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The microbunching instability has been a long-standing issue for high-brightness free-electron lasers (FELs), and is a significant show-stopper to achieving full longitudinal coherence in the x-ray regime. This paper reports the first experimental demonstration of microbunching instability mitigation through transverse Landau damping, based on linear optics control in a dispersive region. Analytical predictions for the microbunching content are supported by numerical calculations of the instability gain and confirmed through the experimental characterization of the spectral brightness of the FERMI FEL under different transverse optics configurations of the transfer line between the linear accelerator and the FEL.

Electromagnetic waves possessing orbital angular momentum (OAM) are powerful tools for applications in optical communications, new quantum technologies and optical tweezers. Recently, they have attracted growing interest since they can be harnessed to detect peculiar helical dichroic effects in chiral molecular media and in magnetic nanostructures. In this work, we perform single-shot per position ptychography on a nanostructured object at a seeded free-electron laser, using extreme ultraviolet OAM beams of different topological charge order $\ell$ generated with spiral zone plates. By controlling $\ell$, we demonstrate how the structural features of OAM beam profile determine an improvement of about 30% in image resolution with respect to conventional Gaussian beam illumination. This result extends the capabilities of coherent diffraction imaging techniques, and paves the way for achieving time-resolved high-resolution (below 100 nm) microscopy on large area samples., Comment: M. Pancaldi and F. Guzzi contributed equally to this work

Chiral molecules are widespread in nature, playing a fundamental role in bio-chemical processes and in the origin of life itself. The observation of dynamics in chiral molecules is crucial for the understanding and control of the chiral activity of photo-excited states. One of the most promising techniques for the study of photo-excited chiral systems is time-resolved photoelectron circular dichroism (TR-PECD), which offers an intense and sensitive probe for vibronic and geometric molecular structure as well as electronic structures, and their evolution on a femtosecond timescale. However, the non-local character of the PECD effect, which is imprinted during the electron scattering off the molecule, makes the interpretation of TR-PECD experiments challenging. In this respect, core-photoionization is known to allow site- and chemical-sensitivity to photelectron spectroscopy. Here we demonstrate that TR-PECD utilising core-level photoemission enables probing the chiral electronic structure and its relaxation dynamics with atomic site sensitivity. Following UV pumped excitation to a 3s Rydberg state, fenchone enantiomers (C 10 H 16 O) were probed on a femtosecond scale using circularly polarized soft X-ray light pulses provided by the free-electron laser FERMI. C 1s binding energy shifts caused by the redistribution of valence electron density in this 3s-valence-Rydberg excitation allowed us to measure transient PECD chiral responses with an enhanced C-atom site-selectivity compared to that achievable in the ground state molecule. These results represent the first chemical-specific and site-specific, enantio-sensitive observations on the electronic structure of a photo-excited chiral molecule and pave the way towards chiral femtochemistry probed by core-level photoemission.

Echo-enabled harmonic generation free-electron lasers (EEHG FELs) are promising candidates to produce fully coherent soft x-ray pulses by virtue of efficient high harmonic frequency up-conversion from UV lasers. The ultimate spectral limit of EEHG, however, remains unclear, because of the broadening and distortions induced in the output spectrum by residual broadband energy modulations in the electron beam. We present a mathematical description of the impact of incoherent (broadband) energy modulations on the bunching spectrum produced by the microbunching instability through both the accelerator and the EEHG line. The model is in agreement with a systematic experimental characterization of the FERMI EEHG FEL in the photon energy range $130-210$ eV. We find that amplification of electron beam energy distortions primarily in the EEHG dispersive sections explains an observed reduction of the FEL spectral brightness that is proportional to the EEHG harmonic number. Local maxima of the FEL spectral brightness and of the spectral stability are found for a suitable balance of the dispersive sections' strength and the first seed laser pulse energy. Such characterization provides a benchmark for user experiments and future EEHG implementations designed to reach shorter wavelengths.

High-brightness electron bunches, such as those generated and accelerated in free-electron lasers (FELs), can develop small-scale structure in the longitudinal phase space. This causes variations in the slice energy spread and current profile of the bunch which then undergo amplification, in an effect known as the microbunching instability. By imposing energy spread modulations on the bunch in the low-energy section of an accelerator, using an undulator and a modulated laser pulse in the centre of a dispersive chicane, it is possible tomanipulate the bunch longitudinal phase space. This allows for the control and study of the instability in unprecedented detail. We report measurements and analysis of such modulated electron bunches in the 2Dspectro-temporal domain at the FERMI FEL, for three different bunch compression schemes. We also perform corresponding simulations of these experiments and show that the codes are indeed able to reproduce the measurements across a wide spectral range. This detailed experimental verification of the ability of codes to capture the essential beam dynamics of the microbunching instability will benefit the design and performance of future FELs., Comment: 12 pages, 14 figures

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 XUV 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 \emph{ab initio} quantum mechanical calculations.

