Coherent X-ray Free-electron Laser Research Articles

Towards a wavefront-preservation X-ray crystal monochromator for high-repetition-rate FELs.

The wavefront preservation of coherent X-ray free-electron laser beams is pushing the requirement on the quality and performance of X-ray optics to an unprecedented level. The Strehl ratio can be used to quantify this requirement. In this paper, the criteria for thermal deformation of the X-ray optics are formulated, especially for crystal monochromators. To preserve the X-ray wavefront, the standard deviation of the height error should be sub-nm for mirrors and less than 25 pm for crystal monochromators. Cryocooled silicon crystals combined with two techniques can be used to achieve this level of performance for monochromator crystals: (1) using a focusing element to compensate the second-order component of the thermal deformation; (2)introducing a cooling pad between the cooling block and silicon crystal and optimizing the effective cooling temperature. Each of these techniques allows the thermal deformation in standard deviation of the height error to be reduced by an order of magnitude. As an example, for the LCLS-II-HE Dynamic X-ray Scattering instrument, the criteria on thermal deformation of a high-heat-load monochromator crystal can be achieved for a 100 W SASE FEL beam. Wavefront propagation simulations confirm that the reflected beam intensity profile is satisfactory on both the peak power density and focused beam size.

Hard X-ray transient grating spectroscopy on bismuth germanate

Optical-domain transient grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique that is used to probe vibrational, magnetic and electronic degrees of freedom in the time domain1. The newly developed coherent X-ray free-electron laser sources allow its extension to the X-ray regime. X-rays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element specificity can address core excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. Here, we demonstrate TG excitation in the hard X-ray range at 7.1 keV. In bismuth germanate (BGO), the non-resonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods.

High field X-ray laser physics

High field X-ray laser physics

Double grating shearing interferometry for X-ray free-electron laser beams

The advancements in bright and coherent X-ray free-electron lasers (XFEL) have in the last decade revolutionized diverse fields of study, leading to an ever-increasing demand in more intense X-ray pulses. The accurate knowledge of the wavefront and the focal profile of such pulses ultimately dictates much of the experimental outcome. Here we present a single-shot shearing interferometry method to measure the wavefront of a focused hard XFEL pulse. Two identical transmission gratings are placed near the focus, and the interference pattern of overlapping diffraction orders is analyzed, resulting in a two-dimensional reconstruction of the X-ray wavefront. The spatial resolution and wavefront sensitivity can be tuned in-situ during the measurement. The method is non-invasive (i.e., the zeroth order or transmitted pulse is not modified in intensity or profile), allowing for either a simultaneous intensity measurement at high resolution or a fully characterized transmitted pulse for general experimental use.

Towards coherent X-ray free-electron lasers

Increased bandwidth and fluctuations are hurdles on the path towards generating intense fully coherent X-ray free-electron laser output. A recent experiment at FERMI Trieste demonstrated that these difficulties can be overcome by an approach called echo-enabled harmonic generation.

BRIGHT: the three-dimensional X-ray crystal Bragg diffraction code

In pursuit of a fully coherent X-ray free-electron laser (FEL), highly reflective Bragg crystals are used and will be used as a highly selective spectral filter in hard X-ray self-seeding FELs and X-ray FEL oscillators (XFELO), respectively. However, currently, when simulating self-seeding and XFELO, the three-dimensional effect of Bragg diffraction is not fully considered. In this paper, we derive a comprehensive solution for the response function of the crystal in Bragg diffraction. A three-dimensional X-ray crystal Bragg diffraction code, named BRIGHT, is introduced, which can be combined with other FEL-related codes, e.g., GENESIS and OPC. Performance and feasibility are assessed using two numerical examples, namely a self-seeding experiment for the linac coherent light source and XFELO options for Shanghai high repetition rate XFEL. The results indicate that BRIGHT provides a new and useful tool for three-dimensional modeling of FEL.

Common structural features of toxic intermediates from α-synuclein and GroES fibrillogenesis detected using cryogenic coherent X-ray diffraction imaging.

