Coherent THz Emission Enhanced by Coherent Synchrotron Radiation Wakefield.

We demonstrate that emission of coherent transition radiation by a ∼1 GeV energy-electron beam passing through an Al foil is enhanced in intensity and extended in frequency spectral range, by the energy correlation established along the beam by coherent synchrotron radiation wakefield, in the presence of a proper electron optics in the beam delivery system. Analytical and numerical models, based on experimental electron beam parameters collected at the FERMI free electron laser (FEL), predict transition radiation with two intensity peaks at ∼0.3 THz and ∼1.5 THz, and extending up to 8.5 THz with intensity above 20 dB w.r.t. the main peak. Up to 80-µJ pulse energy integrated over the full bandwidth is expected at the source, and in agreement with experimental pulse energy measurements. By virtue of its implementation in an FEL beam dump line, this work promises dissemination of user-oriented multi-THz beamlines parasitic and self-synchronized to EUV and x-ray FELs.

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.

Tunable orbital angular momentum in high-harmonic generation.

Optical vortices are currently one of the most intensively studied topics in optics. These light beams, which carry orbital angular momentum (OAM), have been successfully utilized in the visible and infrared in a wide variety of applications. Moving to shorter wavelengths may open up completely new research directions in the areas of optical physics and material characterization. Here, we report on the generation of extreme-ultraviolet optical vortices with femtosecond duration carrying a controllable amount of OAM. From a basic physics viewpoint, our results help to resolve key questions such as the conservation of angular momentum in highly nonlinear light-matter interactions, and the disentanglement and independent control of the intrinsic and extrinsic components of the photon's angular momentum at short-wavelengths. The methods developed here will allow testing some of the recently proposed concepts such as OAM-induced dichroism, magnetic switching in organic molecules and violation of dipolar selection rules in atoms.

Time-Resolved Measurement of Interatomic Coulombic Decay Induced by Two-Photon Double Excitation of Ne_{2}.

The hitherto unexplored two-photon doubly excited states [Ne^{*}(2p^{-1}3s)]_{2} were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD), which predominantly produces singly ionized dimers. In order to obtain the rate of ICD, the resulting yield of Ne_{2}^{+} ions was recorded as a function of delay between the extreme ultraviolet pump and UV probe laser pulses. The extracted lifetimes of the long-lived doubly excited states, 390(-130/+450) fs, and of the short-lived ones, less than 150 fs, are in good agreement with ab initio quantum mechanical calculations.

Slow Interatomic Coulombic Decay of Multiply Excited Neon Clusters.

Ne clusters (∼5000 atoms) were resonantly excited (2p→3s) by intense free electron laser (FEL) radiation at FERMI. Such multiply excited clusters can decay nonradiatively via energy exchange between at least two neighboring excited atoms. Benefiting from the precise tunability and narrow bandwidth of seeded FEL radiation, specific sites of the Ne clusters were probed. We found that the relaxation of cluster surface atoms proceeds via a sequence of interatomic or intermolecular Coulombic decay (ICD) processes while ICD of bulk atoms is additionally affected by the surrounding excited medium via inelastic electron scattering. For both cases, cluster excitations relax to atomic states prior to ICD, showing that this kind of ICD is rather slow (picosecond range). Controlling the average number of excitations per cluster via the FEL intensity allows a coarse tuning of the ICD rate.

Single Shot Polarization Characterization of XUV FEL Pulses from Crossed Polarized Undulators.

Polarization control is a key feature of light generated by short-wavelength free-electron lasers. In this work, we report the first experimental characterization of the polarization properties of an extreme ultraviolet high gain free-electron laser operated with crossed polarized undulators. We investigate the average degree of polarization and the shot-to-shot stability and we analyze aspects such as existing possibilities for controlling and switching the polarization state of the emitted light. The results are in agreement with predictions based on Gaussian beams propagation.

The FERMI free-electron lasers.

FERMI is a seeded free-electron laser (FEL) facility located at the Elettra laboratory in Trieste, Italy, and is now in user operation with its first FEL line, FEL-1, covering the wavelength range between 100 and 20 nm. The second FEL line, FEL-2, a high-gain harmonic generation double-stage cascade covering the wavelength range 20-4 nm, has also completed commissioning and the first user call has been recently opened. An overview of the typical operating modes of the facility is presented.

Experimental demonstration of enhanced self-amplified spontaneous emission by an optical klystron.

