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Angular streaking experiments enable for experimentation in the attosecond regions. However, the deployed Time-of-flight detectors are susceptible to noise and failure. These shortcomings make the outputs of the Time-of-flight detectors hard to understand for humans and further processing, such as for example the extraction of beam properties. In this article, we present an approach to remove high noise levels and reconstruct up to three failed Time-of-flight detectors from an arrangement of 16 Time-of-flight detectors. Due to its fast evaluation time, the presented method is applicable online during a running experiment. It is trained with simulation data, and we show the results of denoising and reconstruction of our method on real-world experiment data., Comment: Submitted to APS Physical Review Accelerators and Beams

Attosecond X-ray pulses are the key to studying electron dynamics at their natural timescale in specifically targeted electronic states. They promise to build the conceptual bridge between physical and chemical photo-reaction processes. Free-electron lasers (FELs) have demonstrated their capability of generating intense attosecond X-ray pulses. The use of SASE-based FELs for time-resolving experiments and investigations of nonlinear X-ray absorption mechanisms, however, necessitates their full pulse-to-pulse characterisation which remains a cutting-edge challenge. We have characterised X-ray pulses with durations of down to 600 attoseconds and peak powers up to 200 GW at ~1 keV photon energy via angular streaking at the Small Quantum Systems instrument of the European XFEL in Germany. As a direct application, we present results of nonlinear X-ray--matter interaction via time-resolved electron spectroscopy on a transient system, observing single- and double-core-hole generation in neon atoms. Using the derived temporal information about each single X-ray pulse, we reveal an otherwise hidden peak-intensity dependence of the probability for formation of double-core vacancies in neon after primary K-shell ionisation. Our results advance the field of attosecond science with highly intense and fully characterised X-ray pulses to the state-specific investigation of electronic motion in non-stationary media.

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.

The toolbox for time-resolved direct measurements of electron dynamics covers a variety of methods. Since the experimental effort is increasing rapidly with achievable time resolution, there is an urge for simple and robust measurement techniques. Within this paper prove of concept experiments and numerical simulations are utilized to investigate the applicability of a new setup for the generation of ultrashort electron pulses in the energy range of 300 eV up to 1.6 keV. The experimental approach combines an in-vacuum liquid microjet and a few-cycle femtosecond laser system, while the threshold for electron impact ionization serves as a gate for the effective electron pulse duration. The experiments prove that electrons in the keV regime are accessible and that the electron spectrum can be easily tuned by laser intensity and focal position alignment with respect to the water jet. Numerical simulations show that a sub-picosecond temporal resolution is achievable., Comment: 13 Pages, 6 Fugures

X-ray free-electron lasers (XFELs) as the world's brightest light sources provide ultrashort X-ray pulses with a duration typically in the order of femtoseconds. Recently, they have approached and entered the attosecond regime, which holds new promises for single-molecule imaging and studying nonlinear and ultrafast phenomena such as localized electron dynamics. The technological evolution of XFELs toward well-controllable light sources for precise metrology of ultrafast processes has been, however, hampered by the diagnostic capabilities for characterizing X-ray pulses at the attosecond frontier. In this regard, the spectroscopic technique of photoelectron angular streaking has successfully proven how to non-destructively retrieve the exact time-energy structure of XFEL pulses on a single-shot basis. By using artificial intelligence techniques, in particular convolutional neural networks, we here show how this technique can be leveraged from its proof-of-principle stage toward routine diagnostics even at high-repetition-rate XFELs, thus enhancing and refining their scientific accessibility in all related disciplines., Comment: This version includes Supplementary Information

In quantum systems, coherent superpositions of electronic states evolve on ultrafast timescales (few femtosecond to attosecond, 1 as = 0.001 fs = 10^{-18} s), leading to a time dependent charge density. Here we exploit the first attosecond soft x-ray pulses produced by an x-ray free-electron laser to induce a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse we create a clock to time-resolve the electron dynamics, and demonstrate control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter.

