X-ray Free-electron Laser Pulses Research Articles

Investigating charge-up and fragmentation dynamics of oxygen molecules after interaction with strong X-ray free-electron laser pulses

During the last decade, X-ray free-electron lasers (XFELs) have enabled the study of light-matter interaction under extreme conditions. Atoms which are subject to XFEL radiation are charged by a complex interplay of (several subsequent) photoionization events and electronic decay processes within a few femtoseconds. The interaction with molecules is even more intriguing, since intricate nuclear dynamics occur as the molecules start to dissociate during the charge-up process. Here, we demonstrate that by analyzing photoelectron angular emission distributions and kinetic energy release of charge states of ionic molecular fragments, we can obtain a detailed understanding of the charge-up and fragmentation dynamics. Our novel approach allows for gathering such information without the need of complex ab initio modeling. As an example, we provide a detailed view on the processes happening on a femtosecond time scale in oxygen molecules exposed to intense XFEL pulses.

Matching-based two-color X-ray free-electron laser generation utilizing laser–plasma accelerated electron beam

Abstract Laser–plasma accelerators (LPAs) have great potential to realize a compact X-ray free-electron laser (FEL), which is limited by the beam properties currently. Two-color high-intensity X-ray FEL provides a powerful tool for probing ultrafast dynamic systems. In this paper, we present a simple and feasible method to generate a two-color X-ray FEL pulse based on an LPA beam. In this scheme, time-dependent mismatch along the bunch is generated and manipulated by the designed lattice system, enabling FEL lasing at different wavelength within two undulator sections. The time separation between the two pulses can be precisely adjusted by varying the time-delay chicane. Numerical simulations show that two-color soft X-ray FELs with gigawatt-level peak power and femtosecond duration can be generated, which confirm the validity and feasibility of the scheme.

Numerical study of transverse position monitor and compensation for x-ray polarization diagnosis.

Diagnosing free electron laser (FEL) polarization is critical for polarization-modulated research such as x-ray FEL diffraction imaging and probing material magnetism. In an electron time-of-flight (eTOF) polarimeter, the flight time and angular distribution of photoelectrons were designed based on x-ray polarimetry for on-site diagnosis. However, the transverse position of x-ray FEL pulses introduces error into the measured photoelectron angular distribution. This work, thus, proposes a method of compensating transverse position jitters for the polarization by the eTOF polarimeter itself without an external x-ray beam-position monitor. A comprehensive numerical model is developed to demonstrate the feasibility of the compensation method, and the results reveal that a spatial resolution of 20 μm and a polarity improved by 0.02 are possible with fully polarized FEL pulses. The impact of FEL pulses and a method to calibrate their linearity are also discussed.

Effects of x-ray free-electron laser pulse intensity on the Mn K β 1,3 x-ray emission spectrum in photosystem II-A case study for metalloprotein crystals and solutions.

In the last ten years, x-ray free-electron lasers (XFELs) have been successfully employed to characterize metalloproteins at room temperature using various techniques including x-ray diffraction, scattering, and spectroscopy. The approach has been to outrun the radiation damage by using femtosecond (fs) x-ray pulses. An example of an important and damage sensitive active metal center is the Mn4CaO5 cluster in photosystem II (PS II), the catalytic site of photosynthetic water oxidation. The combination of serial femtosecond x-ray crystallography and Kβ x-ray emission spectroscopy (XES) has proven to be a powerful multimodal approach for simultaneously probing the overall protein structure and the electronic state of the Mn4CaO5 cluster throughout the catalytic (Kok) cycle. As the observed spectral changes in the Mn4CaO5 cluster are very subtle, it is critical to consider the potential effects of the intense XFEL pulses on the Kβ XES signal. We report here a systematic study of the effects of XFEL peak power, beam focus, and dose on the Mn Kβ1,3 XES spectra in PS II over a wide range of pulse parameters collected over seven different experimental runs using both microcrystal and solution PS II samples. Our findings show that for beam intensities ranging from ∼5 × 1015 to 5 × 1017 W/cm2 at a pulse length of ∼35 fs, the spectral effects are small compared to those observed between S-states in the Kok cycle. Our results provide a benchmark for other XFEL-based XES studies on metalloproteins, confirming the viability of this approach.