An understanding of collective effects is of fundamental importance for the design and optimisation of the performance of modern accelerators. In particular, the design of an accelerator with strict requirements on the beam quality, such as a free electron laser (FEL), is highly dependent on a correspondence between simulation, theory and experiments in order to correctly account for the effect of coherent synchrotron radiation (CSR), and other collective effects. A traditional approach in accelerator simulation codes is to utilise an analytic one-dimensional approximation to the CSR force. We present an extension of the 1D CSR theory in order to correctly account for the CSR force at the entrance and exit of a bending magnet. A limited range of applicability to this solution, in particular in bunches with a large transverse spot size or offset from the nominal axis, is recognised. More recently developed codes calculate the CSR effect in dispersive regions directly from the Lienard-Wiechert potentials, albeit with approximations to improve the computational time. A new module of the General Particle Tracer (GPT) code was developed for simulating the effects of CSR, and benchmarked against other codes. We experimentally demonstrate departure from the commonly used 1D CSR theory for more extreme bunch length compression scenarios at the FERMI FEL facility. Better agreement is found between experimental data and the codes which account for the transverse extent of the bunch, particularly in more extreme compression scenarios., Comment: 33 pages, 19 figures, submitted to New J. Phys

XUV and X-ray Free Electron Lasers (FELs) produce short wavelength pulses with high intensity, ultrashort duration, well-defined polarization and transverse coherence, and have been utilised for many experiments previously possible at long wavelengths only: multiphoton ionization, pumping an atomic laser, and four-wave mixing spectroscopy. However one important optical technique, coherent control, has not yet been demonstrated, because Self- Amplified Spontaneous Emission FELs have limited longitudinal coherence. Single-colour pulses from the FERMI seeded FEL are longitudinally coherent, and two-colour emission is predicted to be coherent. Here we demonstrate the phase correlation of two colours, and manipulate it to control an experiment. Light of wavelengths 63.0 and 31.5 nm ionized neon, and the asymmetry of the photoelectron angular distribution was controlled by adjusting the phase, with temporal resolution 3 attoseconds. This opens the door to new shortwavelength coherent control experiments with ultrahigh time resolution and chemical sensitivity.

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.

We present the main features of CITIUS, a new light source for ultrafast science, generating tunable, intense, femtosecond pulses in the spectral range from IR to 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, allowing also 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. The new light source will become the fulcrum of a new center located at the University of Nova Gorica, active in a wide range of scientific fields, including materials science, catalysis, biochemistry and magnetism. 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 studying of ultra-fast dynamics.

We present the experimental demonstration of a method for generating two spectrally and temporally separated pulses by an externally seeded, single-pass free-electron laser operating in the extreme-ultraviolet spectral range. Our results, collected on the FERMI@Elettra facility and confirmed by numerical simulations, demonstrate the possibility of controlling both the spectral and temporal features of the generated pulses. A free-electron laser operated in this mode becomes a suitable light source for jitter-free, two-colour pump-probe experiments.

We demonstrate experimentally the full tunability of a coherent femtosecond source in the whole ultraviolet spectral region. The experiment relies on the technique of high-order harmonic generation driven by a near-infrared parametric laser source in krypton gas. By tuning the drive wavelength in the range between 1100 to 1900 nm, we generated intense harmonics from near to extreme ultraviolet. A number of photons per shot of the order of 10^7 has been measured for the first harmonic orders. Many novel scientific prospects are expected to benefit from the use of such a table-top tunable source.

Tunable polarization over a wide spectral range is a required feature of light sources employed to investigate the properties of local symmetry in both condensed and low-density matter. Among new-generation sources, free-electron lasers possess a unique combination of very attractive features, as they allow to generate powerful and coherent ultra-short optical pulses in the VUV and X-ray spectral range. However, the question remains open about the possibility to freely vary the light polarization of a free-electron laser, when the latter is operated in the so-called nonlinear harmonic-generation regime. In such configuration, one collects the harmonics of the free-electron laser fundamental emission, gaining access to the shortest possible wavelengths the device can generate. In this letter we provide the first experimental characterization of the polarization of the harmonic light produced by a free-electron laser and we demonstrate a method to obtain tunable polarization in the VUV and X-ray spectral range. Experimental results are successfully compared to those obtained using a theoretical model based on the paraxial solution of Maxwell's equations. Our findings can be expected to have a deep impact on the design and realization of experiments requiring full control of light polarization to explore the symmetry properties of matter samples.

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.

Using harmonic emission from circularly polarized undulator is a procedure that is normally employed on synchrotron beamlines in order to extend the covered spectral range. A similar capability is likewise beneficial for next generation free-electron lasers. In this paper, we perform a first quantitative experimental analysis of the angular distribution of free-electron laser harmonic emission from helical undulators. Experimental results are compared to those obtained by means of a theoretical model based on the paraxial solution of Maxwell's equations.

