Generation of entanglement using a short-wavelength seeded free-electron laser.

Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance.

Wave packet dynamics and control in excited states of molecular nitrogen.

Wave packet interferometry with vacuum ultraviolet light has been used to probe a complex region of the electronic spectrum of molecular nitrogen, N2. Wave packets of Rydberg and valence states were excited by using double pulses of vacuum ultraviolet (VUV), free-electron-laser (FEL) light. These wave packets were composed of contributions from multiple electronic states with a moderate principal quantum number (n ∼ 4-9) and a range of vibrational and rotational quantum numbers. The phase relationship of the two FEL pulses varied in time, but as demonstrated previously, a shot-by-shot analysis allows the spectra to be sorted according to the phase between the two pulses. The wave packets were probed by angle-resolved photoionization using an infrared pulse with a variable delay after the pair of excitation pulses. The photoelectron branching fractions and angular distributions display oscillations that depend on both the time delays and the relative phases of the VUV pulses. The combination of frequency, time delay, and phase selection provides significant control over the ionization process and ultimately improves the ability to analyze and assign complex molecular spectra.

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.

The MagneDyn beamline at the FERMI free electron laser.

The scope of this paper is to outline the main marks and performances of the MagneDyn beamline, which was designed and built to perform ultrafast magnetodynamic studies in solids. Open to users since 2019, MagneDyn operates with variable circular and linear polarized femtosecond pulses delivered by the externally laser-seeded FERMI free-electron laser (FEL). The very high degree of polarization, the high pulse-to-pulse stability, and the photon energy tunability in the 50-300 eV range allow performing advanced time-resolved magnetic dichroic experiments at the K-edge of light elements, e.g., carbon and at the M- and N-edge of the 3d-transition-metals and rare earth elements, respectively. To this end, two experimental end-stations are available. The first is equipped with an in situ dedicated electromagnet, a cryostat, and an extreme ultraviolet Wollaston-like polarimeter. The second, designed for carry-in user instruments, hosts also a spectrometer for pump-probe resonant x-ray emission and inelastic spectroscopy experiments with a sub-eV energy resolution. A Kirkpatrick-Baez active optics system provides a minimum focus of ∼20×20µm2 FWHM at the sample. A pump laser setup, synchronized with the FEL-laser seeding system, delivers sub-picosecond pulses with photon energies ranging from the mid-IR to near-UV for optical pump-FEL probe experiments with a minimal pump-probe jitter of few femtoseconds. The overall combination of these features renders MagneDyn a unique state-of-the-art tool for studying ultrafast magnetic and resonant emission phenomena in solids.

Observation of Rabi dynamics with a short-wavelength free-electron laser.

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light-matter interactions within the rotating-wave approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7-9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler-Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom-field interactions11. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

Time-Resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-Doped Helium Nanodroplets.

The autoionization dynamics of superexcited superfluid He nanodroplets doped with Na atoms is studied by extreme-ultraviolet (XUV) time-resolved electron spectroscopy. Following excitation into the higher-lying droplet absorption band, the droplet relaxes into the lowest metastable atomic 1s2s 1,3S states from which interatomic Coulombic decay (ICD) takes place either between two excited He atoms or between an excited He atom and a Na atom attached to the droplet surface. Four main ICD channels are identified, and their decay times are determined by varying the delay between the XUV pulse and a UV pulse that ionizes the initial excited state and thereby quenches ICD. The decay times for the different channels all fall in the range of ∼1 ps, indicating that the ICD dynamics are mainly determined by the droplet environment. A periodic modulation of the transient ICD signals is tentatively attributed to the oscillation of the bubble forming around the localized He excitation.

Light-Induced Magnetization at the Nanoscale.

Triggering and switching magnetic moments is of key importance for applications ranging from spintronics to quantum information. A noninvasive ultrafast control at the nanoscale is, however, an open challenge. Here, we propose a novel laser-based scheme for generating atomic-scale charge current loops within femtoseconds. The associated orbital magnetic moments remain ferromagnetically aligned after the laser pulses have ceased and are localized within an area that is tunable via laser parameters and can be chosen to be well below the diffraction limit of the driving laser field. The scheme relies on tuning the phase, polarization, and intensities of two copropagating Gaussian and vortex laser pulses, allowing us to control the spatial extent, direction, and strength of the atomic-scale charge current loops induced in the irradiated sample upon photon absorption. In the experiment we used He atoms driven by an ultraviolet and infrared vortex-beam laser pulses to generate current-carrying Rydberg states and test for the generated magnetic moments via dichroic effects in photoemission. Ab initio quantum dynamic simulations and analysis confirm the proposed scenario and provide a quantitative estimate of the generated local moments.