We report the design of an angular array of electron Time-of-Flight (eToF) spectrometers intended for non-invasive spectral, temporal, and polarization characterization of single shots of high-repetition rate, quasi-continuous, short-wavelength Free-Electron Lasers (FELs) such as the LCLS-II at SLAC. This array also enables angle-resolved, high-resolution eToF spectroscopy to address a variety of scientific questions of ultrafast and nonlinear light--matter interaction at FELs. The presented device is specifically designed for the Time-resolved atomic, Molecular and Optical science end station (TMO) at LCLS-II. In its final version, it can comprise of up to 20 eToF spectrometers aligned to collect electrons from the interaction point defined by the intersection of the incoming FEL radiation and a gaseous target. There are 16 such spectrometers forming a circular equiangular array in the plane normal to x-ray propagation and 4 spectrometers at 54.7$^\circ$ angle relative to the principle linear x-ray polarization axis. The spectrometers are capable of independent and minimally chromatic electrostatic lensing and retardation in order to enable simultaneous angle-resolved photo-electron and Auger electron spectroscopy with high energy resolution. They are designed to ensure energy resolution of 0.25 eV across an energy window of up to 75 eV which can be individually centered via the adjustable retardation to cover ranges of electron kinetic energies relevant to soft x-ray methods, 0--2 keV. The full spectrometer array will enable non-invasive and online spectral-polarimetry measurements, polarization-sensitive attoclock spectroscopy for characterizing the full time--energy structure of even SASE or seeded LCLS-II pulses, and also supports emerging trends in molecular frame spectroscopy measurements., Comment: under review

Short-wavelength free-electron lasers with their ultrashort pulses at high intensities have originated new approaches for tracking molecular dynamics from the vista of specific sites. X-ray pump X-ray probe schemes even allow to address individual atomic constituents with a 'trigger'-event that preludes the subsequent molecular dynamics while being able to selectively probe the evolving structure with a time-delayed second X-ray pulse. Here, we use a linearly polarized X-ray photon to trigger the photolysis of a prototypical chiral molecule, namely trifluoromethyloxirane (C$_3$H$_3$F$_3$O), at the fluorine K-edge at around 700 eV. The evolving fluorine-containing fragments are then probed by a second, circularly polarized X-ray pulse of higher photon energy in order to investigate the chemically shifted inner-shell electrons of the ionic motherfragment for their stereochemical sensitivity. We experimentally demonstrate and theoretically support how two-color X-ray pump X-ray probe experiments with polarization control enable XFELs as tools for chiral recognition., Comment: 14 pages, 5 figures

We present a novel, highly versatile, and self-referenced arrival time monitor for measuring the femtosecond time delay between a hard X-ray pulse from a free-electron laser and an optical laser pulse, measured directly on the same sample used for pump-probe experiments. Two chirped and picosecond long optical supercontinuum pulses traverse the sample with a mutually fixed time delay of 970 fs, while a femtosecond X-ray pulse arrives at an instant in between both pulses. Behind the sample the supercontinuum pulses are temporally overlapped to yield near-perfect destructive interference in the absence of the X-ray pulse. Stimulation of the sample with an X-ray pulse delivers non-zero contributions at certain optical wavelengths, which serve as a measure of the relative arrival time of the X-ray pulse with an accuracy of better than 25 fs. We find an excellent agreement of our monitor with the existing timing diagnostics at the SACLA XFEL with a Pearson correlation value of 0.98. We demonstrate a high sensitivity to measure X-ray pulses with pulse energies as low as 30 $\mu$J. Using a free-flowing liquid jet as interaction sample ensures the full replacement of the sample volume for each X-ray/optical event, thus enabling its utility even at MHz repetition rate XFEL sources.

The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the resultant photoproducts. The spectral bandwidth inherent to attosecond pulses is wide compared to the resonant features typically probed, which generally precludes the application of this technique in the attosecond regime. In this paper we propose and demonstrate a new technique to conduct transient absorption spectroscopy with broad bandwidth attosecond pulses with the aid of ghost imaging, recovering sub-bandwidth resolution in photoproduct-based absorption measurements., Comment: 13 pages, 3 figures

The quantum mechanical motion of electrons in molecules and solids occurs on the sub-femtosecond timescale. Consequently, the study of ultrafast electronic phenomena requires the generation of laser pulses shorter than 1 fs and of sufficient intensity to interact with their target with high probability. Probing these dynamics with atomic-site specificity requires the extension of sub-femtosecond pulses to the soft X-ray spectral region. Here we report the generation of isolated GW-scale soft X-ray attosecond pulses with an X-ray free-electron laser. Our source has a pulse energy that is six orders of magnitude larger than any other source of isolated attosecond pulses in the soft X-ray spectral region, with a peak power in the tens of gigawatts. This unique combination of high intensity, high photon energy and short pulse duration enables the investigation of electron dynamics with X-ray non-linear spectroscopy and single-particle imaging.