The aggregation and deposition of α-synuclein (αSyn) in neuronal cells is correlated to pathogenesis of Parkinson's disease. Although the mechanism of αSyn aggregation and fibril formation has been studied extensively, the structural hallmarks that are directly responsible for toxicity toward cells are still under debate. Here, we have compared the structural characteristics of the toxic intermediate molecular species of αSyn and similar toxic species of another protein, GroES, using coherent X-ray diffraction analysis. Using coherent X-ray free electron laser pulses of SACLA, we analysed αSyn and GroES fibril intermediate species and characterized various aggregate structures. Unlike previous studies where an annular oligomeric form of αSyn was identified, particle reconstruction from scattering traces suggested that the specific forms of the toxic particles were varied, with the sizes of the particles falling within a specific range. We did however discover a common structural feature in both αSyn and GroES samples; the edges of the detected particles were nearly parallel and produced a characteristic diffraction pattern in the diffraction experiments. The presence of parallel-edged particles in toxic intermediates of αSyn and GroES fibrillogenesis pointed towards a plausible common molecular interface that leads to the formation of mature fibrils.

Fixed target combined with spectral mapping: approaching 100% hit rates for serial crystallography

The advent of ultrafast highly brilliant coherent X-ray free-electron laser sources has driven the development of novel structure-determination approaches for proteins, and promises visualization of protein dynamics on sub-picosecond timescales with full atomic resolution. Significant efforts are being applied to the development of sample-delivery systems that allow these unique sources to be most efficiently exploited for high-throughput serial femtosecond crystallography. Here, the next iteration of a fixed-target crystallography chip designed for rapid and reliable delivery of up to 11 259 protein crystals with high spatial precision is presented. An experimental scheme for predetermining the positions of crystals in the chip by means of in situ spectroscopy using a fiducial system for rapid, precise alignment and registration of the crystal positions is presented. This delivers unprecedented performance in serial crystallography experiments at room temperature under atmospheric pressure, giving a raw hit rate approaching 100% with an effective indexing rate of approximately 50%, increasing the efficiency of beam usage and allowing the method to be applied to systems where the number of crystals is limited.

Elimination of X-Ray Diffraction through Stimulated X-Ray Transmission.

X-ray diffractive imaging with laterally coherent x-ray free-electron laser (XFEL) pulses is increasingly utilized to obtain ultrafast snapshots of matter. Here we report the amazing disappearance of single-shot charge and magnetic diffraction patterns recorded with resonantly tuned, narrow bandwidth XFEL pulses. Our experimental results reveal the exquisite sensitivity of single-shot charge and magnetic diffraction patterns of a magnetic film to the onset of field-induced stimulated elastic x-ray forward scattering. The loss in diffraction contrast, measured over 3 orders of magnitude in intensity, is in remarkable quantitative agreement with a recent theory that is extended to include diffraction.

A comprehensive simulation framework for imaging single particles and biomolecules at the European X-ray Free-Electron Laser.

The advent of newer, brighter, and more coherent X-ray sources, such as X-ray Free-Electron Lasers (XFELs), represents a tremendous growth in the potential to apply coherent X-rays to determine the structure of materials from the micron-scale down to the Angstrom-scale. There is a significant need for a multi-physics simulation framework to perform source-to-detector simulations for a single particle imaging experiment, including (i) the multidimensional simulation of the X-ray source; (ii) simulation of the wave-optics propagation of the coherent XFEL beams; (iii) atomistic modelling of photon-material interactions; (iv) simulation of the time-dependent diffraction process, including incoherent scattering; (v) assembling noisy and incomplete diffraction intensities into a three-dimensional data set using the Expansion-Maximisation-Compression (EMC) algorithm and (vi) phase retrieval to obtain structural information. We demonstrate the framework by simulating a single-particle experiment for a nitrogenase iron protein using parameters of the SPB/SFX instrument of the European XFEL. This exercise demonstrably yields interpretable consequences for structure determination that are crucial yet currently unavailable for experiment design.

A Stable 200TW / 1Hz Ti:sapphire laser for driving full coherent XFEL

Basic features of the ultra-short Ti:sapphire laser for driving compact X-ray free electron laser (XFEL) seeded by laser-driven high harmonic generation (HHG) at SIOM (Shanghai, China) is presented. The laser system consists of four-stage Ti:sapphire amplifiers and can produce 8J energy at 1Hz repetition rate after the final power amplifier. The best shot-to-shot energy fluctuation is as low as 0.54% in rms value, which is a desirable characteristic for driving stable electron acceleration and HHG seed. After compression, maximal pulse energy of 5.6J and pulse duration of 27fs can be obtained, the corresponding pulse peak power is above 200TW. To achieve full coherent XFEL, the amplified chirped laser beam is split into two beams after the final power amplifier. After compression in two independent compressors, the two laser beams can be used to drive laser wakefield acceleration (LWFA) and HHG respectively. The benefit of such a scheme is to improve the timing jitter and achieve all-optical synchronization between the electron beam and HHG seed in the near future.