Tomography of a seeded free-electron laser focal spot: qualitative and quantitative comparison of two reconstruction methods for spot size characterization.

Performing experiments at free-electron lasers (FELs) requires an exhaustive knowledge of the pulse temporal and spectral profile, as well as the focal spot shape and size. Operating FELs in the extreme ultraviolet (EUV) and soft X-ray (SXR) spectral regions calls for designing ad-hoc optical layouts to transport and characterize the EUV/SXR beam, as well as tailoring its spatial dimensions at the focal plane down to sizes in the few micrometers range. At the FERMI FEL (Trieste, Italy) this task is carried out by the Photon Analysis Delivery and Reduction System (PADReS). In particular, to meet the different experimental requests on the focal spot shape and size, a proper tuning of the optical systems is required, and this should be monitored by means of dedicated techniques. Here, we present and compare two reconstruction methods for spot characterization: single-shot imprints captured via ablation on a poly(methyl methacrylate) sample (PMMA) and pulse profiles retrieved by means of a Hartmann wavefront sensor (WFS). By recording complementary datasets at and nearby the focal plane, we exploit the tomography of the pulse profile along the beam propagation axis, as well as a qualitative and quantitative comparison between these two reconstruction methods.

Unravelling the full relaxation dynamics of superexcited helium nanodroplets.

The relaxation dynamics of superexcited superfluid He nanodroplets is thoroughly investigated by means of extreme-ultraviolet (XUV) femtosecond electron and ion spectroscopy complemented by time-dependent density functional theory (TDDFT). Three main paths leading to the emission of electrons and ions are identified: droplet autoionization, pump-probe photoionization, and autoionization induced by re-excitation of droplets relaxing into levels below the droplet ionization threshold. The most abundant product ions are He2+, generated by droplet autoionization and by photoionization of droplet-bound excited He atoms. He+ appear with some pump-probe delay as a result of the ejection He atoms in their lowest excited states from the droplets. The state-resolved time-dependent photoelectron spectra reveal that intermediate excited states of the droplets are populated in the course of the relaxation, terminating in the lowest-lying metastable singlet and triplet He atomic states. The slightly faster relaxation of the triplet state compared to the singlet state is in agreement with the simulation showing faster formation of a bubble around a He atom in the triplet state.

A novel free-electron laser single-pulse Wollaston polarimeter for magneto-dynamical studies.

Here, we report on the conceptual design, the hardware realization, and the first experimental results of a novel and compact x-ray polarimeter capable of a single-pulse linear polarization angle detection in the extreme ultraviolet photon energy range. The polarimeter is tested by performing time resolved pump-probe experiments on a Ni80Fe20 Permalloy film at the M2,3 Ni edge at an externally seeded free-electron laser source. Comparison with similar experiments reported in the literature shows the advantages of our approach also in view of future experiments.

Time-resolved photoelectron imaging of complex resonances in molecular nitrogen.

We have used the FERMI free-electron laser to perform time-resolved photoelectron imaging experiments on a complex group of resonances near 15.38 eV in the absorption spectrum of molecular nitrogen, N2, under jet-cooled conditions. The new data complement and extend the earlier work of Fushitani et al. [Opt. Express 27, 19702-19711 (2019)], who recorded time-resolved photoelectron spectra for this same group of resonances. Time-dependent oscillations are observed in both the photoelectron yields and the photoelectron angular distributions, providing insight into the interactions among the resonant intermediate states. In addition, for most states, we observe an exponential decay of the photoelectron yield that depends on the ionic final state. This observation can be rationalized by the different lifetimes for the intermediate states contributing to a particular ionization channel. Although there are nine resonances within the group, we show that by detecting individual photoelectron final states and their angular dependence, we can identify and differentiate quantum pathways within this complex system.

Simultaneous two-color snapshot view on ultrafast charge and spin dynamics in a Fe-Cu-Ni tri-layer.

