Long-lived nonthermal electron distribution in aluminum excited by femtosecond extreme ultraviolet radiation

We report a time-resolved study of the relaxation dynamics of Al films excited by ultrashort intense free-electron laser (FEL) extreme ultraviolet pulses. The system response was measured through a pump-probe detection scheme, in which an intense FEL pulse tuned around the Al L2,3 edge (72.5 eV) acted as the pump, while a time-delayed ultrafast pulse probed the near-infrared (NIR) reflectivity of the Al film. Remarkably, following the intense FEL excitation, the reflectivity of the film exhibited no detectable variation for hundreds of femtoseconds. Following this latency time, sizable reflectivity changes were observed. Exploiting recent theoretical calculations of the EUV-excited electron dynamics [N. Medvedev et al., Phys. Rev. Lett. 107, 165003 (2011)], the delayed NIR-reflectivity evolution is interpreted invoking the formation of very-long-living nonthermal hot electron distributions in Al after exposure to EUV pulses. Our data represent the first evidence in the time domain of such an intriguing behavior

Optical constants modelling in silicon nitride membrane transiently excited by EUV radiation.

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

Saturable Absorption of Free-Electron Laser Radiation by Graphite near the Carbon K-Edge

The interaction of intense light with matter gives rise to competing nonlinear responses that can dynamically change material properties. Prominent examples are saturable absorption (SA) and two-photon absorption (TPA), which dynamically increase and decrease the transmission of a sample depending on pulse intensity, respectively. The availability of intense soft X-ray pulses from free-electron lasers (FELs) has led to observations of SA and TPA in separate experiments, leaving open questions about the possible interplay between and relative strength of the two phenomena. Here, we systematically study both phenomena in one experiment by exposing graphite films to soft X-ray FEL pulses of varying intensity. By applying real-time electronic structure calculations, we find that for lower intensities the nonlinear contribution to the absorption is dominated by SA attributed to ground-state depletion; our model suggests that TPA becomes more dominant for larger intensities (\u3e1014 W/cm2). Our results demonstrate an approach of general utility for interpreting FEL spectroscopies

{\AA}ngstr\"om-resolved Interfacial Structure in Organic-Inorganic Junctions

Charge transport processes at interfaces which are governed by complex interfacial electronic structure play a crucial role in catalytic reactions, energy storage, photovoltaics, and many biological processes. Here, the first soft X-ray second harmonic generation (SXR-SHG) interfacial spectrum of a buried interface (boron/Parylene-N) is reported. SXR-SHG shows distinct spectral features that are not observed in X-ray absorption spectra, demonstrating its extraordinary interfacial sensitivity. Comparison to electronic structure calculations indicates a boron-organic separation distance of 1.9 {\AA}, wherein changes as small as 0.1 {\AA} result in easily detectable SXR-SHG spectral shifts (ca. 100s of meV). As SXR-SHG is inherently ultrafast and sensitive to individual atomic layers, it creates the possibility to study a variety of interfacial processes, e.g. catalysis, with ultrafast time resolution and bond specificity.Comment: 19 page

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

FEL stochastic spectroscopy revealing silicon bond softening dynamics

Time-resolved X-ray Emission/Absorption Spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires X-ray pulses with both a narrow bandwidth and sub-picosecond pulse duration, a combination that in principle finds its optimum with Fourier transform-limited pulses. In this work, we explore an alternative xperimental approach, capable of simultaneously retrieving information about unoccupied (XAS) and occupied (XES) states from the stochastic fluctuations of broadband extreme ultraviolet pulses of a free-electron laser. We used this method, in combination with singular value decomposition and Tikhonov regularization procedures, to determine the XAS/XES response from a crystalline silicon sample at the L2,3-edge, with an energy resolution of a few tens of meV. Finally, we combined this spectroscopic method with a pump-probe approach to measure structural and electronic dynamics of a silicon membrane. Tr-XAS/XES data obtained after photoexcitation with an optical laser pulse at 390 nm allowed us to observe perturbations of the band structure, which are compatible with the formation of the predicted precursor state of a non-thermal solid-liquid phase transition associated with a bond softening phenomenon

Terahertz-wave decoding of femtosecond extreme-ultraviolet light pulses

In recent years, femtosecond extreme-ultraviolet (XUV) and x-ray pulses from free-electron lasers have developed into important probes to monitor processes and dynamics in matter on femtosecond-time and angstrom-length scales. With the rapid progress of versatile ultrafast x-ray spectroscopy techniques and more sophisticated data analysis tools, accurate single-pulse information on the arrival time, duration, and shape of the probing x-ray and XUV pulses becomes essential. Here, we demonstrate that XUV pulses can be converted into terahertz electromagnetic pulses using a spintronic terahertz emitter. We observe that the duration, arrival time, and energy of each individual XUV pulse is encoded in the waveform of the associated terahertz pulses, and thus can be readily deduced from single-shot terahertz time-domain detection

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

Progettazione e valutazione del comportamento ad impatto di un dispositivo di monitoraggio e memorizzazione integrabile nei dispositivi di protezione

Negli ultimi anni le statistiche relative ad infortuni ed incidenti nel mondo del lavoro, nel settore delle due ruote e del volo libero mostrano una discreta riduzione dei casi che si assesta però, in tutti e tre gli ambiti, intorno ad un plateau con valori che restano preoccupanti. In contemporanea, le istituzioni prima e l’opinione pubblica poi hanno sviluppato una sempre più crescente coscienza dell’importanza della sicurezza sia sul luogo di lavoro che in altri contesti. Questo inevitabilmente ha influito in modo positivo sul mercato dei dispositivi di protezione attraverso un aumento della domanda ed allo stesso tempo si è avuto un impulso per lo sviluppo di dispositivi innovativi rispetto a quanto già offerto. Questo scenario ci ha spinti a proporre un nuovo concetto di DPI rispetto ai vecchi canoni, ovvero l’obiettivo è stato rendere tali sistemi automatici, attivi, interattivi e dotati di memoria, così da ottenere un significativo incremento di sicurezza per l’utente finale. Il seguente studio descrive, dall’idea al prototipo, il progetto di un dispositivo elettronico di monitoraggio e memorizzazione, in grado di attivare autonomamente il gonfiaggio di airbag disposti a protezione dell’utente ed integrabile in indumenti e/o attrezzature. In particolare l’analisi verifica in prima approssimazione, qualora si abbia caduta dall’alto, la bontà o meno della resistenza all’urto delle configurazioni scelte per l’integrazione dell’elettronica

Special Issue on Latest Trends in Free Electron Lasers

In the last decade, free electron laser (FEL) sources operating from the extreme ultraviolet (EUV) up to the hard X-ray photon energy range [...