Single-shot terahertz time-domain spectrometer using 1550 nm probe pulses and diversity electro-optic sampling.

Classical terahertz spectroscopy usually requires the use of Fourier transform or Time-Domain Spectrometers. However, these classical techniques become impractical when using recent high peak power terahertz sources - based on intense lasers or accelerators - which operate at low repetition rate. We present and test the design of a novel Time-Domain Spectrometer, that is capable of recording a whole terahertz spectrum at each shot of the source, and that uses a 1550 nm probe fiber laser. Single-shot operation is obtained using chirped-pulse electro-optic sampling in Gallium Arsenide, and high bandwidth is obtained by using the recently introduced Diversity Electro-Optic Sampling (DEOS) method. We present the first real-time measurements of THz spectra at the TeraFERMI Coherent Transition Radiation source. The system achieves 2.5 THz bandwidth with a maximum dynamic range reaching up to 25 dB. By reducing the required measurement time from minutes to a split-second, this strategy dramatically expands the application range of high power low-repetition rate THz sources.

Quantum state features of the FEL radiation from the occupation number statistics.

The coherence of free-electron laser (FEL) radiation has so far been accessed mainly through first and second order correlation functions. Instead, we propose to reconstruct the energy state occupation number distribution of FEL radiation, avoiding the photo-counting drawbacks with high intensities, by means of maximum likelihood techniques based on the statistics of no-click events. Though the ultimate goal regards the FEL radiation statistical features, the interest of the proposal also resides in its applicability to any process of harmonic generation from a coherent light pulse, ushering in the study of the preservation of quantum features in general non-linear optical processes.

Terahertz Tuning of Dirac Plasmons in Bi_{2}Se_{3} Topological Insulator.

Light can be strongly confined in subwavelength spatial regions through the interaction with plasmons, the collective electronic modes appearing in metals and semiconductors. This confinement, which is particularly important in the terahertz spectral region, amplifies light-matter interaction and provides a powerful mechanism for efficiently generating nonlinear optical phenomena. These effects are particularly relevant in graphene and topological insulators, where massless Dirac fermions show a naturally nonlinear optical behavior in the terahertz range. The strong interaction scenario has been considered so far from the point of view of light. In this Letter, we investigate instead the effect of strong interaction on the plasmon itself. In particular, we will show that Dirac plasmons in Bi_{2}Se_{3} topological insulator are strongly renormalized when excited by high-intensity terahertz radiation by displaying a huge red-shift down to 60% of its characteristic frequency. This opens the road towards tunable terahertz nonlinear optical devices based on topological insulators.

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.

Passive Linearization of the Magnetic Bunch Compression Using Self-Induced Fields.

In linac-driven free-electron lasers, colliders, and energy recovery linacs, a common way to compress the electron bunch to kiloampere level is based upon the implementation of a magnetic dispersive element that converts particle energy deviation into a path-length difference. Nonlinearities of such a process are usually compensated by enabling a high harmonic rf structure properly tuned in amplitude and phase. This approach is however not straightforward, e.g., in C-band and X-band linacs. In this Letter we demonstrate that the longitudinal self-induced field excited by the electron beam itself is able to linearize the compression process without any use of high harmonic rf structure. The method is implemented at the FERMI linac, with the resulting high quality beam used to drive the seeded free-electron laser during user experiments.

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.

Four-wave-mixing experiments with seeded free electron lasers.

