Free-electron Laser FLASH Research Articles

Coupled Electron-Nuclear Dynamics Induced and Monitored with Femtosecond Soft X-ray Pulses in the Amino Acid Glycine.

The coupling of electronic and nuclear motion in polyatomic molecules is at the heart of attochemistry. The molecular properties, transient structures, and reaction mechanism of these many-body quantum objects are defined on the level of electrons and ions by molecular wave functions and their coherent superposition, respectively. In the present contribution, we monitor nonadiabatic quantum wave packet dynamics during molecular charge motion by reconstructing both the oscillatory charge density distribution and the characteristic time-dependent nuclear configuration coordinate from time-resolved Auger electron spectroscopic data recorded in previous studies on glycine molecules [Schwickert et al. Sci. Adv. 2022, 8, eabn6848]. The electronic and nuclear motion on the femtosecond time scale was induced and probed in kinematically complete soft X-ray experiments at the FLASH free-electron laser facility. The detailed analysis of amplitude, instantaneous phase, and instantaneous frequency of the propagating many-body wave packet during its lifecycle provides unprecedented insight into dynamical processes beyond the Born-Oppenheimer approximation. We are confident that the refined experimental data evaluation helps to develop new theoretical tools to describe time-dependent molecular wave functions in complicated but ubiquitous non-Born-Oppenheimer photochemical conditions.

Detector developments for photon science at DESY

The past, current and planned future developments of X-ray imagers in the Photon-Science Detector Group at DESY-Hamburg is presented. the X-ray imagers are custom developed and tailored to the different X-ray sources in Hamburg, including the storage ring PETRA III/IV; the VUV-soft X-ray free electron laser FLASH, and the European Free-Electron Laser. Each source puts different requirements on the X-ray detectors, which is described in detail, together with the technical solutions implemented.

Tunable UV Laser for External Seeding of the High Repetition Rate Soft X-ray Free Electron Laser FLASH

We are currently developing a tunable high-repetition rate femtosecond UV laser system for external seeding superconducting soft X-ray Free Electron Laser FLASH. Initial results show excellent power and wavelength stability of the Optical Parametric Chirped Pulse Amplification system.

FLASH free electron laser pump-probe laser concept based on spectral broadening of high-power ytterbium picosecond systems in multi-pass cells.

Within the FLASH2020+ upgrade, the pump-probe laser capabilities of the extreme ultraviolet and soft x-ray free-electron laser (XFEL) FLASH in Hamburg will be extended. In particular, providing wavelength tunability, shorter pulse durations, and reduced arrival time jitter will increase the scientific opportunities and the time resolution for the XFEL-optical laser pump-probe experiments. We present here a novel concept for the pump-probe laser at FLASH that is based on the post-compression of picosecond pulses emitted from high-power Ytterbium:YAG slab amplifiers. Flexible reduction of the pulse duration is facilitated by spectral broadening in pressure-tunable multi-pass cells. As an application, we show the pumping of a commercial optical parametric amplifier with 150fs post-compressed pulses. By means of an additional difference frequency generation stage, tunable spectral coverage from 1.3 to 16μm is reached with multi-μJ, sub-150fs pulses. Finally, a modular reconfiguration approach to the optical setups close to the free-electron laser instruments is implemented. This enables fast installation of the nonlinear frequency converters at the end stations for user operation and flexibility between different instruments in the two experimental halls.

Unsupervised real-world knowledge extraction via disentangled variational autoencoders for photon diagnostics

We present real-world data processing on measured electron time-of-flight data via neural networks. Specifically, the use of disentangled variational autoencoders on data from a diagnostic instrument for online wavelength monitoring at the free electron laser FLASH in Hamburg. Without a-priori knowledge the network is able to find representations of single-shot FEL spectra, which have a low signal-to-noise ratio. This reveals, in a directly human-interpretable way, crucial information about the photon properties. The central photon energy and the intensity as well as very detector-specific features are identified. The network is also capable of data cleaning, i.e. denoising, as well as the removal of artefacts. In the reconstruction, this allows for identification of signatures with very low intensity which are hardly recognisable in the raw data. In this particular case, the network enhances the quality of the diagnostic analysis at FLASH. However, this unsupervised method also has the potential to improve the analysis of other similar types of spectroscopy data.