We report the first experimental evidence of enhancement of self-amplified spontaneous emission, due to the use of an optical klystron. In this free-electron laser scheme, a relativistic electron beam passes through two undulators, separated by a dispersive section. The latter converts the electron-beam energy modulation produced in the first undulator in density modulation, thus enhancing the free-electron laser gain. The experiment has been carried out at the FERMI facility in Trieste. Powerful radiation has been produced in the extreme ultraviolet range, with an intensity a few orders of magnitude larger than in pure self-amplified spontaneous emission mode. Data have been benchmarked with an existing theoretical model.

Magnetization and microstructure dynamics in Fe/MnAs/GaAs(001): Fe magnetization reversal by a femtosecond laser pulse.

Thin film magnetization reversal without applying external fields is an attractive perspective for applications in sensors and devices. One way to accomplish it is by fine-tuning the microstructure of a magnetic substrate via temperature control, as in the case of a thin Fe layer deposited on a MnAs/GaAs(001) template. This work reports a time-resolved resonant scattering study exploring the magnetic and structural properties of the Fe/MnAs system, using a 100 fs optical laser pulse to trigger local temperature variations and a 100 fs x-ray free-electron laser pulse to probe the induced magnetic and structural dynamics. The experiment provides direct evidence that a single optical laser pulse can reverse the Fe magnetization locally. It reveals that the time scale of the magnetization reversal is slower than that of the MnAs structural transformations triggered by the optical pulse, which take place after a few picoseconds already.

Double-configuration grating monochromator for extreme-ultraviolet ultrafast pulses.

We present the design and characterization of a double-configuration grating monochromator for the spectral selection of extreme-ultraviolet ultrafast pulses. Two grating geometries are joined in an instrument with two interchangeable diffracting stages, both used at grazing incidence: one with the gratings in the off-plane mount (OPM), the other in the classical diffraction mount (CDM). The use of two stages gives great flexibility: the OPM stage is used for sub-50 fs time response and low spectral resolution, while the CDM stage is for 100-200 fs time response and high spectral resolution. The monochromator spectral and temporal performances have been experimentally demonstrated on a high-order laser-harmonics beam line.

Determining the polarization state of an extreme ultraviolet free-electron laser beam using atomic circular dichroism.

Ultrafast extreme ultraviolet and X-ray free-electron lasers are set to revolutionize many domains such as bio-photonics and materials science, in a manner similar to optical lasers over the past two decades. Although their number will grow steadily over the coming decade, their complete characterization remains an elusive goal. This represents a significant barrier to their wider adoption and hence to the full realization of their potential in modern photon sciences. Although a great deal of progress has been made on temporal characterization and wavefront measurements at ultrahigh extreme ultraviolet and X-ray intensities, only few, if any progress on accurately measuring other key parameters such as the state of polarization has emerged. Here we show that by combining ultra-short extreme ultraviolet free electron laser pulses from FERMI with near-infrared laser pulses, we can accurately measure the polarization state of a free electron laser beam in an elegant, non-invasive and straightforward manner using circular dichroism.

CITIUS: an infrared-extreme ultraviolet light source for fundamental and applied ultrafast science.

We present the main features of CITIUS, a new light source for ultrafast science, generating tunable, intense, femtosecond pulses in the spectral range from infrared to extreme ultraviolet (XUV). The XUV pulses (about 10(5)-10(8) photons/pulse in the range 14-80 eV) are produced by laser-induced high-order harmonic generation in gas. This radiation is monochromatized by a time-preserving monochromator, also allowing one to work with high-resolution bandwidth selection. The tunable IR-UV pulses (10(12)-10(15) photons/pulse in the range 0.4-5.6 eV) are generated by an optical parametric amplifier, which is driven by a fraction of the same laser pulse that generates high order harmonics. The IR-UV and XUV pulses follow different optical paths and are eventually recombined on the sample for pump-probe experiments. We also present the results of two pump-probe experiments: with the first one, we fully characterized the temporal duration of harmonic pulses in the time-preserving configuration; with the second one, we demonstrated the possibility of using CITIUS for selective investigation of the ultra-fast dynamics of different elements in a magnetic compound.

Experimental demonstration of electron longitudinal-phase-space linearization by shaping the photoinjector laser pulse.

