The role of the electron recoiling mechanism in coherent light high-order harmonics generation: from the source to the applications

2008/2009I processi di generazione di armoniche di ordine superiore (High-order Harmonic Generation o HHG) in gas inerti rappresentano, attualmente, la tecnica piu` promettente per la creazione di impulsi di luce coerente nell'estremo ultra-violetto (EUV) in una configurazione table-top. I processi HHG si basano sull'interazione non-lineare, tra impulsi laser ultra-corti, tipicamente dell'ordine della decina di femtosecondi, e atomi di gas inerti. Le caratteristiche che distinguono i processi HHG sono la loro durata temporale, che puo` essere nel dominio degli attosecondo e il fatto che l'interazione e` non perturbativa. Invece, la natura quantistica dei processi HHG implica la presenza di meccanismi di diffusione che influenzano la funzione d'onda dell'elettrone atomico coinvolto nell'interazione con il campo laser. Il ruolo della diffusione viene usualmente trascurato nella letteratura corrente, sebbene quest'ultima sia strettamente legata al controllo dell'efficienza del processo HHG e dello stato di polarizzazione dei fotoni generati. Il lavoro di tesi e` focalizzato sullo studio sperimentale e teorico/fenomenologico del ruolo dei meccanismi di diffusione, e sul loro controllo, al fine di incrementare l'efficienza e la qualita` ottica, i.e. coerenza, struttura temporale, etc., dei fotoni HHG prodotti. Gli studi e gli esperimenti condotti forniscono, in base alla nostra attuale conoscenza, la prima dimostrazione quantitativa a supporto del modello di Leweinstein. Accanto alla caratterizzazione spettrale, viene presentato uno studio accurato circa le condizioni minime necessarie a generare impulsi HHG, sempre legate al ruolo della diffusione della funzione d'onda elettronica. I risultati hanno permesso di ottenere una piu` profonda comprensione della complessa dinamica non-lineare, che sta alla base dei processi HHG. Accanto allo studio della diffusione si e` cercato di ottenere il controllo sullo stato di polarizzazione degli impulsi HHG, i quali mantengono la polarizzazione della radiazione laser utilizzata. La stessa diffusione impedisce di creare efficientemente armoniche di ordine superiore con polarizzazione ellittica (o circolare). Per risovere questo problema e` stata abbiamo sviluppato una collaborazione con il gruppo CXRO del Lawrence Berkeley National Laboratory, (Berkeley, USA), grazie al quale sono state realizzate una serie di ottiche multistrati innovative basate sul principio dell'angolo di Brewster, e disegnate appositamente per polarizzare circolarmente impulsi di luce EUV. Queste ultime sono state preliminarmente testate con successo sulla beam-line 6.3.2 del sincrotrone di Berkeley. La parte finale della tesi presenta la prima sorgente di impulsi HHG, polarizzati circolarmente utilizzando i citati multistrati. Per verificare l'efficienza e` di questi multistrati e` stato condotto un esperimento di dicroismo magnetico circolare con radiazioni EUV (EUV-MCD), unico nel sul genere, in quanto utilizza gli impulsi HHG polarizzati circolarmente per sondare il comportamento dicroico in corrispondenza delle soglie di assorbimento M di metalli ferromagnetici come Fe e Ni o delle loro leghe. Il fine ultimo e` dato dalla realizzazione di un esperimento risolto in tempo capace di utlizzare impulsi HHG circolarmente polarizzati per comprendere il processo di demagnetizzazione di sistemi ferromagnetici, sulla scala temporale del femtosecondo.XXII Ciclo198

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

{\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

AC/DC: The FERMI FEL Split and Delay Optical Device for Ultrafast X-ray Science

Free-electron lasers (FELs) are the most advanced class of light-sources, by virtue of their unique capability to lase high-brightness pulses characterized by wavelengths spanning the extreme-ultraviolet, the soft and hard X-ray spectral domains, as well as by temporal lengths lying in the femtosecond (fs) timescale. The next step to push the current standards in ultrafast X-ray science is strongly linked to the possibility of engineering and exploiting time-resolved experiments exclusively for FELs pulses, ideally having different colors tunable at specific electronic resonance of the chemical elements. At the seeded FERMI FEL (Trieste, Italy) this goal is committed to the optical device known as AC/DC, which stands for the auto correlator/delay creator. AC/DC is designed to double the incoming FEL pulse splitting the photon beam by inserting a grazing incidence flat mirror, thus preserving the spectral and temporal properties, and further delaying one of these two pulses in time. It can independently tune the FEL pulses fluence on the two optical paths by means of solid-state filters, too. Here, we present a detailed description about this optical device. Strong emphasis is dedicated to the AC/DC opto-mechanical design and to the laser-based feedback systems implemented to compensate for any mismatch affecting the FEL optical trajectory, ascribable to both mechanical imperfections and paraxial errors rising during a temporal delay scan