Tracking the surface atomic motion in a coherent phonon oscillation

X-ray photoelectron diffraction is a powerful tool for determining the structure of clean and adsorbate-covered surfaces. Extending the technique into the ultrafast time domain will open the door to studies as diverse as the direct determination of the electron-phonon coupling strength in solids and the mapping of atomic motion in surface chemical reactions. Here we demonstrate time-resolved photoelectron diffraction using ultrashort soft x-ray pulses from the free electron laser FLASH. We collect Se $3d$ photoelectron diffraction patterns over a wide angular range from optically excited $\mathrm{Bi}{}_{2}\mathrm{Se}{}_{3}$ with a time resolution of 140 fs. Combining these with multiple scattering simulations allows us to track the motion of near-surface atoms within the first 3 ps after triggering a coherent vibration of the ${A}_{1g}$ optical phonons. Using a fluence of $4.2\phantom{\rule{0.28em}{0ex}}\mathrm{mJ}/{\mathrm{cm}}^{2}$ from a 1.55 eV pump laser, we find the resulting coherent vibrational amplitude in the first two interlayer spacings to be on the order of 0.01 \AA{}.

Single-shot ptychography at a soft X-ray free-electron laser

In this work, single-shot ptychography was adapted to the XUV range and, as a proof of concept, performed at the free-electron laser FLASH at DESY to obtain a high-resolution reconstruction of a test sample. Ptychography is a coherent diffraction imaging technique capable of imaging extended samples with diffraction-limited resolution. However, its scanning nature makes ptychography time-consuming and also prevents its application for mapping of dynamical processes. Single-shot ptychography can be realized by collecting the diffraction patterns of multiple overlapping beams in one shot and, in recent years, several concepts based on two con-focal lenses were employed in the visible regime. Unfortunately, this approach cannot be extended straightforwardly to X-ray wavelengths due to the use of refractive optics. Here, a novel single-shot ptychography setup utilizes a combination of X-ray focusing optics with a two-dimensional beam-splitting diffraction grating. It facilitates single-shot imaging of extended samples at X-ray wavelengths.

High-intensity laser experiments with highly charged ions in a Penning trap

We have conceived and built the HILITE (High-Intensity Laser-Ion Trap Experiment) Penning-trap setup for the production, confinement and preparation of pure ensembles of highly charged ions in a defined quantum state as a target for various high-intensity lasers. This enables a broad suite of laser-ion interaction studies at high photon energies and/or intensities, such as non-linear photo-ionisation studies. The setup has now been used to perform experiments at one such laser facility, namely the FLASH Free-Electron Laser at DESY in Hamburg, Germany. We describe the experimental possibilities of the apparatus, the results of the first measurements and future experiments at other laser facilities.

X-ray Ptychographic Imaging and Spectroscopic Studies of Plasma-Treated Plastic Films.

Polyethylene terephthalate (PET) is a thermoplastic polyester with numerous applications in industry. However, it requires surface modification on an industrial scale for printing and coating processes and plasma treatment is one of the most commonly used techniques to increase the hydrophilicity of the PET films. Systematic improvement of the surface modification by adaption of the plasma process can be aided by a comprehensive understanding of the surface morphology and chemistry. However, imaging large surface areas (tens of microns) with a resolution that allows understanding the surface quality and modification is challenging. As a proof-of-principle, plasma-treated PET films were used to demonstrate the capabilities of X-ray ptychography, currently under development at the soft X-ray free-electron laser FLASH at DESY, for imaging macroscopic samples. In combination with scanning electron microscopy (SEM), this new technique was used to study the effects of different plasma treatment processes on PET plastic films. The studies on the surface morphology were complemented by investigations of the surface chemistry using X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR). While both imaging techniques consistently showed an increase in roughness and change in morphology of the PET films after plasma treatment, X-ray ptychography can provide additional information on the three-dimensional morphology of the surface. At the same time, the chemical analysis shows an increase in the oxygen content and polarity of the surface without significant damage to the polymer, which is important for printing and coating processes.

Investigating Coherent Magnetization Control with Ultrashort THz Pulses

Coherent terahertz control of magnetization dynamics is an area of current interest due to its great potential for the realization of magnetization control on ultrafast timescales in commercial devices. Here we report on an experiment realized at the THz beamline of the free electron laser FLASH at DESY which offers a tunable terahertz radiation source and spontaneously synchronized free-electron laser X-ray pulses to resonantly probe the magnetization state of a ferromagnetic film. In this proof-of-principle experiment, we have excited a thin Permalloy film at different THz wavelengths and recorded the induced magnetization dynamics with photons resonantly tuned to the Ni M2,3 absorption edge. For THz pump pulses including higher orders of the undulator source we observed demagnetization dynamics, which precise shape depended on the employed fundamental wavelength of the undulator source. Analyzing the shape in detail, we can reconstruct the temporal profile of the electric field of the THz pump pulse. This offers a new method for the realization of an in-situ terahertz beamline diagnostic which will help researchers to adjust the pulse characteristics as needed, for example, for future studies of THz induced coherent control of magnetization dynamics.

