R. Mincigrucci

Towards jitter-free pump-probe measurements at seeded free electron laser facilities.

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.

Soft X-Ray Second Harmonic Generation as an Interfacial Probe

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.

Free electron laser-driven ultrafast rearrangement of the electronic structure in Ti

High-energy density extreme ultraviolet radiation delivered by the FERMI seeded free-electron laser has been used to create an exotic nonequilibrium state of matter in a titanium sample characterized by a highly excited electron subsystem at temperatures in excess of 10 eV and a cold solid-density ion lattice. The obtained transient state has been investigated through ultrafast absorption spectroscopy across the Ti M2,3-edge revealing a drastic rearrangement of the sample electronic structure around the Fermi level occurring on a time scale of about 100 fs.

Toward an integrated device for spatiotemporal superposition of free-electron lasers and laser pulses

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.

Four-wave-mixing experiments and beyond: the TIMER/mini-TIMER setups at FERMI

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.

FEL-based transient grating spectroscopy

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.

Timing methodologies and studies at the FERMI free-electron laser

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.

Characterization of ultrafast free-electron laser pulses using extreme-ultraviolet transient gratings

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.

EUV stimulated emission from MgO pumped by FEL pulses

Stimulated emission is a fundamental process in nature that deserves to be investigated and understood in the extreme ultra-violet (EUV) and x-ray regimes. Today, this is definitely possible through high energy density free electron laser (FEL) beams. In this context, we give evidence for soft-x-ray stimulated emission from a magnesium oxide solid target pumped by EUV 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 develop a novel 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 L2,3 characteristic emission and the pumping threshold.

The EIS beamline at the seeded free-electron laser FERMI

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.