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Photons have fixed spin and unbounded orbital angular momentum (OAM). While the former is manifested in the polarization of light, the latter corresponds to the spatial phase distribution of its wavefront1. The distinctive way in which the photon spin dictates the electron motion upon light–matter interaction is the basis for numerous well-established spectroscopies. By contrast, imprinting OAM on a matter wave, specifically on a propagating electron, is generally considered very challenging and the anticipated effect undetectable2. In refs. 3,4, the authors provided evidence of OAM-dependent absorption of light by a bound electron. Here, we seek to observe an OAM-dependent dichroic photoelectric effect, using a sample of He atoms. Surprisingly, we find that the OAM of an optical field can be imprinted coherently onto a propagating electron wave. Our results reveal new aspects of light–matter interaction and point to a new kind of single-photon electron spectroscopy.The findings that the spatial distribution of an optical field with vortex phase profile can be imprinted coherently onto a propagating electron wave reveal new aspects of light–matter interactions and will help develop future single-photon electron spectroscopy.

The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within an XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths. Light pulses with controllable parameters are desired for studying the fundamental properties of matter. Here the authors generate and use phase-manipulated and highly time-stable XUV pulse pairs to probe the coherent evolution and dephasing of XUV electronic coherences in helium and argon.

Free-electron lasers producing ultrashort pulses with high peak power promise to extend ultrafast non-linear spectroscopic techniques into the extreme-ultraviolet–X-ray regime. Key aspects are the synchronization between pump and probe, and the control of the pulse properties (duration, intensity and coherence). Externally seeded free-electron lasers produce coherent pulses that can be synchronized with femtosecond accuracy. An important goal is to shorten the pulse duration, but the simple approach of shortening the seed is not sufficient because of the finite-gain bandwidth of the conversion process. An alternative is the amplification of a soliton in a multistage, superradiant cascade: here, we demonstrate the generation of few-femtosecond extreme-ultraviolet pulses, whose duration we measure by autocorrelation. We achieve pulses four times shorter, and with a higher peak power, than in the standard high-gain harmonic generation mode and we prove that the pulse duration matches the Fourier transform limit of the spectral intensity distribution.By amplifying a soliton in a multistage cascade, few-femtosecond extreme-ultraviolet free-electron laser pulses are achieved.

The operation of modern free-electron lasers (FELs) necessitates precise knowledge of electron beam properties at the undulator to ensure the level of control required by increasingly demanding experiments. In seeded FELs, where only electrons interacting with the seed laser contribute to the process, it is crucial to determine the local values of these properties. We present a novel method, based on accurate modeling of the FEL process in high-gain harmonic generation, to accurately retrieve the electron beam slice energy spread, current and laser-induced energy modulation. Understanding these values is essential for enabling advanced FEL schemes and optimally setting advanced seeding schemes such as echo-enabled harmonic generation. We describe the method and provide an experimental application to the FERMI FEL-1, where a slice energy spread in the range 40–100 keV with a few keV accuracy is measured.

We present a numerical study that characterizes the dependence on the radiator length of the output power produced by a free-electron laser (FEL) operated in the high gain harmonic generation (HGHG) configuration. Using the main parameters of the FERMI@Elettra FEL, numerical simulations of the FEL process have been performed for different lengths of the radiator. Our results show that in the case of HGHG the achievable output power has a dependence on the radiator length that is linear. The impact of the electron beam parameters on the achievable maximum power vs radiator length dependence is also studied. A normalization of the results to the FEL saturation power and to the FEL gain length shows that this dependence can be expressed by a universal linear equation that, in some conditions, is independent on the electron beam current and brightness. The reported results could be useful for the design of future FELs based on the HGHG scheme and could be used for a quick estimate of the best undulator length.

Many high-gain free electron lasers worldwide are planning to incorporate seeding setups into their day-to-day operation. These techniques provide both longitudinal and transverse coherence and extended control of the output free electron laser radiation spectral properties. However, the output wavelength and repetition rate strongly depend on the properties of the seed laser system. With the laser peak power required for successful seeded operation, it is currently not possible to increase their repetition rate to an extent that it matches the electron bunch repetition rate of superconducting accelerators. Here, we investigate the advantages of a modification of standard seeding setups, by combining the seeding with the so-called optical klystron. With this new seeding setup, it is possible to decrease the seed laser power requirements and therefore, seed laser systems can increase their repetition rate at the same wavelength. We show simulation results in a high-gain harmonic generation (HGHG) setup for a range of harmonics (8th to 15th) and we verify the reduction of seed laser power required with an Optical Klystron HGHG scheme. Finally, we comment on the stability of the proposed setup to jitter sources and to shot-to-shot fluctuations and compare to the standard HGHG scheme.