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements, where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Here, we report on an experiment using a dedicated optical element and the two-color emission of the FERMI XUV free-electron laser to follow the charge and spin dynamics in composite materials at two distinct absorption edges, simultaneously. The sample, consisting of ferromagnetic Fe and Ni layers, separated by a Cu layer, is pumped by an infrared laser and probed by a two-color XUV pulse with photon energies tuned to the M-shell resonances of these two transition metals. The experimental geometry intrinsically avoids any timing uncertainty between the two elements and unambiguously reveals an approximately 100 fs delay of the magnetic response with respect to the electronic excitation for both Fe and Ni. This delay shows that the electronic and spin degrees of freedom are decoupled during the demagnetization process. We furthermore observe that the electronic dynamics of Ni and Fe show pronounced differences when probed at their resonance, while the demagnetization dynamics are similar. These observations underline the importance of simultaneous investigation of the temporal response of both charge and spin in multi-component materials. In a more general scenario, the experimental approach can be extended to continuous energy ranges, promising the development of jitter-free transient absorption spectroscopy in the XUV and soft X-ray regimes.

Kirkpatrick-Baez active optics system at FERMI: system performance analysis.

FERMI is the first and only seeded EUV-SXR free-electron laser (FEL) facility available to users; it operates at Elettra - Sincrotrone Trieste (Italy) and it presents five operating endstations. Three of them, namely LDM (Low Density Matter), DiProI (Diffraction and Projection Imaging) and MagneDyn (Magneto-Dynamical studies), use a Kirkpatrick-Baez (KB) active X-ray optics system to focus the FEL pulses into the experimental chambers. The present work reports on the final results of the upgraded KB Active Optics Systems (KAOS), which have been mechanically modified in order to improve stability and repeatability with respect to the original design. The results have been obtained on both the FERMI FEL lines, FEL1 and FEL2, and are particularly relevant for the latter as it is the low-wavelength line recently opened to users. After a thorough description of the new mechanical layout of the system and the aspects that have been improved after the refurbishment, a set of simulations of the optical performances are presented. The code used to simulate the behavior of KAOS is WISEr, a physical-optics-based tool, which is freely accessible, and integrated into the Oasys platform, that takes into account the specific surface metrology characterization of the beamline mirrors, including figure errors and microroughness power spectral density. The results of WISEr are then used as a reference for the actual optimization of the optical system. This procedure relies heavily on a wavefront sensor (WFS) mounted out of focus to optimize the refocusing mirrors alignment as well as their curvature bending (by minimization of the coefficients of the Zernike wavefront expansion). Moreover, the WFS data are used to reconstruct the focal spot parameters by means of a back-propagation of the electric field. Finally, these results are compared with those obtained after the FEL ablation of a PMMA layer positioned on the focal plane, and analyzed ex situ in a post-mortem fashion. The mechanically refurbished optical system and the multi-technique alignment approach, aimed at optimizing the mirrors' curvature, pitch and roll angles, allowed a focal spot of 1.8 µm × 2.4 µm at 4.14 nm wavelength (FEL2) to be inferred, confirmed by the PMMA ablation imprints.

Focal shift induced by source displacements and optical figure errors.

In this work the longitudinal shifts of the focal plane of an ellipsoidal mirror induced by longitudinal shifts of the source and by the optical figure error of the mirror itself are investigated. The case of an ideal mirror illuminated by a Gaussian beam is considered first, deriving an analytical formula predicting the source-to-focus shift. Then the realistic case of a mirror affected by surface shape defects is examined, by taking into account metrological data and numerically solving the Huygens-Fresnel integral. The analytical and numerical solutions in the ideal and real cases are compared. Finally, it is shown that an additional dependence of the focal shift is introduced on the wavelength and the pointing angle of the source. Both effects are investigated by numerical computations. We limit the treatment in the XUV spectral range, choosing as a test bench the Kirkpatrick-Baez mirror system of the DiProI and LDM end-stations and at the FERMI seeded free-electron laser (FEL). The work is primarily aimed at disentangling the different causes of focal shift at FEL light sources, where source position, wavelength and pointing angle are either tunable or rapidly fluctuating. The method can be easily extended to parabolic reflectors and refractors (lenses) with other kinds of illuminating sources and wavelengths.