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-levels initial conditions, the caloric curve $\beta(E)$ only depends on the initial value $f_0$ of the distribution function. We evidence different regions in the parameter space where the nature of phase transitions between magnetized and non-magnetized states changes: (i) for $f_0>0.10965$, the system displays a second order phase transition; (ii) for $0.109497

The Vlasov equation is well known to provide a good description of the dynamics of mean-field systems in the $N \to \infty$ limit. This equation has an infinity of stationary states and the case of {\it homogeneous} states, for which the single-particle distribution function is independent of the spatial variable, is well characterized analytically. On the other hand, the inhomogeneous case often requires some approximations for an analytical treatment: the dynamics is then best treated in action-angle variables, and the potential generating inhomogeneity is generally very complex in these new variables. We here treat analytically the linear stability of toy-models where the inhomogeneity is created by an external field. Transforming the Vlasov equation into action-angle variables, we derive a dispersion relation that we accomplish to solve for both the growth rate of the instability and the stability threshold for two specific models: the Hamiltonian Mean-Field model with additional asymmetry and the mean-field $\phi^4$ model. The results are compared with numerical simulations of the $N$-body dynamics. When the {\it inhomogeneous} state is stationary, we expect to observe in the $N$-body dynamics Quasi-Stationary-States (QSS), whose lifetime diverge algebraically with $N$.

The possibility of observing phenomena peculiar to long-range interactions, and more specifically in the so-called Quasi-Stationary State (QSS) regime is investigated within the framework of two devices, namely the Free-Electron Laser (FEL) and the Collective Atomic Recoil Laser (CARL). The QSS dynamics has been mostly studied using the Hamiltonian Mean-Field (HMF) toy model, demonstrating in particular the presence of first versus second order phase transitions from magnetized to unmagnetized regimes in the case of HMF. Here, we give evidence of the strong connections between the HMF model and the dynamics of the two mentioned devices, and we discuss the perspectives to observe some specific QSS features experimentally. In particular, a dynamical analog of the phase transition is present in the FEL and in the CARL in its conservative regime. Regarding the dissipative CARL, a formal link is established with the HMF model. For both FEL and CARL, calculations are performed with reference to existing experimental devices, namely the FERMI@Elettra FEL under construction at Sincrotrone Trieste (Italy) and the CARL system at LENS in Florence (Italy).

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., Comment: 5 pages, 3 figures

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 momentum variable) and Fourier modes (in configuration variable) converges fast if an appropriate scaling parameter is introduced and identified with the inverse of the system 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 of the Hamiltonian mean-field model.

Systems with long-range interactions display a short-time relaxation towards Quasi Stationary States (QSSs) whose lifetime increases with system size. The application of Lynden-Bell's theory of "violent relaxation" to the Hamiltonian Mean Field model leads to the prediction of out-of-equilibrium first and second order phase transitions between homogeneous (zero magnetization) and inhomogeneous (non-zero magnetization) QSSs, as well as an interesting phenomenon of phase re-entrances. We compare these theoretical predictions with direct $N$-body numerical simulations. We confirm the existence of phase re-entrance in the typical parameter range predicted from Lynden-Bell's theory, but also show that the picture is more complicated than initially thought. In particular, we exhibit the existence of secondary re-entrant phases: we find un-magnetized states in the theoretically magnetized region as well as persisting magnetized states in the theoretically unmagnetized region., Comment: Submitted to Phys. Rev E

The temporal dynamics of a storage-ring Free Electron Laser is here investigated with particular attention to the case in which an external modulation is applied to the laser-electron beam detuning. The system is shown to produce bifurcations, multi-furcations as well as chaotic regimes. The peculiarities of this phenomenon with respect to the analogous behavior displayed by conventional laser sources are pointed out. Theoretical results, obtained by means of a phenomenological model reproducing the evolution of the main statistical parameters of the system, are shown to be in a good agreement with experiments carried out on the Super-ACO Free Electron Laser., Comment: submitted to Europ Phys. Journ. D

Analyses of betatron coupling can be broadly divided into two categories: the matrix approach that decouples the single-turn matrix to reveal the normal modes and the hamiltonian approach that evaluates the coupling in terms of the action of resonances in perturbation theory. The latter is often regarded as being less exact but good for physical insight. The common opinion is that the correction of the two closest sum and difference resonances to the working point is sufficient to reduce the off-axis terms in the 4X4 single-turn matrix, but this is only partially true. The reason for this is explained, and a method is developed that sums to infinity all coupling resonances and, in this way, obtains results equivalent to the matrix approach. The two approaches is discussed with reference to the dynamic aperture. Finally, the extension of the summation method to resonances of all orders is outlined and the relative importance of a single resonance compared to all resonances of a given order is analytically described as a function of the working point., Comment: 22 pages, 10 figures