Coherent Hard X-ray Research Articles

Efficient end-to-end simulation of time-dependent coherent X-ray scattering experiments.

Physical optics simulations for beamlines and experiments allow users to test experiment feasibility and optimize beamline settings ahead of beam time in order to optimize valuable beam time at synchrotron light sources like NSLS-II. Further, such simulations also help to develop and test experimental data processing methods and software in advance. The Synchrotron Radiation Workshop (SRW) software package supports such complex simulations. We demonstrate how recent developments in SRW significantly improve the efficiency of physical optics simulations, such as end-to-end simulations of time-dependent X-ray photon correlation spectroscopy experiments with partially coherent undulator radiation (UR). The molecular dynamics simulation code LAMMPS was chosen to model the sample: a solution of silica nanoparticles in water at room temperature. Real-space distributions of nanoparticles produced by LAMMPS were imported into SRW and used to simulate scattering patterns of partially coherent hard X-ray UR from such a sample at the detector. The partially coherent UR illuminating the sample can be represented by a set of orthogonal coherent modes obtained by simulation of emission and propagation of this radiation through the coherent hard X-ray (CHX) scattering beamline followed by a coherent-mode decomposition. GPU acceleration is added for several key functions of SRW used in propagation from sample to detector, further improving the speed of the calculations. The accuracy of this simulation is benchmarked by comparison with experimental data.

An Ultra-Compact X-ray Regenerative Amplifier Free-Electron Laser

There is a growing interest in designing and building compact X-ray Free Electron Lasers (FELs) for scientific and industry applications. In this paper, we report an X-ray Regenerative Amplifier FEL (XRAFEL) design based on a proposed Ultra Compact X-ray FEL configuration. Our results show that an XRAFEL can dramatically enhance the temporal coherence and increase the spectral brightness of the radiation in the hard X-ray regime without increasing the footprint of the FEL configuration. The proposed compact, fully coherent, and high-flux hard X-ray source holds promise as a valuable candidate for a wide range of high-impact applications in both academia and industry.

Toward a fully coherent tender and hard X-ray free-electron laser via cascaded EEHG in fourth-generation synchrotron light sources.

Free-electron-laser-based beamlines utilize fully coherent laser pulses with extremely narrow bandwidth allowing direct use of X-rays without monochromators. This could be very beneficial for all users of current and future fourth-generation diffraction-limited synchrotron light sources (DL-SLSs) who need narrowband full-coherence high-brightness X-ray pulses. Based on our previous finding, i.e. that separating the two stages of echo-enabled harmonic generation (EEHG) with a few extra bending-magnet sections provides an effective way to increase the momentum compaction of chicane 1, one can simultaneously achieve adequate prebunching at extremely high harmonics as well as keep the energy modulation to the ideal minimum. This could open the door for cascaded EEHG, toward fully coherent tender and hard X-ray wavelengths. Built on our compact design of a twin-pulse seeding electron beam with an adjustable delay and timing jitter at the level of a few femtoseconds, a cascaded EEHG can be implemented, which includes two EEHG beamlines, where the radiation pulse generated by the first beamline with harmonic h1 could be used as the input seed laser pulse to the second beamline with harmonic h2. Hence, the second radiator could potentially reach very high harmonics [h = h1(20)h2(25-100)] from 500 to 2000, corresponding to tender and hard X-ray wavelengths. It is demonstrated that the cascaded EEHG scheme is compatible with almost any current or planned fourth-generation DL-SLS, with significant benefits for space-limited storage rings in particular. The main advantage is that this scheme requires almost no change of the storage-ring lattice and is fully compatible with other beamlines. Current proposals for rings with much longer straight sections would add self-amplified spontaneous emission as another viable option for storage-ring-based free-electron lasers.

Finite-difference propagation for the simulation of x-ray multilayer optics

Recent progress in nanofabrication, namely of multilayer optics, and the construction of coherent hard x-ray sources has enabled high resolution x-ray microscopy with large numerical aperture optics for small focal spot sizes. Sub-10 nm and even sub-5 nm focal spot sizes have already been achieved using multilayer optics such as multilayer Laue lenses and multilayer zone plates. However these optics can not be described by the kinematic theory given their extreme aspect-ratio between the depth (thickness) and the layer width. Moreover, the numerical simulation of these optics is challenging, and the absence of an accessible numerical framework inhibits further progress in their design and utilization. Here, we simulate the propagation of x-ray wavefields within and behind optical multilayer elements using a finite-difference propagation method. We show that the method offers high accuracy at reasonable computational cost. We investigate how small focal spot sizes and highest diffraction efficiency of multilayer optics can be achieved, considering volume diffraction effects such as waveguiding and Pendellösung. Finally, we show the simulation of a novel imaging scheme, allowing for a detailed study of image formation and the development of customized phase retrieval schemes.

