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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.

Free-electron lasers (FELs) are the world's most brilliant light sources with rapidly evolving technological capabilities in terms of ultrabright and ultrashort pulses over a large range of accessible photon energies. Their revolutionary and innovative developments have opened new fields of science regarding nonlinear light-matter interaction, the investigation of ultrafast processes from specific observer sites, and approaches to imaging matter with atomic resolution. A core aspect of FEL science is the study of isolated and prototypical systems in the gas phase with the possibility of addressing well-defined electronic transitions or particular atomic sites in molecules. Notably for polarization-controlled short-wavelength FELs, the gas phase offers new avenues for investigations of nonlinear and ultrafast phenomena in spin orientated systems, for decoding the function of the chiral building blocks of life as well as steering reactions and particle emission dynamics in otherwise inaccessible ways. This roadmap comprises descriptions of technological capabilities of facilities worldwide, innovative diagnostics and instrumentation, as well as recent scientific highlights, novel methodology and mathematical modeling. The experimental and theoretical landscape of using polarization controllable FELs for dichroic light-matter interaction in the gas phase will be discussed and comprehensively outlined to stimulate and strengthen global collaborative efforts of all disciplines.

We present the generation of transient polarization gratings at the nanoscale, achieved using a tailored accelerator configuration of the FERMI free electron laser. We demonstrate the capabilities of such a transient polarization grating by comparing its induced dynamics with the ones triggered by a more conventional intensity grating on a thin film ferrimagnetic alloy. While the signal of the intensity grating is dominated by the thermoelastic response of the system, such a contribution is suppressed in the case of the polarization grating. This exposes helicity-dependent magnetization dynamics that have so-far remained hidden under the large thermally driven response. We anticipate nanoscale transient polarization gratings to become useful for the study of any physical, chemical and biological systems possessing chiral symmetry.

Complex systems are characterized by strong coupling between different microscopic degrees of freedom. Photoexcitation of such materials can drive them into new transient and long-lived hidden phases that may not have any counterparts in equilibrium. By exploiting femtosecond time- and angle-resolved photoemission spectroscopy, we probe the photoinduced transient phase and the recovery dynamics of the ground state in a complex material: the charge density wave (CDW)-Mott insulator 1$T$-TaS$_2$. We reveal striking similarities between the band structures of the transient phase and the (equilibrium) structurally undistorted metallic phase, with evidence for the coexistence of the low-temperature Mott insulating phase and high-temperature metallic phase. Following the transient phase, we find that the restoration of the Mott and CDW order begins around the same time. This highlights that the Mott transition is tied to the CDW structural distortion, although earlier studies have shown that the collapse of Mott and CDW phases are decoupled from each other. Interestingly, as the suppressed order starts to recover, a long-lived metastable phase emerges before the material recovers to the ground state. Our results demonstrate that it is the CDW lattice order that drives the material into this metastable phase, which is indeed a commensurate CDW-Mott insulating phase but with a smaller CDW amplitude. Moreover, we find that the long-lived state emerges only under strong photoexcitation and has no evidence when the photoexcitation strength is weak.

We present an angle-resolved photoemission study of the electronic band structure of the excitonic insulator Ta$_2$NiSe$_5$, as well as its evolution upon Sulfur doping. Our experimental data show that while the excitonic insulating phase is still preserved at a Sulfur-doping level of 25$\%$, such phase is heavily suppressed when there is a substantial amount, $\sim$ 50$\%$, of S-doping at liquid nitrogen temperatures. Moreover, our photon energy-dependent measurements reveal a clear three dimensionality of the electronic structure, both in Ta$_2$NiSe$_5$ and Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$ ($x=0.25, 0.50$) compounds. This suggests a reduction of electrical and thermal conductivities, which might make these compounds less suitable for electronic transport applications.

Crack initiation governs high cycle fatigue life and is susceptible to microstructural details. While corresponding microstructure-sensitive models are available, their validation is difficult. We propose a validation framework where a fatigue test is mimicked in a sub-modeling simulation by embedding the measured microstructure into the specimen geometry and adopting the experimental boundary conditions. Exemplary, a phenomenological crystal plasticity model was applied to predict deformation in ferritic steel (EN1.4003). Hotspots in commonly used fatigue indicator parameter maps are compared with damage segmented from micrographs. Along with the data, the framework is published for benchmarking future micromechanical fatigue models.

Understanding how a spin current flows across metal-semiconductor interfaces at pico- and femtosecond timescales has implications for ultrafast spintronics, data processing and storage applications. However, the possibility to directly access the propagation of spin currents on such time scales has been hampered by the simultaneous lack of both ultrafast element specific magnetic sensitive probes and tailored metal-semiconductor interfaces. Here, by means of free electron laser-based element sensitive Kerr spectroscopy, we report direct experimental evidence of spin currents across a Ni/Si interface in the form of different magnetodynamics at the Ni M2,3 and Si L2,3 absorption edges. This further allows us to calculate the propagation velocity of the spin current in silicon, which is on the order of 0.2 nm/fs.