Extreme-ultraviolet vortices may be exploited to steer the magnetic properties of nanoparticles, increase the resolution in microscopy, and gain insight into local symmetry and chirality of a material; they might even be used to increase the bandwidth in long-distance space communications. However, in contrast to the generation of vortex beams in the infrared and visible spectral regions, production of intense, extreme-ultraviolet and x-ray optical vortices still remains a challenge. Here, we present an in-situ and an ex-situ technique for generating intense, femtosecond, coherent optical vortices at a free-electron laser in the extreme ultraviolet. The first method takes advantage of nonlinear harmonic generation in a helical undulator, producing vortex beams at the second harmonic without the need for additional optical elements, while the latter one relies on the use of a spiral zone plate to generate a focused, micron-size optical vortex with a peak intensity approaching1014W/cm2, paving the way to nonlinear optical experiments with vortex beams at short wavelengths.

The advent of free-electron laser (FEL) sources delivering two synchronized pulses of different wavelengths (or colours) has made available a whole range of novel pump–probe experiments. This communication describes a major step forward using a new configuration of the FERMI FEL-seeded source to deliver two pulses with different wavelengths, each tunable independently over a broad spectral range with adjustable time delay. The FEL scheme makes use of two seed laser beams of different wavelengths and of a split radiator section to generate two extreme ultraviolet pulses from distinct portions of the same electron bunch. The tunability range of this new two-colour source meets the requirements of double-resonant FEL pump/FEL probe time-resolved studies. We demonstrate its performance in a proof-of-principle magnetic scattering experiment in Fe–Ni compounds, by tuning the FEL wavelengths to the Fe and Ni 3 p resonances. Two-colour X-ray free electron laser is a powerful tool for pump–probe measurements, but currently constrained by limited tunability. Here, Ferrari et al . develop a configuration that allows tuning both the pump and the probe to specific electronic excitations, providing element selectivity.

Intense ultrashort X-ray pulses produced by modern free-electron lasers (FELs) allow one to probe biological systems, inorganic materials and molecular reaction dynamics with nanoscale spatial and femtoscale temporal resolution. These experiments require the knowledge, and possibly the control, of the spectro-temporal content of individual pulses. FELs relying on seeding have the potential to produce spatially and temporally fully coherent pulses. Here we propose and implement an interferometric method, which allows us to carry out the first complete single-shot spectro-temporal characterization of the pulses, generated by an FEL in the extreme ultraviolet spectral range. Moreover, we provide the first direct evidence of the temporal coherence of a seeded FEL working in the extreme ultraviolet spectral range and show the way to control the light generation process to produce Fourier-limited pulses. Experiments are carried out at the FERMI FEL in Trieste. X-ray free-electron laser is a power probe for materials, but it is challenging to measure the spectro-temporal characters of individual pulses. Here, De Ninno et al. implement an interferometric method allowing one to characterize and control the ultrashort XUV pulses seeded by a femtosecond laser.

Light manipulation at the nanoscale is essential both for fundamental science and modern technology. The quest to shorter lengthscales, however, requires the use of light wavelengths beyond the visible. In particular, in the extreme ultraviolet regime these manipulation capabilities are hampered by the lack of efficient optics, especially for polarization control. Here, we present a method to create periodic, polarization modulations at the nanoscale using a tailored configuration of the FERMI free electron laser and demonstrate its capabilities by comparing the dynamics induced by this polarization transient grating with those driven by a conventional intensity grating on a thin ferrimagnetic alloy. While the intensity grating signal is dominated by the thermoelastic response, the polarization grating excitation minimizes it, uncovering helicity-dependent responses previously undetected. We anticipate nanoscale polarization transient gratings to become useful for the study of physical, chemical and biological systems possessing chiral symmetry. This study presents a method to create nanoscale polarization transient gratings in the EUV range. Unlike intensity gratings, it reduces thermal effects, revealing hidden material dynamics. This enables new insights in chiral materials and ultrafast magnetism.