Attosecond pulse shaping using a seeded free-electron laser.

Attosecond pulses are central to the investigation of valence- and core-electron dynamics on their natural timescales1-3. The reproducible generation and characterization of attosecond waveforms has been demonstrated so far only through the process of high-order harmonic generation4-7. Several methods for shaping attosecond waveforms have been proposed, including the use of metallic filters8,9, multilayer mirrors10 and manipulation of the driving field11. However, none of these approaches allows the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free-electron lasers, by contrast, deliver femtosecond, extreme-ultraviolet and X-ray pulses with energies ranging from tens of microjoules to a few millijoules12,13. Recent experiments have shown that they can generate subfemtosecond spikes, but with temporal characteristics that change shot-to-shot14-16. Here we report reproducible generation of high-energy (microjoule level) attosecond waveforms using a seeded free-electron laser17. We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with an approach for its temporal reconstruction. The results presented here open the way to performing attosecond time-resolved experiments with free-electron lasers.

Generation of intense phase-stable femtosecond hard X-ray pulse pairs.

Coherent nonlinear spectroscopies and imaging in the X-ray domain provide direct insight into the coupled motions of electrons and nuclei with resolution on the electronic length scale and timescale. The experimental realization of such techniques will strongly benefit from access to intense, coherent pairs of femtosecond X-ray pulses. We have observed phase-stable X-ray pulse pairs containing more than 3 × 107 photons at 5.9 keV (2.1 Å) with ∼1 fs duration and 2 to 5 fs separation. The highly directional pulse pairs are manifested by interference fringes in the superfluorescent and seeded stimulated manganese Kα emission induced by an X-ray free-electron laser. The fringes constitute the time-frequency X-ray analog of Young's double-slit interference, allowing for frequency domain X-ray measurements with attosecond time resolution.

Population inversion X-ray laser oscillator.

Oscillators are at the heart of optical lasers, providing stable, transform-limited pulses. Until now, laser oscillators have been available only in the infrared to visible and near-ultraviolet (UV) spectral region. In this paper, we present a study of an oscillator operating in the 5- to 12-keV photon-energy range. We show that, using the [Formula: see text] line of transition metal compounds as the gain medium, an X-ray free-electron laser as a periodic pump, and a Bragg crystal optical cavity, it is possible to build X-ray oscillators producing intense, fully coherent, transform-limited pulses. As an example, we consider the case of a copper nitrate gain medium generating ∼ 5 × [Formula: see text] photons per pulse with 37-fs pulse length and 48-meV spectral resolution at 8-keV photon energy. Our theoretical study and simulation of this system show that, because of the very large gain per pass, the oscillator saturates and reaches full coherence in four to six optical-cavity transits. We discuss the feasibility and design of the X-ray optical cavity and other parts of the oscillator needed for its realization, opening the way to extend X-ray-based research beyond current capabilities.

Characterization of a hard X-ray self-seeding diamond crystal orientation.

We present a method to accurately control the photon energies for hard X-ray Self-seeding schemes with a single crystal monochromator in transmissive geometry. The energy calibration is performed by measuring which pairs of the machine pitch and yaw angles for different crystallographic planes reflect the X-ray at the same wavelength. The free parameters of an analytical formula for the self-seeding energies are determined by fitting the observed intersections and the normalized derivative with respect to the pitch and yaw angles in the observed intersections. The method requires a hard X-ray spectrometer, but it does not rely on its absolute energy calibration. Instead, identifying the self-seeded energies above the SASE background or the monochromatic notches within the SASE bandwidth is sufficient for the calibration.

Controllable X-Ray Pulse Trains from Enhanced Self-Amplified Spontaneous Emission.

We report the demonstration of optical compression of an electron beam and the production of controllable trains of femtosecond, soft x-ray pulses with the Linac Coherent Light Source (LCLS) free-electron laser (FEL). This is achieved by enhanced self-amplified spontaneous emission with a 2 µm laser and a dechirper device. Optical compression was achieved by modulating the energy of an electron beam with the laser and then compressing with a chicane, resulting in high current spikes on the beam which we observe to lase. A dechirper was then used to selectively control the lasing region of the electron beam. Field autocorrelation measurements indicate a train of pulses, and we find that the number of pulses within the train can be controlled (from 1 to 5 pulses) by varying the dechirper position and undulator taper. These results are a step toward attosecond spectroscopy with x-ray FELs as well as future FEL schemes relying on optical compression of an electron beam.