X-ray vacuum diffraction at finite spatiotemporal offset

We study the nonlinear QED signature of x-ray vacuum diffraction in the head-on collision of optical high-intensity and x-ray free-electron laser pulses at finite spatiotemporal offsets between the laser foci. The high-intensity laser driven scattering of signal photons outside the forward cone of the x-ray probe constitutes a prospective experimental signature of quantum vacuum nonlinearity. Resorting to a simplified phenomenological ad hoc model, it was recently argued that the angular distribution of the signal in the far-field is sensitive to the wavefront curvature of the probe beam in the interaction region with the high-intensity pump. In this work, we model both the pump and probe fields as pulsed paraxial Gaussian beams and reanalyze this effect from first principles. We focus on vacuum diffraction both as an individual signature of quantum vacuum nonlinearity and as a potential means to improve the signal-to-background separation in vacuum birefringence experiments.

Shortening X-Ray Pulse Duration via Saturable Absorption.

To shorten the duration of x-ray pulses, we present a nonlinear optical technique using atoms with core-hole vacancies (core-hole atoms) generated by inner-shell photoionization. The weak Coulomb screening in the core-hole atoms results in decreased absorption at photon energies immediately above the absorption edge. By employing this phenomenon, referred to as saturable absorption, we successfully reduce the duration of x-ray free-electron laser pulses (photon energy: 9.000keV, duration: 6-7fs, fluence: 2.0-3.5×10^{5} J/cm^{2}) by ∼35%. This finding that core-hole atoms are applicable to nonlinear x-ray optics is an essential stepping stone for extending nonlinear technologies commonplace at optical wavelengths to the hard x-ray region.

Comparison of EMC and CM methods for orienting diffraction images in single-particle imaging experiments.

In single-particle imaging (SPI) experiments, diffraction patterns of identical particles are recorded. The particles are injected into the X-ray free-electron laser (XFEL) beam in random orientations. The crucial step of the data processing of SPI is finding the orientations of the recorded diffraction patterns in reciprocal space and reconstructing the 3D intensity distribution. Here, two orientation methods are compared: the expansion maximization compression (EMC) algorithm and the correlation maximization (CM) algorithm. To investigate the efficiency, reliability and accuracy of the methods at various XFEL pulse fluences, simulated diffraction patterns of biological molecules are used.

Resonant X-ray Emission Spectroscopy with a SASE Beam

Aqueous iron (III) oxide nanoparticles were irradiated with pure self-amplified spontaneous emission (SASE) X-ray free-electron laser (XFEL) pulses tuned to the energy around the Fe K-edge ionization threshold. For each XFEL shot, the incident X-ray pulse spectrum and Fe Kβ emission spectrum were measured synchronously with dedicated spectrometers and processed through a reconstruction algorithm allowing for the determination of Fe Kβ resonant X-ray emission spectroscopy (RXES) plane with high energy resolution. The influence of the number of X-ray shots employed in the experiment on the reconstructed data quality was evaluated, enabling the determination of thresholds for good data acquisition and experimental times essential for practical usage of scarce XFEL beam times.

Frequency-Mixing Lasing Mode at European XFEL

We demonstrate generation of X-ray Free-Electron Laser (XFEL) pulses in frequency mixing mode at the SASE3 line of the European XFEL. The majority of the SASE3 FEL segments are tuned at two frequencies ω1 and ω2 following an alternate pattern. Leveraging on non-linearities generated through longitudinal dispersion in the system, we obtain electron bunching at a frequency difference ωFM=ω2−ω1. FEL amplification at ωFM follows in a few last radiator segments. We report on the generation of frequency mixing at photon energies between 500 eV and 1100 eV with pulse energies, depending on the length of the radiator, in the mJ level. This method allows generating low photon energies in cases where the FEL runs at high electron energy and the target photon energy cannot be reached in the main undulator, with the simple addition of a short, custom-made afterburner.