PRIME: Probabilistic Initial 3D Model Generation for Single-Particle Cryo-Electron Microscopy

Low-dose electron microscopy of cryo-preserved individual biomolecules (single-particle cryo-EM) is a powerful tool for obtaining information about the structure and dynamics of large macromolecular assemblies. Acquiring images with low dose reduces radiation damage, preserves atomic structural details, but results in low signal-to-noise ratio of the individual images. The projection directions of the two-dimensional images are random and unknown. The grand challenge is to achieve the precise three-dimensional (3D) alignment of many (tens of thousands to millions) noisy projection images, which may then be combined to obtain a faithful 3D map. An accurate initial 3D model is critical for obtaining the precise 3D alignment required for high-resolution (<10Å) map reconstruction. We report a method (PRIME) that, in a single step and without prior structural knowledge, can generate an accurate initial 3D map directly from the noisy images.

Two-bunch self-seeding for narrow-bandwidth hard x-ray free-electron lasers

It is well known that seeding can be used to produce narrow-bandwidth and fully coherent x-ray free-electron lasers (FELs). Self-seeding, which uses an extra undulator to generate the seed pulse, is perhaps one of the most promising methods to accomplish this. In the hard x-ray regime with high-energy electrons, this method requires a large magnetic chicane to match the path-length delay of the x-ray monochromator that selects a narrow bandwidth of radiation. Such a chicane not only takes a large footprint to build, but also may degrade the electron-beam qualities through incoherent and coherent synchrotron radiation. In this paper, we present an alternative two-bunch self-seeding scheme. The two bunches are precisely separated to match the x-ray delay of the monochromator and eliminate the need for a long, complex magnetic chicane. The spectrally filtered self-amplified spontaneous emission x-ray pulse produced by the first bunch is combined with the second electron bunch at the entrance of the second undulator and then amplified to the saturation level. We present start-to-end simulation results based on the linac coherent light source hard x-ray FEL and show that this method can produce a nearly fully coherent x-ray pulse at a few GW power level.

Laser-pumped coherent x-ray free-electron laser

In a laser-pumped x-ray free-electron laser (FEL) an intense laser field replaces the magnetic wiggler field of a conventional FEL. Depending on the intensity and quality of both the electron beam and pump laser, the Thomson backscattered radiation can be coherently amplified. In a conventional FEL the generation of x rays requires electron beam energies in the multi-GeV range. In a laser-pumped x-ray FEL, electron beam energies in the multi-MeV range would be sufficient. To generate coherent x rays with this mechanism a number of physics and technology issues must be addressed. Foremost among these are the stringent requirements placed on the electron beam quality and brightness as well as on the pump laser. The seed radiation for the laser-pumped FEL is the laser-induced spontaneous radiation. The evolution of incoherent radiation into coherent radiation as well as the power gain lengths associated with the coherent x rays are analyzed and discussed. There is excellent agreement between our analytical results and GENESIS simulations for the radiated power, gain length, conversion efficiency, linewidth, and saturation length. These issues, as well as others, necessary to achieve coherent amplified x rays in a laser-pumped FEL are discussed. While a coherent x-ray source would have a number of attractive features, the requirements placed on both the electron beam and pump laser are extremely challenging.

Lensless imaging of magnetic nanostructures by X-ray spectro-holography

Our knowledge of the structure of matter is largely based on X-ray diffraction studies of periodic structures and the successful transformation (inversion) of the diffraction patterns into real-space atomic maps. But the determination of non-periodic nanoscale structures by X-rays is much more difficult. Inversion of the measured diffuse X-ray intensity patterns suffers from the intrinsic loss of phase information, and direct imaging methods are limited in resolution by the available X-ray optics. Here we demonstrate a versatile technique for imaging nanostructures, based on the use of resonantly tuned soft X-rays for scattering contrast and the direct Fourier inversion of a holographically formed interference pattern. Our implementation places the sample behind a lithographically manufactured mask with a micrometre-sized sample aperture and a nanometre-sized hole that defines a reference beam. As an example, we have used the resonant X-ray magnetic circular dichroism effect to image the random magnetic domain structure in a Co/Pt multilayer film with a spatial resolution of 50 nm. Our technique, which is a form of Fourier transform holography, is transferable to a wide variety of specimens, appears scalable to diffraction-limited resolution, and is well suited for ultrafast single-shot imaging with coherent X-ray free-electron laser sources.