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.

We report on the experimental evidence of magnetic helicoidal dichroism, observed in the interaction of an extreme ultraviolet vortex beam carrying orbital angular momentum with a magnetic vortex. Numerical simulations based on classical electromagnetic theory show that this dichroism is based on the interference of light modes with different orbital angular momenta, which are populated after the interaction between the light phase chirality and the magnetic topology. This observation gives insight into the interplay between orbital angular momentum and magnetism, and sets the framework for the development of new analytical tools to investigate ultrafast magnetization dynamics., Comment: 7 pages, 4 figures

We investigate the non-equilibrium electronic structure and characteristic time scales in a candidate excitonic insulator, Ta$_2$NiSe$_5$, using time- and angle-resolved photoemission spectroscopy with a temporal resolution of 50 fs. Following a strong photoexcitation, the band gap closes transiently within 100 fs, i.e., on a time scale faster than the typical lattice vibrational period. Furthermore, we find that the characteristic time associated with the rise of the photoemission intensity above the Fermi energy decreases with increasing excitation strength, while the relaxation time of the electron population towards equilibrium shows an opposite behaviour. We argue that these experimental observations can be consistently explained by an excitonic origin of the band gap in the material. The excitonic picture is supported by microscopic calculations based on the non-equilibrium Green's function formalism for an interacting two-band system. We interpret the speedup of the rise time with fluence in terms of an enhanced scattering probability between photo-excited electrons and excitons, leading to an initially faster decay of the order parameter. We show that the inclusion of electron-phonon coupling at a semi-classical level changes only the quantitative aspects of the proposed dynamics, while the qualitative features remain the same. The experimental observations and microscopic calculations allow us to develop a simple and intuitive phenomenological model that captures the main dynamics after photoexcitation in Ta$_2$NiSe$_5$.

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

Collinear double-pulse seeding of the High-Gain Harmonic Generation (HGHG) process in a free-electron laser (FEL) is a promising approach to facilitate various coherent nonlinear spectroscopy schemes in the extreme ultraviolet (XUV) spectral range. However, in collinear arrangements using a single nonlinear medium, temporally overlapping seed pulses may introduce nonlinear mixing signals that compromise the experiment at short time delays. Here, we investigate these effects in detail by extending the analysis described in a recent publication (Wituschek et al., Nat. Commun., 11, 883, 2020). High-order fringe-resolved autocorrelation and wave-packet interferometry experiments at photon energies > $23\,$eV are performed, accompanied by numerical simulations. It turns out that both the autocorrelation and the wave-packet interferometry data are very sensitive to saturation effects and can thus be used to characterize saturation in the HGHG process. Our results further imply that time-resolved spectroscopy experiments are feasible even for time delays smaller than the seed pulse duration., Comment: This is accepted version of the article. The Version of Record is available online at https://doi.org/10.1364/OE.401249

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 edges 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. 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.

Quantum materials display exotic behaviours related to the interplay between temperature-driven phase transitions. Here, we study electron dynamics in one such material, CaFe2As2, a parent Fe-based superconductor, employing time and angle-resolved photoemission spectroscopy. CaFe2As2 exhibits concomitant transition to spin density wave state and nematic order below 170 K. We discover that magnetic excitations can be induced selectively, by using polarized pump pulses, significantly before the destruction of nematic order. More specifically, we observe that s-polarized light enhances electron temperature by several hundreds of degrees at a time scale of about 200 fs, while the temperature of the electrons participating in magnetic order can be enhanced by similar amount at a much faster time scale (50 fs) using p-polarized pump pulse. These results provide a pathway to achieve selective electron heating, which is not possible with other methods, as well as to disentangle phase transitions in quantum materials.

In the Falicov-Kimball model, a model for (annealed) disorder, we expect weak localization corrections to the optical conductivity. However, we get such weak localization effects only when employing a pp-ladder approximation in the dual fermion approach. In the full parquet approach these pp-contributions are suppressed by ph-reducible diagrams. For the optical conductivity, we find that the pht-channel yields the main contribution, even in the region where weak localization in the pp-ladder was indicated., Comment: 11 pages, 17 figures

