Current X-ray Free-electron Laser Research Articles

A High-Flux Compact X-ray Free-Electron Laser for Next-Generation Chip Metrology Needs

Recently, considerable work has been directed at the development of an ultracompact X-ray free-electron laser (UCXFEL) based on emerging techniques in high-field cryogenic acceleration, with attendant dramatic improvements in electron beam brightness and state-of-the-art concepts in beam dynamics, magnetic undulators, and X-ray optics. A full conceptual design of a 1 nm (1.24 keV) UCXFEL with a length and cost over an order of magnitude below current X-ray free-electron lasers (XFELs) has resulted from this effort. This instrument has been developed with an emphasis on permitting exploratory scientific research in a wide variety of fields in a university setting. Concurrently, compact FELs are being vigorously developed for use as instruments to enable next-generation chip manufacturing through use as a high-flux, few nm lithography source. This new role suggests consideration of XFELs to urgently address emerging demands in the semiconductor device sector, as identified by recent national need studies, for new radiation sources aimed at chip manufacturing. Indeed, it has been shown that one may use coherent X-rays to perform 10–20 nm class resolution surveys of macroscopic, cm scale structures such as chips, using ptychographic laminography techniques. As the XFEL is a very promising candidate for realizing such methods, we present here an analysis of the issues and likely solutions associated with extending the UCXFEL to harder X-rays (above 7 keV), much higher fluxes, and increased levels of coherence, as well as methods of applying such a source for ptychographic laminography to microelectronic device measurements. We discuss the development path to move the concept to rapid realization of a transformative XFEL-based application, outlining both FEL and metrology system challenges.

Gain dynamics of inner-shell vacancy states pumped by high-intensity XFEL in Mg, Al and Si.

High-intensity X-ray free-electron laser (XFEL) beams create transient and non-equilibrium dense states of matter in solid-density targets. These states can be used to develop atomic X-ray lasers with narrow bandwidth and excellent longitudinal coherence, which is not possible with current XFEL pulses. An atomic kinetics model is used to simulate the population dynamics of atomic inner-shell vacancy states in Mg, Al, and Si, revealing the feasibility of population inversion between K-shell and L-shell vacancy states. We also discuss the gain characteristics of these states implying the possibility of atomic X-ray lasers based on inner-shell vacancy states in the 1.5 keV region. The development of atomic X-ray lasers could have applications in high-resolution spectroscopy and nonlinear optics in the X-ray region.

Electrically stimulated droplet injector for reduced sample consumption in serial crystallography

With advances in X-ray free-electron lasers (XFELs), serial femtosecond crystallography (SFX) has enabled the static and dynamic structure determination for challenging proteins such as membrane protein complexes. In SFX with XFELs, the crystals are typically destroyed after interacting with a single XFEL pulse. Therefore, thousands of new crystals must be sequentially introduced into the X-ray beam to collect full data sets. Because of the serial nature of any SFX experiment, up to 99% of the sample delivered to the X-ray beam during its “off-time” between X-ray pulses is wasted due to the intrinsic pulsed nature of all current XFELs. To solve this major problem of large and often limiting sample consumption, we report on improvements of a revolutionary sample-saving method that is compatible with all current XFELs. We previously reported 3D-printed injection devices coupled with gas dynamic virtual nozzles (GDVNs) capable of generating samples containing droplets segmented by an immiscible oil phase for jetting crystal-laden droplets into the path of an XFEL. Here, we have further improved the device design by including metal electrodes inducing electrowetting effects for improved control over droplet generation frequency to stimulate the droplet release to matching the XFEL repetition rate by employing an electrical feedback mechanism. We report the improvements in this electrically triggered segmented flow approach for sample conservation in comparison with a continuous GDVN injection using the microcrystals of lysozyme and 3-deoxy-D-manno-octulosonate 8-phosphate synthase and report the segmented flow approach for sample injection applied at the Macromolecular Femtosecond Crystallography instrument at the Linear Coherent Light Source for the first time.