Nonuniform Flow Dynamics Probed by Nanosecond X-Ray Speckle Visibility Spectroscopy.

We report observations of nanosecond nonuniform colloidal dynamics in a free flowing liquid jet using ultrafast x-ray speckle visibility spectroscopy. Utilizing a nanosecond double-bunch mode, the Linac Coherent Light Source free electron laser produced pairs of femtosecond coherent hard x-ray pulses. By exploring anisotropy in the visibility of summed speckle patterns which relates to the correlation functions, we evaluate not only the average particle flow rate in a colloidal nanoparticle jet, but also the nonuniform flow field within. The methodology presented here establishes the foundation for the study of nano- and atomic-scale inhomogeneous fluctuations in complex matter using x-ray free electron laser sources.

Generating X-rays with orbital angular momentum in a free-electron laser oscillator

Light with orbital angular momentum (OAM) provides new insights into a wide range of physical phenomena and has engendered advanced applications in various fields. Additionally, interest in X-ray OAM has been rapidly rising. We present a straightforward method to generate intense OAM beams from an X-ray free-electron laser oscillator (XFELO). The method leverages Bragg mirrors and longitudinal-transverse mode coupling to enable mode selection in a conventional XFELO configuration, thereby natively producing the fully coherent hard X-ray beams carrying OAM. Furthermore, simulation results demonstrate that fully coherent hard X-ray OAM beams at 1 MHz with a pulse energy of about 120 µJ can be generated without the optical mode converters. This simple approach could significantly advance the creation of X-ray OAM while stimulating the development of experimental methods.

Operando 3D imaging of defects dynamics of twinned-nanocrystal during catalysis

Using operando Bragg coherent x-ray diffraction imaging, we visualised three-dimensionally a single twinned-gold nanocrystal during the CO oxidation reaction. We describe the defect dynamics process occurring under operating conditions and indicate the correlation between the nucleation of highly strained regions at the surface of the nanocrystal and its catalytic activity. Understanding the twinning deformation mechanism sheds light on the creation of active sites, and could well contribute to the understanding of the catalytic behaviour of other catalysts. With the start-up of 4th generation synchrotron sources, we anticipate that coherent hard x-ray diffraction imaging techniques will play a major role in imaging in situ chemical processes.

Refractive Guide Switching a Regenerative Amplifier Free-Electron Laser for High Peak and Average Power Hard X Rays.

We present an x-ray regenerative amplifier free-electron laser design capable of producing fully coherent hard x-ray pulses across a broad tuning range at a high steady state repetition rate. The scheme leverages a strong undulator taper and an apertured diamond output-coupling cavity crystal to produce both high peak and average spectral brightness radiation that is 2 to 3 orders of magnitude greater than conventional single-pass self-amplified spontaneous emission free-electron laser amplifiers. Refractive guiding in the postsaturation regime is found to play a key role in passively controlling the stored cavity power. The scheme is explored both analytically and numerically in the context of the Linac Coherent Light Source II High Energy upgrade.

Thermal loading on crystals in an x-ray free-electron laser oscillator

X-ray free electron laser oscillators (XFELO) is future light source to produce fully coherent hard X-ray pulses. The X-rays circulate in an optical cavity built from multiple Bragg reflecting mirrors, which has a high reflectance in a bandwidth of ten meV level. The X-ray crystal mirrors exposed to intense X-ray beams in the cavity are subjects to thermal deformations that shift and distort the Bragg reflection. Therefore, the stability of the XFELO operation relies on the abilities of mirrors to preserve the Bragg reflection under such heat load. A new approach was used to analyze the heat load of mirrors and the XFELO operation. The essential light-matter interaction is simulated by the GEANT4 with a dedicated Bragg-reflection physical process to obtain the precise absorption information of the XFELO pulse in the crystals. The transient thermal conduction is analyzed by the finite-element analysis software upon the energy absorption information extract from GEANT4 simulation. A simplified heat-load model is then developed to integrate the heat load in the XFELO. With the help of the heat-load model, the analysis of XFELO operating with several cryogenically cooled diamond mirrors is conducted. The results indicate that the heat load would induce an oscillation when XFELO operates without enough cooling.