Towards chemically neutral carbon cleaning processes: plasma cleaning of Ni, Rh and Al reflective optical coatings and thin Al filters for free-electron lasers and synchrotron beamline applications.

The choice of a reflective optical coating or filter material has to be adapted to the intended field of application. This is mainly determined by the required photon energy range or by the required reflection angle. Among various materials, nickel and rhodium are common materials used as reflective coatings for (soft) X-ray mirrors. Similarly, aluminium is one of the most commonly used materials for extreme ultraviolet and soft X-ray transmission filters. However, both of these types of optics are subject to carbon contamination, which can be increasingly problematic for the operation of the high-performance free-electron laser and synchrotron beamlines. As an attempt to remove this type of contamination, an inductively coupled plasma source has been used in conjunction with N2/O2/H2 and N2/H2 feedstock gas plasmas. Results from the chemical surface analysis of the above materials before and after plasma treatment using X-ray photoelectron spectroscopy are reported. It is concluded that a favorable combination of an N2/H2 plasma feedstock gas mixture leads to the best chemical surface preservation of Ni, Rh and Al while removing the carbon contamination. However, this feedstock gas mixture does not remove C contamination as rapidly as, for example, an N2/O2/H2 plasma which induces the surface formation of NiO and NiOOH in Ni and RhOOH in Rh foils. As an applied case, the successful carbon removal from ultrathin Al filters previously used at the FERMI FEL1 using an N2/H2 plasma is demonstrated.

In situ single-shot diffractive fluence mapping for X-ray free-electron laser pulses.

Free-electron lasers (FELs) in the extreme ultraviolet (XUV) and X-ray regime opened up the possibility for experiments at high power densities, in particular allowing for fluence-dependent absorption and scattering experiments to reveal non-linear light-matter interactions at ever shorter wavelengths. Findings of such non-linear effects are met with tremendous interest, but prove difficult to understand and model due to the inherent shot-to-shot fluctuations in photon intensity and the often structured, non-Gaussian spatial intensity profile of a focused FEL beam. Presently, the focused beam is characterized and optimized separately from the actual experiment. Here, we present the simultaneous measurement of XUV diffraction signals from solid samples in tandem with the corresponding single-shot spatial fluence distribution on the actual sample. Our in situ characterization scheme enables direct monitoring of the sample illumination, providing a basis to optimize and quantitatively understand FEL experiments.

PhotonDiag2017 workshop: introductory overview.

This issue of the Journal of Synchrotron Radiation is a special issue including papers from the PhotonDiag2017 workshop. Here, a brief introduction is given.

Timing methodologies and studies at the FERMI free-electron laser.

Time-resolved investigations have begun a new era of chemistry and physics, enabling the monitoring in real time of the dynamics of chemical reactions and matter. Induced transient optical absorption is a basic ultrafast electronic effect, originated by a partial depletion of the valence band, that can be triggered by exposing insulators and semiconductors to sub-picosecond extreme-ultraviolet pulses. Besides its scientific and fundamental implications, this process is very important as it is routinely applied in free-electron laser (FEL) facilities to achieve the temporal superposition between FEL and optical laser pulses with tens of femtoseconds accuracy. Here, a set of methodologies developed at the FERMI facility based on ultrafast effects in condensed materials and employed to effectively determine the FEL/laser cross correlation are presented.

High resolution beam profiling of X-ray free electron laser radiation by polymer imprint development.

High resolution metrology of beam profiles is presently a major challenge at X-ray free electron lasers. We demonstrate a characterization method based on beam imprints in poly (methyl methacrylate). By immersing the imprints formed at 47.8 eV into organic solvents, the regions exposed to the beam are removed similar to resist development in grayscale lithography. This allows for extending the sensitivity of the method by more than an order of magnitude compared to the established analysis of imprints created solely by ablation. Applying the Beer-Lambert law for absorption, the intensity distribution in a micron-sized focus can be reconstructed from one single shot with a high dynamic range, exceeding 103. The procedure described here allows for beam characterization at free electron lasers revealing even faint beam tails, which are not accessible when using ablation imprint methods. We demonstrate the greatly extended dynamic range on developed imprints taken in focus of conventional Fresnel zone plates and spiral zone plates producing beams with a topological charge.