Quantum mechanically, photoionization can be fully described by the complex photoionization amplitudes that describe the transition between the ground state and the continuum state. Knowledge of the value of the phase of these amplitudes has been a central interest in photoionization studies and newly developing attosecond science, since the phase can reveal important information about phenomena such as electron correlation. We present a new attosecond-precision interferometric method of angle-resolved measurement for the phase of the photoionization amplitudes, using two phase-locked Extreme Ultraviolet pulses of frequency $\omega$ and $2\omega$, from a Free-Electron Laser. Phase differences $\Delta \tilde \eta$ between one- and two-photon ionization channels, averaged over multiple wave packets, are extracted for neon $2p$ electrons as a function of emission angle at photoelectron energies 7.9, 10.2, and 16.6 eV. $\Delta \tilde \eta$ is nearly constant for emission parallel to the electric vector but increases at 10.2 eV for emission perpendicular to the electric vector. We model our observations with both perturbation and \textit{ab initio} theory, and find excellent agreement. In the existing method for attosecond measurement, Reconstruction of Attosecond Beating By Interference of Two-photon Transitions (RABBITT), a phase difference between two-photon pathways involving absorption and emission of an infrared photon is extracted. Our method can be used for extraction of a phase difference between single-photon and two-photon pathways and provides a new tool for attosecond science, which is complementary to RABBITT.

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 a 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., Comment: This is the accepted version of the article. The Version of Record is available online at 10.1038/s41467-020-14721-2

The interaction of light with solids gives rise to new bosonic quasiparticles, with the exciton being---undoubtedly---the most famous of these polaritons. While excitons are the generic polaritons of semiconductors, we show that for strongly correlated systems another polariton is prevalent---originating from the dominant antiferromagnetic or charge density wave fluctuations in these systems. As these are usually associated with a wave vector ${\mathbf k}= (\pi,\pi,\ldots)$ or close to it, we propose to call the derived polaritons $\pi$-tons. These $\pi$-tons yield the leading vertex correction to the optical conductivity in all correlated models studied: the Hubbard, the extended Hubbard model, the Falicov-Kimball, and the Pariser-Parr-Pople model, both in the insulating and in the metallic phase., Comment: 6 pages, 3 figures + Supplemental Material (6 pages, 8 figures)

The dual fermion (DF) method allows for calculating corrections due to non-local correlations relative to an effective impurity model. Choosing the impurity as that of a dynamical mean field theory (DMFT) solution at self-consistency is popular, and the corrections from dual fermion theory are physically meaningful. We investigate the effect of choosing the impurity instead in a self-consistent manner and find for the two dimensional Hubbard model an exponentially increase of the correlation length and susceptibility at low temperatures. There are pronounced differences for the two self-consistency schemes that are discussed in the literature; the self-consistent DF solution can even be more metallic than the DMFT solution., Comment: 8 pages, 10 figures

We show the existence of many infinite classes of permutations over finite fields and bent functions by extending the notion of linear translators, introduced by Kyureghyan [12]. We call these translators Frobenius translators since the derivatives of $f : F_{p^n} \rightarrow F_{p^k}$, where $n = rk$, are of the form $f(x + u\phi) - f(x) = u^{p^i}b$, for a fixed $b \in F_{p^k}$ and all $u \in F_{p^k}$, rather than considering the standard case corresponding to $i = 0$. This considerably extends a rather rare family {f} admitting linear translators of the above form. Furthermore, we solve a few open problems in the recent article [4] concerning the existence and an exact specification of $f$ admitting classical linear translators, and an open problem introduced in [9] of finding a triple of bent functions $f_1, f_2, f_3$ such that their sum $f_4$ is bent and that the sum of their duals $f_1* +f_2* +f_3* +f_4* = 1$. Finally, we also specify two huge families of permutations over $F_{p^n}$ related to the condition that $G(y) = -L(y)+(y+\delta)^s -(y+\delta)^{p^ks}$ permutes the set $S =\{\beta \in F_{p^n} : Tr^n_k(\beta) = 0\}$, where $n = 2k$ and $p > 2$. Finally, we offer generalizations of constructions of bent functions from [16] and described some new bent families using the permutations found in [4].

We report on orbital-dependent quasiparticle dynamics in EuFe$_2$As$_2$, a parent compound of Fe-based superconductors and a novel way to experimentally identify this behavior, using time- and angle-resolved photoelectron spectroscopy across the spin density wave transition. We observe two different relaxation time scales for photo-excited d$_x$$_z$/d$_y$$_z$ and d$_x$$_y$ electrons. While d$_x$$_z$/d$_y$$_z$ electrons relax faster through the electron-electron scattering channel, showing an itinerant character, d$_x$$_y$ electrons form a quasi-equilibrium state with the lattice due to their localized character, and the state decays slowly. Our findings suggest that electron correlation in Fe-pnictides is an important property, which should be taken into careful account when describing the electronic properties of both parent and electron-doped compounds, and therefore establish a strong connection with cuprates.