Thermal loading on self-seeding monochromators in x-ray free electron lasers

One approach to achieve longitudinally coherent hard X-ray free electron laser (XFEL) radiation is to introduce a single-crystal monochromator in the beam path to generate a co-propagating, time-synchronized self-seeding radiation pulse. For modern high-repetition rate XFELs, however, thermal loading on the crystal can degrade the quality of the seed pulse. To assess limitations on the maximum XFEL pulse repetition rate imposed by the seeding crystal, a comprehensive study of thermomechanical, and X-ray diffraction effects within the crystal is presented for two consecutive self-amplified spontaneous emission pulses incident on both reflective and transmissive crystal monochromators.

Polarization control of an x-ray free electron laser oscillator

High-intensity, fully coherent x-ray pulse with a tunable polarization over a wide spectral range is of great importance to many experiments. In this paper, we propose a tapered crossed-polarized undulator configuration for an x-ray free electron laser oscillator (XFELO) to produce arbitrarily polarized x-ray pulses in the hard x-ray region. A numerical example utilizing the parameters of the Shanghai High-Repetition-Rate XFEL and Extreme Light Facility (SHINE) is presented to demonstrate the generation of polarization controllable, fully coherent hard x-ray pulses with 99.9% polarization degree and 20 kHz polarization switching rate. The analysis presents that this scheme holds the possibility to be used in an energy tunable XFELO built from multiple Bragg mirrors.

Effect of undulators on magnet lattice and emittance

NSLS-II is now one of the brightest synchrotron light sources worldwide, in user operations since 2014. Currently, 20 light-generating insertion devices (IDs) are installed: 3 damping wigglers and 17 undulators of various types. These devices introduce significant distortions into the magnet lattice of the storage ring. For each ID, the distortions have been locally corrected using quadrupole magnets located nearby the ID. The insertion devices have also a significant impact on the electron beam emittance. Precise measurements of the emittance were carried out at the Coherent Hard X-ray beamline for three different lattices: without IDs, with 3 pairs of damping wigglers only, and with all IDs. A minimum horizontal emittance of 0.76 nm was achieved. The radiation energy loss and relative energy spread were also measured using a streak-camera. The measured data show good agreement with analytical formulas and numerical simulations.

High Bragg reflectivity of diamond crystals exposed to multi-kW mm-2 X-ray beams.

X-ray free-electron lasers in the oscillator configuration (XFELO) are future fully coherent hard X-rays sources with ultrahigh spectral purity. X-ray beams circulate in an XFELO optical cavity comprising diamond single crystals. They function as high-reflectance (close to 100%), narrowband (∼10 meV) Bragg backscattering mirrors. The average power density of the X-ray beams in the XFELO cavity is predicted to be as high as ∼10 kW mm-2. Therefore, XFELO feasibility relies on the ability of diamond crystals to withstand such a high radiation load and preserve their high reflectivity. Here the endurance of diamond crystals to irradiation with multi-kW mm-2 power density X-ray beams is studied. It is shown that the high Bragg reflectivity of the diamond crystals is preserved after the irradiation, provided it is performed at ∼1 × 10-8 Torr high-vacuum conditions. Irradiation under 4 × 10-6 Torr results in a ∼1 meV shift of the Bragg peak, which corresponds to a relative lattice distortion of 4 × 10-8, while the high Bragg reflectivity stays intact.

Dynamical scattering in coherent hard x-ray nanobeam Bragg diffraction

Unique intensity features arising from dynamical diffraction arise in coherent x-ray nanobeam diffraction patterns of crystals having thicknesses larger than the x-ray extinction depth or exhibiting combinations of nanoscale and mesoscale features. We demonstrate that dynamical scattering effects can be accurately predicted using an optical model combined with the Darwin theory of dynamical x-ray diffraction. The model includes the highly divergent coherent x-ray nanobeams produced by Fresnel zone plate focusing optics and accounts for primary extinction, multiple scattering, and absorption. The simulation accurately reproduces the dynamical scattering features of experimental diffraction patterns acquired from a GaAs/AlGaAs epitaxial heterostructure on a GaAs (001) substrate.