Vacuum birefringence at x-ray free-electron lasers

We study the perspectives of measuring the phenomenon of vacuum birefringence predicted by quantum electrodynamics using an x-ray free-electron laser (XFEL) alone. We devise an experimental scheme allowing two consecutive XFEL pulses to collide under a finite angle, and thus act as both pump and probe field for the effect. The signature of vacuum birefringence is encoded in polarization-flipped signal photons to be detected with high-purity x-ray polarimetry. Our findings for idealized scenarios underline that the discovery potential of solely XFEL-based setups can be comparable to those involving optical high-intensity lasers. For currently achievable scenarios, we identify several key details of the x-ray optical ingredients that exert a strong influence on the magnitude of the desired signatures.

Ultrafast structural changes in matter induced by intense X-ray free-electron laser pulses

Ultrafast structural changes in matter induced by intense X-ray free-electron laser pulses

Vacuum birefringence and diffraction at an x-ray free-electron laser: From analytical estimates to optimal parameters

We study vacuum birefringence and x-ray photon scattering in the head-on collision of x-ray free electron and high-intensity laser pulses. Resorting to analytical approximations for the numbers of attainable signal photons, we analyze the behavior of the phenomenon under the variation of various experimental key-parameters and provide new analytical scalings. Our optimized approximations allow for quantitatively accurate results on the one-percent level. We in particular demonstrate that an appropriate choice of the x-ray focus and pulse duration can significantly improve the signal for given laser parameters, using the experimental parameters to be available at the Helmholtz International Beamline for Extreme Fields at the European XFEL as example. Our results are essential for the identification of the optimal choice of parameters in a discovery experiment of vacuum birefringence at the high-intensity frontier.

Fluorescence intensity correlation imaging with high spatial resolution and elemental contrast using intense x-ray pulses.

We theoretically investigate the fluorescence intensity correlation (FIC) of Ar clusters and Mo-doped iron oxide nanoparticles subjected to intense, femtosecond, and sub-femtosecond x-ray free-electron laser pulses for high-resolution and elemental contrast imaging. We present the FIC of and emission in Ar clusters and discuss the impact of sample damage on retrieving high-resolution structural information and compare the obtained structural information with those from the coherent diffractive imaging (CDI) approach. We found that, while sub-femtosecond pulses will substantially benefit the CDI approach, few-femtosecond pulses may be sufficient for achieving high-resolution information with the FIC. Furthermore, we show that the fluorescence intensity correlation computed from the fluorescence of the Mo atoms in Mo-doped iron oxide nanoparticles can be used to image dopant distributions in the nonresonant regime.

Bridging the gap of storage ring light sources and linac-driven free-electron lasers

High-gain free-electron lasers (FELs) are driven by short, high-charge density electron beams as only produced at dedicated single pass or recirculating linear accelerators. We describe new conceptual, technical, and modeling solutions to produce subpicosecond, up to $\ensuremath{\sim}100\text{ }\text{ }\ensuremath{\mu}\mathrm{J}$-energy extreme ultra-violet and soft x-ray FEL pulses at high- and tunable repetition rates, from diffraction-limited storage ring light source. In contrast to previously proposed schemes, we show that lasing can be simultaneous to the standard multibunch radiation emission from short insertion devices, and that it can be obtained with limited impact on the storage ring infrastructure. By virtue of the high-average power but moderate pulse energy, the storage ring-driven high-gain FEL would open the door to unprecedented accuracy in time-resolved spectroscopic analysis of matter in the linear response regime, in addition to inelastic scattering experiments.

Pump-probe X-ray holographic imaging of laser-induced cavitation bubbles with femtosecond FEL pulses

Cavitation bubbles can be seeded from a plasma following optical breakdown, by focusing an intense laser in water. The fast dynamics are associated with extreme states of gas and liquid, especially in the nascent state. This offers a unique setting to probe water and water vapor far-from equilibrium. However, current optical techniques cannot quantify these early states due to contrast and resolution limitations. X-ray holography with single X-ray free-electron laser pulses has now enabled a quasi-instantaneous high resolution structural probe with contrast proportional to the electron density of the object. In this work, we demonstrate cone-beam holographic flash imaging of laser-induced cavitation bubbles in water with nanofocused X-ray free-electron laser pulses. We quantify the spatial and temporal pressure distribution of the shockwave surrounding the expanding cavitation bubble at time delays shortly after seeding and compare the results to numerical simulations.

Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals

The outcomes and timescales of molecular nonadiabatic dynamics are decisively impacted by the quantum coherences generated at localized molecular regions. In time-resolved X-ray diffraction imaging, these coherences create distinct signatures via inelastic photon scattering, but they are buried under much stronger background elastic features. Here, we exploit the rich dynamical information encoded in the inelastic patterns, which we reveal by frequency-dispersed covariance ultrafast powder X-ray diffraction of stochastic X-ray free-electron laser pulses. This is demonstrated for the photoisomerization of azobenzene involving the passage through a conical intersection, where the nuclear wave packet branches and explores different quantum pathways. Snapshots of the coherence dynamics are obtained at high frequency shifts, not accessible with conventional diffraction measurements. These provide access to the timing and to the confined spatial distribution of the valence electrons directly involved in the conical intersection passage. This study can be extended to full three-dimensional imaging of conical intersections with ultrafast X-ray and electron diffraction.

Resolution of a bent-crystal spectrometer for X-ray free-electron laser pulses: diamond versus silicon.

The resolution function of a spectrometer based on a strongly bent single crystal (bending radius of 10 cm or less) is evaluated. It is shown that the resolution is controlled by two parameters: (i) the ratio of the lattice spacing of the chosen reflection to the crystal thickness and (ii) a single parameter comprising crystal thickness, its bending radius, distance to a detector, and anisotropic elastic constants of the chosen crystal. The results allow the optimization of the parameters of bent-crystal spectrometers for the hard X-ray free-electron laser sources.

Spatially resolved single-shot absorption spectroscopy with x-ray free electron laser pulse.

A new method of spatially resolved single-shot absorption spectroscopy for an x-ray free electron laser (XFEL) pulse has been developed by using a dispersive spectrometer and an elliptical mirror to enhance the spatial resolution. As a demonstration, we performed x-ray absorption near-edge structure measurement of Cu with a pump-probe scheme combining an XFEL pulse and a high-power femtosecond laser pulse. In the experiment, changes of an absorption spectrum in a plasma generated with a laser shot were successfully observed. The method will be a powerful tool for experiments requiring a spatial resolution and/or a single-shot measurement, such as high energy density science using a high-power laser pulse.

Optimization and Design of Cutting-Edge-Technology Tools for Natural Sciences Research in the Twenty-First Century: X-Ray Free Electron Lasers

Regarding the chronologic evolution of accelerator-based light sources, optimization and design issues of cutting-edge-technology insertion devices (i.e., undulators, wigglers, etc.) have been a big competitive concern since the beginning of the twenty-first century. Although these sources are strongly restricted by technological limitations in terms of radiation wavelength, leading X-ray free-electron laser (FEL) facilities are spending considerable efforts to survive in this scientific competition by modifying/updating their insertion devices. In other words, even though they all generate almost identical free-electron laser pulses, advertising a “superconducting undulator based light source” in comparison with a “conventional undulator based light source” may sound more attractive for some scientists. However, in contrast to superconducting undulators, conventional undulators do not require cryogenic cooling systems resulting in a cost-effective operation as a matter of course. Under the circumstances, it is shown that generation of hard X-ray FEL pulses is feasible via unique PPM undulators driven by an electron linear accelerator (linac) within the energy range of 5–10 GeV. The results reveal good consistency with the operating X-ray FEL sources worldwide.

XFEL and HHG interaction with matter: Effects of ultrashort pulses and random spikes

The theory of photoionization describing the interaction of x-ray free-electron laser (XFEL) pulses and high-harmonic-generated (HHG) radiation is generalized to ultrashort laser pulses, where the concept of the standard ionization probability per unit time in Fermi’s golden rule and in Einstein’s theory breaks down. Numerical calculations carried out in terms of a generalized photoionization probability for the total duration of pulses in the near-threshold regime demonstrate essentially nonlinear behavior, while absolute values may change by orders of magnitude for typical XFEL and HHG pulses. XFEL self-amplified spontaneous emission pulses are analyzed to reveal general features of photoionization for random and regular spikes: the dependences of the nonlinear photoionization probability on carrier frequency and spike duration are very similar, allowing an analytical expectation value approach that is valid even when there is only limited knowledge of random and regular parameters. Numerical simulations carried out for typical parameters demonstrate excellent agreement.