Atomistic investigation of cavitation and ablation in tantalum foils under irradiation with x-rays approaching 5 keV

The rapid irradiation and heating of matter can lead to material removal via a process known as ablation. While previous investigations have focused on ablation with optical and soft x-ray pulses, the process is not well understood for the high-energy x-rays delivered at current x-ray free electron laser facilities. In this paper, we use hybrid two-temperature model molecular dynamics simulations to determine the damage threshold and dynamics for tantalum foils under irradiation with x-rays in the range 1--5 keV. We report that damage occurs for foils with thickness $\ensuremath{\ge}300$ nm when heated to around 1.25 eV/atom. This damage results from the combined processes of melting and cavitation, finally resulting in the removal of material layers. The predictions of this study, in terms of the cavitation threshold and underlying dynamics, could guide interpretation of experiments as well as applications including development of beamline optics for free-electron lasers. We report consistency between cavitation and ablation behavior in isochoric heating experiments and spall processes in hydrodynamic compression and release experiments, confirming the primary modes of damage are mechanical in nature for the x-ray energies investigated.

Generation of ultrahigh-brightness pre-bunched beams from a plasma cathode for X-ray free-electron lasers

The longitudinal coherence of X-ray free-electron lasers (XFELs) in the self-amplified spontaneous emission regime could be substantially improved if the high brightness electron beam could be pre-bunched on the radiated wavelength-scale. Here, we show that it is indeed possible to realize such current modulated electron beam at angstrom scale by exciting a nonlinear wake across a periodically modulated plasma-density downramp/plasma cathode. The density modulation turns on and off the injection of electrons in the wake while downramp provides a unique longitudinal mapping between the electrons’ initial injection positions and their final trapped positions inside the wake. The combined use of a downramp and periodic modulation of micrometers is shown to be able to produces a train of high peak current (17 kA) electron bunches with a modulation wavelength of 10’s of angstroms - orders of magnitude shorter than the plasma density modulation. The peak brightness of the nano-bunched beam can be O(1021A/m2/rad2) orders of magnitude higher than current XFEL beams. Such prebunched, high brightness electron beams hold the promise for compact and lower cost XEFLs that can produce nanometer radiation with hundreds of GW power in a 10s of centimeter long undulator.

Segmented flow generator for serial crystallography at the European X-ray free electron laser

Serial femtosecond crystallography (SFX) with X-ray free electron lasers (XFELs) allows structure determination of membrane proteins and time-resolved crystallography. Common liquid sample delivery continuously jets the protein crystal suspension into the path of the XFEL, wasting a vast amount of sample due to the pulsed nature of all current XFEL sources. The European XFEL (EuXFEL) delivers femtosecond (fs) X-ray pulses in trains spaced 100 ms apart whereas pulses within trains are currently separated by 889 ns. Therefore, continuous sample delivery via fast jets wastes >99% of sample. Here, we introduce a microfluidic device delivering crystal laden droplets segmented with an immiscible oil reducing sample waste and demonstrate droplet injection at the EuXFEL compatible with high pressure liquid delivery of an SFX experiment. While achieving ~60% reduction in sample waste, we determine the structure of the enzyme 3-deoxy-D-manno-octulosonate-8-phosphate synthase from microcrystals delivered in droplets revealing distinct structural features not previously reported.

XFEL coherent diffraction imaging for weakly scattering particles using heterodyne interference

The spatial resolution of x-ray free-electron laser (XFEL) coherent diffraction imaging is currently limited by the fluence of XFELs. Here, we clarify this issue by systematically studying the diffraction with a SPring-8 angstrom compact free electron laser XFEL on gold nanoparticles of size from 10 nm to 80 nm in water solution. The coherent x-ray diffraction patterns obtained from single XFEL pulses were quantitatively analyzed using a small-angle x-ray scattering scheme along with computer simulations. The results show that the detectability of Au nanoparticles can be described by a “master curve” as a function of total electron density, particle size, and x-ray fluence. The difficulty in detecting a small particle under the current XFEL fluence, however, could be largely eliminated by the image enhancement effect through interference from a strong scattering nanoparticle nearby. We investigate this image enhancement effect by quantitatively analyzing the two-particle scattering from Au nanoparticles, and further, applying it to detect a weak biological object of influenza virus with the aid of an Au nanoparticle.