Control of the electron-beam longitudinal-phase-space distribution is of crucial importance in a number of accelerator applications, such as linac-driven free-electron lasers, colliders and energy recovery linacs. Some longitudinal-phase-space features produced by nonlinear electron beam self- fields, such as a quadratic energy chirp introduced by geometric longitudinal wakefields in radio-frequency (rf) accelerator structures, cannot be compensated by ordinary tuning of the linac rf phases nor corrected by a single high harmonic accelerating cavity. In this Letter we report an experimental demonstration of the removal of the quadratic energy chirp by properly shaping the electron beam current at the photoinjector. Specifically, a longitudinal ramp in the current distribution at the cathode linearizes the longitudinal wakefields in the downstream linac, resulting in a flat electron current and energy distribution. We present longitudinal-phase-space measurements in this novel configuration compared to those typically obtained without longitudinal current shaping at the FERMI linac.

Two-colour pump-probe experiments with a twin-pulse-seed extreme ultraviolet free-electron laser.

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.

Coherent light with tunable polarization from single-pass free-electron lasers.

Tunable polarization over a wide spectral range is a required feature of light sources employed to investigate the properties of local symmetry in matter. In this Letter, we provide the first experimental characterization of the polarization of the harmonic light produced by a free-electron laser and demonstrate a method to obtain free-electron laser harmonics with tunable polarization. Experimental results are successfully compared with theory. Our findings can be expected to have a deep impact on the design and realization of experiments requiring full control of light polarization.

Out-of-equilibrium phase transitions in the Hamiltonian mean-field model: a closer look.

We provide a detailed discussion of out-of-equilibrium phase transitions in the Hamiltonian mean-field (HMF) model in the framework of Lynden-Bell's statistical theory of the Vlasov equation. For two-level initial conditions, the caloric curve ß(E) only depends on the initial value f(0) of the distribution function. We evidence different regions in the parameter space where the nature of the phase transitions between magnetized and nonmagnetized states changes: (i) For f(0)>0.10965, the system displays a second-order phase transition; (ii) for 0.109497

Vlasov equation for long-range interactions on a lattice.

We show that, in the continuum limit, the dynamics of Hamiltonian systems defined on a lattice with long-range couplings is well described by the Vlasov equation. This equation can be linearized around the homogeneous state, and a dispersion relation, which depends explicitly on the Fourier modes of the lattice, can be derived. This allows one to compute the stability thresholds of the homogeneous state, which turns out to depend on the mode number. When this state is unstable, the growth rates are also functions of the mode number. Explicit calculations are performed for the α-Hamiltonian mean field model with 0≤α<1, for which the mean-field mode is always found to dominate the exponential growth. The theoretical predictions are successfully compared with numerical simulations performed on a finite lattice.

Experimental demonstration of frequency pulling in single-pass free-electron lasers.

Frequency pulling is a well-known phenomenon in standard laser physics, leading to a shift of the laser frequency when the cavity and maximum gain frequencies are detuned. In this letter we present the first experimental demonstration of frequency pulling in single-pass free-electron lasers. Measurements are performed using the single-pass free-electron laser installed on the Elettra storage ring.

Negative specific heat in the canonical statistical ensemble.

According to thermodynamics, the specific heat of Boltzmannian short-range interacting systems is a positive quantity. Less intuitive properties are instead displayed by systems characterized by long-range interactions. In that case, the sign of specific heat depends on the considered statistical ensemble: Negative specific heat can be found in isolated systems, which are studied in the framework of the microcanonical ensemble; on the other hand, it is generally recognized that a positive specific heat should always be measured in systems in contact with a thermal bath, for which the canonical ensemble is the appropriate one. We demonstrate that the latter assumption is not generally true: One can, in principle, measure negative specific heat also in the canonical ensemble if the system under scrutiny is non-Boltzmannian and/or out-of-equilibrium.

Lyapunov stability of Vlasov equilibria using Fourier-Hermite modes.

We propose an efficient method to compute Lyapunov exponents and Lyapunov eigenvectors of long-range interacting many-particle systems, whose dynamics is described by the Vlasov equation. We show that an expansion of a distribution function using Hermite modes (in velocity variable) and Fourier modes (in configuration variable) converges fast if an appropriate scaling parameter is introduced and identified with the inverse of the temperature. As a consequence, dynamics and linear stability properties of many-particle states, both in the close-to and in the far-from equilibrium regimes, can be predicted using a small number of expansion coefficients. As an example of a long-range interacting system we investigate stability properties of stationary states, the Hamiltonian mean-field model.