Laguerre-Gaussian Mode Laser Heater for Microbunching Instability Suppression in Free-Electron Lasers.

Microbunching instability (MBI) driven by beam collective effects is known to be detrimental to high-brightness storage rings, linacs, and free-electron lasers (FELs). One known way to suppress this instability is to induce a small amount of energy spread to an electron beam by a laser heater. The distribution of the induced energy spread greatly affects MBI suppression and can be controlled by shaping the transverse profile of the heater laser. Here, we present the first experimental demonstration of effective MBI suppression using a LG_{01} transverse laser mode and compare the improved results with respect to traditional Gaussian transverse laser mode at the Linac Coherent Light Source. The effects on MBI suppression are characterized by multiple downstream measurements, including longitudinal phase space analysis and coherent radiation spectroscopy. We also discuss the role of LG_{01} shaping in soft x-ray self-seeded FEL emission, one of the most advanced operation modes of a FEL for which controlled suppression of MBI is critical.

Observation of Seeded Mn Kß Stimulated X-Ray Emission Using Two-Color X-Ray Free-Electron Laser Pulses.

Kß x-ray emission spectroscopy is a powerful probe for electronic structure analysis of 3d transition metal systems and their ultrafast dynamics. Selectively enhancing specific spectral regions would increase this sensitivity and provide fundamentally new insights. Recently we reported the observation and analysis of Kα amplified spontaneous x-ray emission from Mn solutions using an x-ray free-electron laser to create the 1s core-hole population inversion [Kroll et al., Phys. Rev. Lett. 120, 133203 (2018)PRLTAO0031-900710.1103/PhysRevLett.120.133203]. To apply this new approach to the chemically more sensitive but much weaker Kß x-ray emission lines requires a mechanism to outcompete the dominant amplification of the Kα emission. Here we report the observation of seeded amplified Kß x-ray emission from a NaMnO_{4} solution using two colors of x-ray free-electron laser pulses, one to create the 1s core-hole population inversion and the other to seed the amplified Kß emission. Comparing the observed seeded amplified Kß emission signal with that from conventional Kß emission into the same solid angle, we obtain a signal enhancement of more than 10^{5}. Our findings are the first important step of enhancing and controlling the emission of selected final states of the Kß spectrum with applications in chemical and materials science.

Attosecond transient absorption spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy.

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.

Phase-Stable Self-Modulation of an Electron Beam in a Magnetic Wiggler.

Electron beams with a sinusoidal energy modulation have the potential to emit subfemtosecond x-ray pulses in a free-electron laser. An energy modulation can be generated by overlapping a powerful infrared laser with an electron beam in a magnetic wiggler. We report on a new infrared source for this modulation, coherent radiation from the electron beam itself. In this self-modulation process, the current spike on the tail of the electron beam radiates coherently at the resonant wavelength of the wiggler, producing a six-period carrier-envelope-phase (CEP)-stable infrared field with gigawatt power. This field creates a few MeV, phase-stable modulation in the electron-beam core. The modulated electron beam is immediately useful for generating subfemtosecond x-ray pulses at any machine repetition rate, and the CEP-stable infrared field may find application as an experimental pump or timing diagnostic.

Demonstration of Model-Independent Control of the Longitudinal Phase Space of Electron Beams in the Linac-Coherent Light Source with Femtosecond Resolution.

The dynamics of intense electron bunches in free electron lasers and plasma wakefield accelerators are dominated by complex collective effects such as wakefields, space charge, coherent synchrotron radiation, and drift unpredictably with time, making it difficult to control and tune beam properties using model-based approaches. We report on a first of its kind combination of automatic, model-independent feedback with a neural network for control of the longitudinal phase space of relativistic electron beams with femtosecond resolution based only on transverse deflecting cavity measurements.