Acoustic Funnel and Buncher for Nanoparticle Injection

Acoustics-based techniques are investigated to focus and bunch nanoparticle beams. This allows to overcome the prominent problem of the longitudinal and transverse mismatch of particle stream and x-ray beam in single-particle/single molecule imaging at x-ray free-electron lasers (XFEL). It will also enable synchronised injection of particle streams at kHz repetition rates. Transverse focusing concentrates the particle flux to the (sub)micrometer x-ray focus. In the longitudinal direction, focused acoustic waves can be used to bunch the particle to the same repetition rate as the x-ray pulses. The acoustic manipulation is based on simple mechanical recoil effects and could be advantageous over light-pressure-based methods, which rely on absorption. The acoustic equipment is easy to implement and can be conveniently inserted into current XFEL endstations. With the proposed method, data collection times could be reduced by a factor of $10^4$. This work does not just provide an efficient method for acoustic manipulation of streams of arbitrary gas phase particles, but also opens up wide avenues for acoustics-based particle optics.

Characterization of high spatial resolution lithium fluoride X-ray detectors

The response of lithium fluoride (LiF) crystal detectors to monochromatic X-rays is measured in the multi-kilo-electron-volt range. This response, as a function of the X-ray dose, is independent of photon energy with no saturation level found. The response, as a function of the incident energy flux, is found to increase for photons of lower energy due to the differing attenuation lengths of X-ray photons within the crystal. Small differences are seen between different confocal microscopes used to scan the data, suggesting the need for absolute calibration. The spatial resolution of the LiF is also measured (1.19-1.36 μm) and is found to be independent of incident photon energy. Finally, a photometric study is performed in order to assess the feasibility of using these detectors at current X-ray free electron laser and laser facilities worldwide.

Towards X-ray transient grating spectroscopy.

The extension of transient grating spectroscopy to the x-ray regime will create numerous opportunities, ranging from the study of thermal transport in the ballistic regime to charge, spin, and energy transfer processes with atomic spatial and femtosecond temporal resolution. Studies involving complicated split-and-delay lines have not yet been successful in achieving this goal. Here we propose a novel, simple method based on the Talbot effect for converging beams, which can easily be implemented at current x-ray free electron lasers. We validate our proposal by analyzing printed interference patterns on polymethyl methacrylate and gold samples using ∼3 keV X-ray pulses.

Perspective: Opportunities for ultrafast science at SwissFEL.

We present the main specifications of the newly constructed Swiss Free Electron Laser, SwissFEL, and explore its potential impact on ultrafast science. In light of recent achievements at current X-ray free electron lasers, we discuss the potential territory for new scientific breakthroughs offered by SwissFEL in Chemistry, Biology, and Materials Science, as well as nonlinear X-ray science.

X-ray amplification by stimulated Brillouin scattering

Plasma-based parametric amplification using stimulated Brillouin scattering offers a route to coherent x-ray pulses orders of magnitude more intense than those of the brightest available sources. Brillouin amplification permits amplification of shorter wavelengths with lower pump intensities than Raman amplification, which Landau and collisional damping limit in the x-ray regime. Analytic predictions, numerical solutions of the three-wave-coupling equations, and particle-in-cell simulations suggest that Brillouin amplification in solid-density plasmas will allow compression of current x-ray free-electron laser pulses to subfemtosecond durations and unprecedented intensities.

Resonant squeezing and the anharmonic decay of coherent phonons

We show that the anharmonic decay of large-amplitude coherent phonons in a solid generates strongly enhanced squeezing of the phonon modes near points of the Brillouin zone where energy conservation in the three-phonon decay process is satisfied. The squeezing process leads to temporal oscillations of the mean-square displacement of target modes in resonance with the coherent phonon, which are characteristic of coherent phonon decay and do not occur in the decay of a phonon in a well-defined number state. For realistic material parameters of optically excited group-V semimetals, we predict that this squeezing results in strongly enhanced oscillations of the x-ray diffuse scattering intensity at sharply defined values of the x-ray momentum transfer. Numerical simulations of the phonon dynamics and the x-ray diffuse scattering in optically excited bismuth, using harmonic and anharmonic force parameters calculated with constrained density functional theory, demonstrate oscillations of the diffuse scattering intensity of magnitude 10%--20% of the thermal background at points of the Brillouin zone, where resonance occurs. Such oscillations should be observable using time-resolved optical-pump and x-ray-probe facilities available at current x-ray free-electron laser sources.