The development of free electron laser (FEL) sources has provided an unprecedented bridge between the scientific communities working with ultrafast lasers and extreme ultraviolet (XUV) and X-ray radiation. Indeed, in recent years an increasing number of FEL-based applications have exploited methods and concepts typical of advanced optical approaches. In this context, we recently used a seeded FEL to demonstrate a four-wave-mixing (FWM) process stimulated by coherent XUV radiation, namely the XUV transient grating (X-TG). We hereby report on X-TG measurements carried out on a sample of silicon nitride (Si3N4). The recorded data bears evidence for two distinct signal decay mechanisms: one occurring on a sub-ps timescale and one following slower dynamics extending throughout and beyond the probed timescale range (100 ps). The latter is compatible with a slower relaxation (time decay > ns), that may be interpreted as the signature of thermal diffusion modes. From the peak intensity of the X-TG signal we could estimate a value of the effective third-order susceptibility which is substantially larger than that found in SiO2, so far the only sample with available X-TG data. Furthermore, the intensity of the time-coincidence peak shows a linear dependence on the intensity of the three input beams, indicating that the measurements were performed in the weak field regime. However, the timescale of the ultrafast relaxation exhibits a dependence on the intensity of the XUV radiation. We interpreted the observed behaviour as the generation of a population grating of free-electrons and holes that, on the sub-ps timescale, relaxes to generate lattice excitations. The background free detection inherent to the X-TG approach allowed the determination of FEL-induced electron dynamics with a sensitivity largely exceeding that of transient reflectivity and transmissivity measurements, usually employed for this purpose.

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.

Multicolor High-Gain Free-Electron Laser Driven by Seeded Microbunching Instability.

Laser-heater systems are essential tools to control and optimize high-gain free-electron lasers (FELs) working in the x-ray wavelength range. Indeed, these systems induce a controllable increase of the energy spread of the electron bunch. The heating suppresses longitudinal microbunching instability which otherwise would limit the FEL performance. Here, we demonstrate that, through the action of the microbunching instability, a long-wavelength modulation of the electron beam induced by the laser heater at low energy can persist until the beam entrance into the undulators. This coherent longitudinal modulation is exploited to control the FEL spectral properties, in particular, multicolor extreme-ultraviolet FEL pulses can be generated through a frequency mixing of the modulations produced by the laser heater and the seed laser in the electron beam. We present an experimental demonstration of this novel configuration carried out at the FERMI FEL.

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.

Microbunching instability suppression via electron-magnetic-phase mixing.

Control of the microbunching instability is a fundamental requirement in modern high-brightness electron linacs, in order to prevent misleading responses of beam optical diagnostics and contamination in the generation of coherent radiation, such as free electron lasers. We present the first experimental demonstration of control and suppression of microbunching instability by means of particles' longitudinal phase mixing in a magnetic chicane. In the presence of phase mixing, the intensity of the beam-emitted optical transition radiation, which is used as an indicator of the instability gain at optical wavelengths, is reduced by one order of magnitude and brought to the same level provided, alternatively, by beam heating. The experimental results are in agreement with particle tracking and analytical evaluations of the instability gain. This article is extended to a discussion of applications of magnetic-phase mixing to the generation of quasicold high-brightness ultrarelativistic electron beams.

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.

The TeraFERMI terahertz source at the seeded FERMI free-electron-laser facility.

We describe the project for the construction of a terahertz (THz) beamline to be called TeraFERMI at the seeded FERMI free electron laser (FEL) facility in Trieste, Italy. We discuss topics as the underlying scientific case, the choice of the source, the expected performance, and THz beam propagation. Through electron beam dynamics simulations we show that the installation of the THz source in the beam dump section provides a new approach for compressing the electron bunch length without affecting FEL operation. Thanks to this further compression of the FEL electron bunch, the TeraFERMI facility is expected to provide THz pulses with energies up to the mJ range during normal FEL operation.

Cancellation of coherent synchrotron radiation kicks with optics balance.

Minimizing transverse emittance is essential in linear accelerators designed to deliver very high brightness electron beams. Emission of coherent synchrotron radiation (CSR), as a contributing factor to emittance degradation, is an important phenomenon to this respect. A manner in which to cancel this perturbation by imposing certain symmetric conditions on the electron transport system has been suggested.We first expand on this idea by quantitatively relating the beam Courant-Snyder parameters to the emittance growth and by providing a general scheme of CSR suppression with asymmetric optics, provided it is properly balanced along the line. We present the first experimental evidence of this cancellation with the resultant optics balance of multiple CSR kicks: the transverse emittance of a 500 pC, sub-picosecond, high brightness electron beam is being preserved after the passage through the achromatic transfer line of the FERMI@Elettra free electron laser, and emittance growth is observed when the optics balance is intentionally broken. We finally show the agreement between the theoretical model and the experimental results. This study holds the promise of compact dispersive lines with relatively large bending angles, thus reducing costs for future electron facilities.