hydrodynamic expansion and ablation. This result exemplifies the essential capabilities of the jitter-free multiple-colour free-electron laser pulse sequences to study evolving states of matter with element sensitivity.

International audienceThe 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

The pulse duration, and, more generally, the temporal intensity profile of free-electron laser (FEL)\ud pulses, is of utmost importance for exploring the new perspectives offered by FELs; it is a nontrivial\ud experimental parameter that needs to be characterized. We measured the pulse shape of an extreme\ud ultraviolet externally seeded FEL operating in high-gain harmonic generation mode. Two different methods\ud based on the cross-correlation of the FEL pulses with an external optical laser were used. The two methods,\ud one capable of single-shot performance, may both be implemented as online diagnostics in FEL facilities.\ud The measurements were carried out at the seeded FEL facility FERMI. The FEL temporal pulse\ud characteristics were measured and studied in a range of FEL wavelengths and machine settings, and they\ud were compared to the predictions of a theoretical model. The measurements allowed a direct observation of\ud the pulse lengthening and splitting at saturation, in agreement with the proposed theory

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FERMI@Elettra is a free electron-laser (FEL)-based user facility that, after two years of commissioning, started preliminary users' dedicated runs in 2011. At variance with other FEL user facilities, FERMI@Elettra has been designed to deliver improved spectral stability and longitudinal coherence. The adopted scheme, which uses an external laser to initiate the FEL process, has been demonstrated to be capable of generating FEL pulses close to the Fourier transform limit. We report on the first instance of FEL wavelength tuning, both in a narrow and in a large spectral range (fine-and coarse-tuning). We also report on two different experiments that have been performed exploiting such FEL tuning. We used fine-tuning to scan across the 1s-4p resonance in He atoms, at ≈23.74 eV (52.2 nm), detecting both UV-visible fluorescence (4p-2s, 400 nm) and EUV fluorescence (4p-1s, 52.2 nm). We used coarse-tuning to scan the M 4,5 absorption edge of Ge (∼29.5 eV) in the wavelength region 30-60 nm, measured in transmission geometry with a thermopile positioned on the rear side of a Ge thin foil.

Advances in developing ultrafast coherent sources operating at extreme ultraviolet (EUV) and x-ray wavelengths allow the extension of nonlinear optical techniques to shorter wavelengths. Here, we describe EUV transient grating spectroscopy, in which two crossed femtosecond EUV pulses produce spatially periodic nanoscale excitations in the sample and their dynamics is probed via diffraction of a third time-delayed EUV pulse. The use of radiation with wavelengths down to 13.3 nm allowed us to produce transient gratings with periods as short as 28 nm and observe thermal and coherent phonon dynamics in crystalline silicon and amorphous silicon nitride. This approach allows measurements of thermal transport on the ~10-nm scale, where the two samples show different heat transport regimes, and can be applied to study other phenomena showing nontrivial behaviors at the nanoscale, such as structural relaxations in complex liquids and ultrafast magnetic dynamics.

Ultrashort, coherent x-ray pulses of a free-electron laser are used to holographically image the magnetization dynamics within a magnetic domain pattern after creation of a localized excitation via an optical standing wave. We observe a spatially confined reduction of the magnetization within a couple of hundred femtoseconds followed by its slower recovery. Additionally, the experimental results show evidence of a spatial evolution of magnetization, which we attribute to ultrafast transport of nonequilibrium spin-polarized electrons for early times and to a fluence-dependent remagnetization rate for later times. DOI: 10.1103/PhysRevLett.112.217203 PACS numbers: 75.78.Jp, 42.40.Kw, 75.25.−j, 78.70.Ck Progress in the field of light-induced, ultrafast manipulation of magnetic order has recently led to all-optical, ultrafast magnetic switching [1][2][3] and to an increased control of its dynamics by designing tailored nanostructured samples [4][5][6][7] as well as by exploiting nanoscale magnetic inhomogeneities [8,9]. The influence of interfaces between different materials and magnetic domain boundaries has cast doubt on our theoretical understanding of the underlying fundamental mechanism responsible for femtosecond magnetization dynamics. The model explaining the ultrafast loss of magnetic order after optical excitation by (e.g., electron-phonon or impurity-mediated) spin-flip scattering events [10] has in part been challenged by an approach based on nonlocal superdiffusive spin transport [11]. In spite of their very different microscopic origins, both have been successful in explaining a wide range of experimental data, suggesting that both mechanisms play an important role and that their respective magnitudes depend on the specific experimental conditions [7]. More specifically, in the case of superdiffusive spin transport, energy-and spin-dependent electron lifetimes and velocities induce spin-polarized currents, leading to significant ultrafast spatial rearrangement of magnetic order.To gain control of magnetization dynamics and all-optical switching in the lateral dimension, one relies on nanometer localization of the optical excitation, as well as detailed knowledge on how (spin-polarized) electron currents lead to a spatial transfer of magnetization. Technologically this plays an important role not only for all-optical approaches, but also for heat-assisted magnetic recording, which has the potential to increase the magnetic recording density by lowering the coercitivity of high-anisotropy materials [12]. Necessary to this end, it is required to deliver the optical energy to a sub-100-nm spot size, i.e., far beyond the diffraction limit of optical light. The most successful approaches include localization of the evanescent light from near-field optical probes [13], using metallic plates to excite surface plasmons [14,15] or a combination thereof [16].Here, we implement time-resolved Fourier transform holography (FTH) [17] and exploit x-ray magnetic circular dichroism (XMCD) to directly image the magnet...