Hybrid approach for structural modeling of biological systems from X-ray free electron laser diffraction patterns.

We present a new hybrid approach for structural modeling using X-ray free electron laser (XFEL) diffraction patterns from non-crystalline biological samples. Reconstruction of a 3D structure requires a large number of diffraction patterns; however, in the current XFEL experiments with biological systems, the analysis often relies on a small number of 2D diffraction patterns. In this study, we explore the strategies to identify plausible 3D structural models by combining the 2D analysis of such diffraction patterns with computational modeling (normal mode analysis or molecular dynamics simulations). As the first step toward such hybrid modeling, we established a protocol to assess the agreement between the model structure and the target XFEL diffraction pattern and showed that XFEL data can be used to study the conformational transitions of biological molecules. We tested the proposed algorithms using data of three biomolecular complexes of different sizes (elongation factor 2, CCM virus, and ribosome) and examined the experimental conditions that are required to perform such studies, in particular the XFEL beam intensity requirements. The results indicate that the current beam intensity is close to a strength that enables us to study conformational transitions of macromolecules, such as ribosomes. The proposed algorithm can be combined with molecular mechanics approaches, such as molecular dynamics simulations and normal mode analysis, to generate a large number of candidate structures to perform hybrid structural modeling.

Ceramic micro-injection molded nozzles for serial femtosecond crystallography sample delivery.

Serial femtosecond crystallography (SFX) using X-ray Free-Electron Lasers (XFELs) allows for room temperature protein structure determination without evidence of conventional radiation damage. In this method, a liquid suspension of protein microcrystals can be delivered to the X-ray beam in vacuum as a micro-jet, which replenishes the crystals at a rate that exceeds the current XFEL pulse repetition rate. Gas dynamic virtual nozzles produce the required micrometer-sized streams by the focusing action of a coaxial sheath gas and have been shown to be effective for SFX experiments. Here, we describe the design and characterization of such nozzles assembled from ceramic micro-injection molded outer gas-focusing capillaries. Trends of the emitted jet diameter and jet length as a function of supplied liquid and gas flow rates are measured by a fast imaging system. The observed trends are explained by derived relationships considering choked gas flow and liquid flow conservation. Finally, the performance of these nozzles in a SFX experiment is presented, including an analysis of the observed background.

Coupling of detailed configuration kinetics and hydrodynamics in materials submitted to x-ray free-electron-laser irradiation

We describe a model for the study of the interaction of short x-ray free-electron laser (XFEL) pulses with matter. Hydrodynamics is solved in one-dimensional planar geometry together with XFEL energy deposition, transport by thermal conduction and electron-ion energy exchange. Along with XFEL energy deposition, a proper detailed configuration accounting atomic physics model has been implemented in line with the calculations. Simulations typical of current XFEL conditions of irradiation are presented and discussed. Finally, the corresponding spectral emission of this XFEL-heated matter is calculated with the unresolved transition array formalism.

Self-terminating diffraction gates femtosecond X-ray nanocrystallography measurements

X-ray free-electron lasers have enabled new approaches to the structural determination of protein crystals that are too small or radiation-sensitive for conventional analysis1. For sufficiently short pulses, diffraction is collected before significant changes occur to the sample, and it has been predicted that pulses as short as 10 fs may be required to acquire atomic-resolution structural information1-4. Here, we describe a mechanism unique to ultrafast, ultra-intense X-ray experiments that allows structural information to be collected from crystalline samples using high radiation doses without the requirement for the pulse to terminate before the onset of sample damage. Instead, the diffracted X-rays are gated by a rapid loss of crystalline periodicity, producing apparent pulse lengths significantly shorter than the duration of the incident pulse. The shortest apparent pulse lengths occur at the highest resolution, and our measurements indicate that current X-ray free-electron laser technology5 should enable structural determination from submicrometre protein crystals with atomic resolution.