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,

The morphology of micrometre−size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X−ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub−micrometre particles to nanometre resolution in their native environment, using intense, coherent X−ray pulses from the Linac Coherent Light Source free−electron laser. We introduced individual aerosol particles into the pulsed X−ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non−equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large−scale production of nanoscale structures by flame synthesi

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