Ultrafast MHz‐Rate Burst‐Mode Pump–Probe Laser for the FLASH FEL Facility Based on Nonlinear Compression of ps‐Level Pulses from an Yb‐Amplifier Chain

AbstractThe Free‐Electron Laser (FEL) FLASH offers the worldwide still unique capability to study ultrafast processes with high‐flux, high‐repetition rate extreme ultraviolet, and soft X‐ray pulses. The vast majority of experiments at FLASH are of pump–probe type. Many of them rely on optical ultrafast lasers. Here, a novel FEL facility laser is reported which combines high average power output from Yb:YAG amplifiers with spectral broadening in a Herriott‐type multipass cell and subsequent pulse compression to sub‐100‐fs durations. Compared to other facility lasers employing optical parametric amplification, the new system comes with significantly improved noise figures, compactness, simplicity, and power efficiency. Like FLASH, the optical laser operates with 10‐Hz burst repetition rate. The bursts consist of 800‐μs long trains of up to 800 ultrashort pulses being synchronized to the FEL with femtosecond precision. In the experimental chamber, pulses with up to 50‐μJ energy, 60‐fs full‐width half‐maximum duration and 1‐MHz rate at 1.03‐μm wavelength are available and can be adjusted by computer‐control. Moreover, nonlinear polarization rotation is implemented to improve laser pulse contrast. First cross‐correlation measurements with the FEL at the plane‐grating monochromator photon beamline are demonstrated, exhibiting the suitability of the laser for user experiments at FLASH.

Synchronized beamline at FLASH2 based on high-order harmonic generation for two-color dynamics studies.

We present the design, integration, and operation of the novel vacuum ultraviolet (VUV) beamline installed at the free-electron laser (FEL) FLASH. The VUV source is based on high-order harmonic generation (HHG) in gas and is driven by an optical laser system synchronized with the timing structure of the FEL. Ultrashort pulses in the spectral range from 10 to 40eV are coupled with the FEL in the beamline FL26, which features a reaction microscope (REMI) permanent endstation for time-resolved studies of ultrafast dynamics in atomic and molecular targets. The connection of the high-pressure gas HHG source to the ultra-high vacuum FEL beamline requires a compact and reliable system, able to encounter the challenging vacuum requirements and coupling conditions. First commissioning results show the successful operation of the beamline, reaching a VUV focused beam size of about 20 µm at the REMI endstation. Proof-of-principle photo-electron momentum measurements in argon indicate the source capabilities for future two-color pump-probe experiments.

Status Report of the Superconducting Free-Electron Laser FLASH at DESY

Status Report of the Superconducting Free-Electron Laser FLASH at DESY

Suppression of the vacuum space-charge effect in fs-photoemission by a retarding electrostatic front lens.

The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e-e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from -20 to -1100 V/mm for Ekin = 100eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 μm above the sample surface for Ekin = 100eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at Ekin = 107eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm2 (retarding field -21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm2, it increases by 0.5eV (pump wavelength 1030nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at Ekin = 3830eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.

Direct observation of charge separation in an organic light harvesting system by femtosecond time-resolved XPS

The ultrafast dynamics of photon-to-charge conversion in an organic light-harvesting system is studied by femtosecond time-resolved X-ray photoemission spectroscopy (TR-XPS) at the free-electron laser FLASH. This novel experimental technique provides site-specific information about charge separation and enables the monitoring of free charge carrier generation dynamics on their natural timescale, here applied to the model donor-acceptor system CuPc:C60. A previously unobserved channel for exciton dissociation into mobile charge carriers is identified, providing the first direct, real-time characterization of the timescale and efficiency of charge generation from low-energy charge-transfer states in an organic heterojunction. The findings give strong support to the emerging realization that charge separation even from energetically disfavored excitonic states is contributing significantly, indicating new options for light harvesting in organic heterojunctions.

60 fs, 1030 nm FEL pump-probe laser based on a multi-pass post-compressed Yb:YAG source.

This paper reports on nonlinear spectral broadening of 1.1 ps pulses in a gas-filled multi-pass cell to generate sub-100 fs optical pulses at 1030 nm and 515 nm at pulse energies of 0.8 mJ and 225 µJ, respectively, for pump-probe experiments at the free-electron laser FLASH. Combining a 100 kHz Yb:YAG laser with180 W in-burst average power and a post-compression platform enables reaching simultaneously high average powers and short pulse durations for high-repetition-rate FEL pump-probe experiments.