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

Femtosecond polarization shaping of free-electron laser pulses

We demonstrate the generation of extreme-ultraviolet (XUV) free-electron laser (FEL) pulses with time-dependent polarization. To achieve polarization modulation on a femtosecond timescale, we combine two mutually delayed counterrotating circularly polarized subpulses from two cross-polarized undulators. The polarization profile of the pulses is probed by angle-resolved photoemission and above-threshold ionization of helium; the results agree with solutions of the time-dependent Schrödinger equation. The stability limit of the scheme is mainly set by electron-beam energy fluctuations, however, at a level that will not compromise experiments in the XUV. Our results demonstrate the potential to improve the resolution and element selectivity of methods based on polarization shaping and may lead to the development of new coherent control schemes for probing and manipulating core electrons in matter

Dissecting Mott and charge-density wave dynamics in the photoinduced phase of 1T-TaS[sub]2

The two-dimensional transition-metal dichalcogenide 1T−TaS2 is a complex material standing out for its puzzling low temperature phase marked by signatures amenable to both Mott-insulating and charge-density wave states. Electronic Mott states, coupled to a lattice, respond to coherent optical excitations via a modulation of the lower (valence) Hubbard band. Such dynamics is driven by strong electron-phonon coupling and typically lasts for tens of picoseconds, mimicking coherent structural distortions. Instead, the response occurring at the much faster timescale, mainly dominated by electronic many-body effects, is still a matter of intense research. By performing time- and angle-resolved photoemission spectroscopy, we investigated the photoinduced phase of 1T−TaS2 and found out that its lower Hubbard band promptly reacts to coherent optical excitations by shifting its binding energy towards a slightly larger value. This process lasts for a time comparable to the optical pump pulse length, mirroring a transient change of the onsite Coulomb repulsion energy (U). Such an observation suggests that the correction to the bare value of U, ascribed to the phonon-mediated screening which slightly opposes the Hubbard repulsion, is lost within an interval of a few tens of femtoseconds and can be understood as a fingerprint of electronic states largely decoupled from the lattice. Additionally, these results enforce the hypothesis, envisaged in the current literature, that the transient photoinduced states belong to a sort of crossover phase instead of an equilibrium metallic one

Transient EUV Reflectivity Measurements of Carbon upon Ultrafast Laser Heating

Time resolved extreme ultraviolet (EUV) transient reflectivity measurements on non-equilibrium amorphous carbon (a-C) have been carried out by combining optical and free electron laser (FEL) sources. The EUV probing was specifically sensitive to lattice dynamics, since the EUV reflectivity is essentially unaffected by the photo-excited surface plasma. Data have been interpreted in terms of the dynamics of an expanding surface, i.e., a density gradient rapidly forming along the normal surface. This allowed us to determine the characteristic time ( τ ≲ 1 ps) for hydrodynamic expansion in photo-excited a-C. This finding suggests an extremely narrow time window during which the system can be assumed to be in the isochoric regime, a situation that may complicate the study of photo-induced metastable phases of carbon. Data also showed a weak dependence on the probing EUV wavelength, which was used to estimate the electronic temperature ( T e ≈ 0.8 eV) of the excited sample. This experimental finding compares fairly well with the results of calculations, while a comparison of our data and calculations with previous transient optical reflectivity measurements highlights the complementarities between optical and EUV probing

Amplified spontaneous and stimulated Mg L emission from MgO pumped by FEL pulses

Conference on X-Ray Lasers and Coherent X-ray Sources - Development and Applications, Prague, CZECH REPUBLIC, APR 24-26, 2017International audienceStimulated emission is a fundamental process in nature that deserves to be investigated and understood in the EUV and X-ray regimes. Today this is definitely possible through high energy density FEL beams. In this context, we show evidence for soft x-ray stimulated emission from a MgO solid target pumped by extreme ultraviolet 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 have developed a 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 L-2,L-3 characteristic emission and the pumping threshold