Laura Foglia

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.

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.

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.

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.

Generation of acoustic waves by an extreme ultra violet free electron laser in a transient grating experiment

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.