The TRIXS end-station for femtosecond time-resolved resonant inelastic x-ray scattering experiments at the soft x-ray free-electron laser FLASH.

We present the experimental end-station TRIXS dedicated to time-resolved soft x-ray resonant inelastic x-ray scattering (RIXS) experiments on solid samples at the free-electron laser FLASH. Using monochromatized ultrashort femtosecond XUV/soft x-ray photon pulses in combination with a synchronized optical laser in a pump-probe scheme, the TRIXS setup allows measuring sub-picosecond time-resolved high-resolution RIXS spectra in the energy range from 35 eV to 210 eV, thus spanning the M-edge (M1 and M2,3) absorption resonances of 3d transition metals and N4,5-edges of rare earth elements. A Kirkpatrick–Baez refocusing mirror system at the first branch of the plane grating monochromator beamline (PG1) provides a focus of (6 × 6) μm2 (FWHM) at the sample. The RIXS spectrometer reaches an energy resolution of 35–160 meV over the entire spectral range. The optical laser system based on a chirped pulse optical parametric amplifier provides approximately 100 fs (FWHM) long photon pulses at the fundamental wavelength of 800 nm and a fluence of 120 mJ/cm2 at a sample for optical pump-XUV probe measurements. Furthermore, optical frequency conversion enables experiments at 400 nm or 267 nm with a fluence of 80 and 30 mJ/cm2, respectively. Some of the first (pump-probe) RIXS spectra measured with this setup are shown. The measured time resolution for time-resolved RIXS measurements has been characterized as 287 fs (FWHM) for the used energy resolution.

Single-shot temporal characterization of XUV pulses with duration from ∼10 fs to ∼350 fs at FLASH

Ultra-short extreme ultraviolet pulses from the free-electron laser FLASH are characterized using terahertz-field driven streaking. Measurements at different ultra-short extreme ultraviolet wavelengths and pulse durations as well as numerical simulations were performed to explore the application range and accuracy of the method. For the simulation of streaking, a standard classical approach is used which is compared to quantum mechanical theory, based on strong field approximation. Various factors limiting the temporal resolution of the presented terahertz streaking setup are investigated and discussed. Special attention is paid to the cases of very short (∼10 fs) and long (up to ∼350 fs) pulses.

Single-shot transverse coherence measurements with Young's double pinholes at FLASH2

We measured the transverse coherence at FLASH2, a variable gap undulator line at the FLASH free-electron laser user facility at DESY in Hamburg. We demonstrate, theoretically and experimentally, a revised version of Young’s double pinhole approach to perform single-shot, repeatable and non-invasive transverse coherence measurements. At beamline FL24 of FLASH2, the transverse coherence of pulses was systematically characterized at wavelengths of 8, 13.5 and 18 nm for different FEL source settings. We determine degrees of coherence of 57% to 87% in the vertical and horizontal direction, respectively. These measurements can facilitate the planning of novel, coherence-based experiments at the FLASH facility.

Benchmarking coherent radiation spectroscopy as a tool for high-resolution bunch shape reconstruction at free-electron lasers

We present a systematic comparison of two complementary methods for determining the longitudinal charge density profile of the compressed electron bunches in the soft x-ray free-electron laser FLASH: a frequency-domain technique---coherent transition radiation (CTR) spectroscopy---and a time-domain technique---streaking of the electron beam with a transversely deflecting microwave structure (TDS). While the direct time-profile measurement with a TDS is a well-established method invented at SLAC, our group has pioneered high-resolution bunch shape analysis based on coherent radiation spectroscopy. We have developed a broadband spectrometer covering the wavelength range from $5\text{ }\text{ }\ensuremath{\mu}\mathrm{m}$ to $433\text{ }\text{ }\ensuremath{\mu}\mathrm{m}$ with two sets of remotely interchangeable staged reflection gratings. The measured spectral intensity allows to compute the absolute magnitude of the bunch form factor but not its phase which, however, is needed to retrieve the bunch profile. Two phase retrieval methods are investigated in detail: analytic phase computation by means of the Kramers-Kronig dispersion relation, and iterative phase retrieval. Several computational techniques are compared and evaluated in view of their applicability and efficiency. For a large variety of bunch shapes, the time profiles derived from the spectroscopic data are compared with the TDS profiles, and generally excellent agreement is observed down to the 10 fs level. For part of the measurements, two independent CTR spectrometer systems have been available, yielding almost identical bunch shapes. In summary, we demonstrate that using well calibrated and broadband spectroscopy data, a fast and reliable phase reconstruction algorithm leads to bunch profiles competitive to high resolution TDS measurements.