Dispersion-Based Fresh-Slice Scheme for Free-Electron Lasers.

The fresh-slice technique improved the performance of several self-amplified spontaneous emission free-electron laser schemes by granting selective control on the temporal lasing slice without spoiling the other electron bunch slices. So far, the implementation has required a special insertion device to create the beam yaw, called a dechirper. We demonstrate a novel scheme to enable fresh-slice operation based on electron energy chirp and orbit dispersion that can be implemented at any free-electron laser facility without additional hardware.

Control of the Lasing Slice by Transverse Mismatch in an X-Ray Free-Electron Laser.

We demonstrated selective slice-dependent lasing by controlling the matching to the undulator of different slices within an electron bunch. The slice-dependent mismatch was realized through quadrupole wakefield generated in a corrugated structure. A deterministic procedure based on empirical beam transport and phase space information is used to match selected slices by turns to lase in the undulator while keeping all other slices from lasing, thus staying fresh. Measurements of time-resolved electron bunch energy loss by a transverse deflecting cavity confirmed the predicted behavior.

Generation of High-Power High-Intensity Short X-Ray Free-Electron-Laser Pulses.

X-ray free-electron lasers combine a high pulse power, short pulse length, narrow bandwidth, and high degree of transverse coherence. Any increase in the photon pulse power, while shortening the pulse length, will further push the frontier on several key x-ray free-electron laser applications including single-molecule imaging and novel nonlinear x-ray methods. This Letter shows experimental results at the Linac Coherent Light Source raising its maximum power to more than 300% of the current limit while reducing the photon pulse length to 10 fs. This was achieved by minimizing residual transverse-longitudinal centroid beam offsets and beam yaw and by correcting the dispersion when operating over 6 kA peak current with a longitudinally shaped beam.

High-Power Femtosecond Soft X Rays from Fresh-Slice Multistage Free-Electron Lasers.

We demonstrate a novel multistage amplification scheme for self-amplified spontaneous-emission free electron lasers for the production of few femtosecond pulses with very high power in the soft x-ray regime. The scheme uses the fresh-slice technique to produce an x-ray pulse on the bunch tail, subsequently amplified in downstream undulator sections by fresh electrons. With three-stages amplification, x-ray pulses with an energy of hundreds of microjoules are produced in few femtoseconds. For single-spike spectra x-ray pulses the pulse power is increased more than an order of magnitude compared to other techniques in the same wavelength range.

Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes.

We report the observation and analysis of the gain curve of amplified Kα x-ray emission from solutions of Mn(II) and Mn(VII) complexes using an x-ray free electron laser to create the 1s core-hole population inversion. We find spectra at amplification levels extending over 4 orders of magnitude until saturation. We observe bandwidths below the Mn 1s core-hole lifetime broadening in the onset of the stimulated emission. In the exponential amplification regime the resolution corrected spectral width of ∼1.7 eV FWHM is constant over 3 orders of magnitude, pointing to the buildup of transform limited pulses of ∼1 fs duration. Driving the amplification into saturation leads to broadening and a shift of the line. Importantly, the chemical sensitivity of the stimulated x-ray emission to the Mn oxidation state is preserved at power densities of ∼10^{20} W/cm^{2} for the incoming x-ray pulses. Differences in signal sensitivity and spectral information compared to conventional (spontaneous) x-ray emission spectroscopy are discussed. Our findings build a baseline for nonlinear x-ray spectroscopy for a wide range of transition metal complexes in inorganic chemistry, catalysis, and materials science.

Atom-specific activation in CO oxidation.

We report on atom-specific activation of CO oxidation on Ru(0001) via resonant X-ray excitation. We show that resonant 1s core-level excitation of atomically adsorbed oxygen in the co-adsorbed phase of CO and oxygen directly drives CO oxidation. We separate this direct resonant channel from indirectly driven oxidation via X-ray induced substrate heating. Based on density functional theory calculations, we identify the valence-excited state created by the Auger decay as the driving electronic state for direct CO oxidation. We utilized the fresh-slice multi-pulse mode at the Linac Coherent Light Source that provided time-overlapped and 30 fs delayed pairs of soft X-ray pulses and discuss the prospects of femtosecond X-ray pump X-ray spectroscopy probe, as well as X-ray two-pulse correlation measurements for fundamental investigations of chemical reactions via selective X-ray excitation.

X-ray absorption spectroscopy using a self-seeded soft X-ray free-electron laser.

X-ray free electron lasers (XFELs) enable unprecedented new ways to study the electronic structure and dynamics of transition metal systems. L-edge absorption spectroscopy is a powerful technique for such studies and the feasibility of this method at XFELs for solutions and solids has been demonstrated. However, the required x-ray bandwidth is an order of magnitude narrower than that of self-amplified spontaneous emission (SASE), and additional monochromatization is needed. Here we compare L-edge x-ray absorption spectroscopy (XAS) of a prototypical transition metal system based on monochromatizing the SASE radiation of the linac coherent light source (LCLS) with a new technique based on self-seeding of LCLS. We demonstrate how L-edge XAS can be performed using the self-seeding scheme without the need of an additional beam line monochromator. We show how the spectral shape and pulse energy depend on the undulator setup and how this affects the x-ray spectroscopy measurements.

Stimulated X-ray Raman scattering - a critical assessment of the building block of nonlinear X-ray spectroscopy.

With the invention of femtosecond X-ray free-electron lasers (XFELs), studies of light-induced chemical reaction dynamics and structural dynamics reach a new era, allowing for time-resolved X-ray diffraction and spectroscopy. To ultimately probe coherent electron and nuclear dynamics on their natural time and length scales, coherent nonlinear X-ray spectroscopy schemes have been proposed. In this contribution, we want to critically assess the experimental realisation of nonlinear X-ray spectroscopy at current-day XFEL sources, by presenting first experimental attempts to demonstrate stimulated resonant X-ray Raman scattering in molecular gas targets.

Prediction on X-ray output of free electron laser based on artificial neural networks.

Knowledge of x-ray free electron lasers' (XFELs) pulse characteristics delivered to a sample is crucial for ensuring high-quality x-rays for scientific experiments. XFELs' self-amplified spontaneous emission process causes spatial and spectral variations in x-ray pulses entering a sample, which leads to measurement uncertainties for experiments relying on multiple XFEL pulses. Accurate in-situ measurements of x-ray wavefront and energy spectrum incident upon a sample poses challenges. Here we address this by developing a virtual diagnostics framework using an artificial neural network (ANN) to predict x-ray photon beam properties from electron beam properties. We recorded XFEL electron parameters while adjusting the accelerator's configurations and measured the resulting x-ray wavefront and energy spectrum shot-to-shot. Training the ANN with this data enables effective prediction of single-shot or average x-ray beam output based on XFEL undulator and electron parameters. This demonstrates the potential of utilizing ANNs for virtual diagnostics linking XFEL electron and photon beam properties.

Revealing core-valence interactions in solution with femtosecond X-ray pump X-ray probe spectroscopy.

Femtosecond pump-probe spectroscopy using ultrafast optical and infrared pulses has become an essential tool to discover and understand complex electronic and structural dynamics in solvated molecular, biological, and material systems. Here we report the experimental realization of an ultrafast two-color X-ray pump X-ray probe transient absorption experiment performed in solution. A 10 fs X-ray pump pulse creates a localized excitation by removing a 1s electron from an Fe atom in solvated ferro- and ferricyanide complexes. Following the ensuing Auger-Meitner cascade, the second X-ray pulse probes the Fe 1s → 3p transitions in resultant novel core-excited electronic states. Careful comparison of the experimental spectra with theory, extracts +2 eV shifts in transition energies per valence hole, providing insight into correlated interactions of valence 3d with 3p and deeper-lying electrons. Such information is essential for accurate modeling and predictive synthesis of transition metal complexes relevant for applications ranging from catalysis to information storage technology. This study demonstrates the experimental realization of the scientific opportunities possible with the continued development of multicolor multi-pulse X-ray spectroscopy to study electronic correlations in complex condensed phase systems.