Nanomodulated electron beams via electron diffraction and emittance exchange for coherent x-ray generation

We present a new method for generation of relativistic electron beams with current modulation on the nanometer scale and below. The current modulation is produced by diffracting relativistic electrons in single crystal Si, accelerating the diffracted beam and imaging the crystal structure, then transferring the image into the temporal dimension via emittance exchange. The modulation period can be tuned by adjusting electron optics after diffraction. This tunable longitudinal modulation can have a period as short as a few angstroms, enabling production of coherent hard x-rays from a source based on inverse Compton scattering with total accelerator length of approximately ten meters. Electron beam simulations from cathode emission through diffraction, acceleration and image formation with variable magnification are presented along with estimates of the coherent x-ray output properties.

Two-stage EEHG for coherent hard X-ray generation based on a superconducting linac

A two-stage echo-enabled harmonic generation (EEHG) scheme is proposed for a superconducting linac-driven FEL to produce coherent hard X-rays. Electron beams of quite different bunch lengths are separately used in each stage of EEHG, and a monochromator is designed to purify the radiation from the first stage for seeding the second stage. Theoretical analysis and 3D simulations indicate that the proposed scheme can generate high-repetition-rate coherent hard X-ray pulses directly from a conventional UV seed laser.

Diamond x-ray optics: Transparent, resilient, high-resolution, and wavefront preserving

Abstract

Thermal Fluctuations of Ferroelectric Nanodomains in a Ferroelectric-Dielectric PbTiO_{3}/SrTiO_{3} Superlattice.

Ferroelectric-dielectric superlattices consisting of alternating layers of ferroelectric PbTiO_{3} and dielectric SrTiO_{3} exhibit a disordered striped nanodomain pattern, with characteristic length scales of 6nm for the domain periodicity and 30nm for the in-plane coherence of the domain pattern. Spatial disorder in the domain pattern gives rise to coherent hard x-ray scattering patterns exhibiting intensity speckles. We show here using variable-temperature Bragg-geometry x-ray photon correlation spectroscopy that x-ray scattering patterns from the disordered domains exhibit a continuous temporal decorrelation due to spontaneous domain fluctuations. The temporal decorrelation can be described using a compressed exponential function, consistent with what has been observed in other systems with arrested dynamics. The fluctuation speeds up at higher temperatures and the thermal activation energy estimated from the Arrhenius model is 0.35±0.21 eV. The magnitude of the energy barrier implies that the complicated energy landscape of the domain structures is induced by pinning mechanisms and domain patterns fluctuate via the generation and annihilation of topological defects similar to soft materials such as block copolymers.

Fully coherent hard X-ray generation by two-stage phase-merging enhanced harmonic generation**Supported by the National Natural Science Foundation of China (21127902 & 11322550) and Ten Thousand Talent Program

Cascading stages of seeded free electron lasers (FELs) is a promising way to produce fully coherent X-ray radiation. We study a new approach to produce coherent hard X-rays by cascading the recently proposed phase-merging enhanced harmonic generation (PEHG) The scheme consists of one dogleg and two PEHG configurations, and may be one of the leading candidates for the extracted undulator branch in future X-ray FEL facilities. FEL physics studies show that such a scheme is feasible within the present technology and can provide high brightness X-ray radiation pulses with narrow bandwidth and full coherence The radiated peak power at 1 Å wavelength converted from an initial 200 nm seed laser is over 2 GW

Electrode-stress-induced nanoscale disorder in Si quantum electronic devices

Disorder in the potential-energy landscape presents a major obstacle to the more rapid development of semiconductor quantum device technologies. We report a large-magnitude source of disorder, beyond commonly considered unintentional background doping or fixed charge in oxide layers: nanoscale strain fields induced by residual stresses in nanopatterned metal gates. Quantitative analysis of synchrotron coherent hard x-ray nanobeam diffraction patterns reveals gate-induced curvature and strains up to 0.03% in a buried Si quantum well within a Si/SiGe heterostructure. Electrode stress presents both challenges to the design of devices and opportunities associated with the lateral manipulation of electronic energy levels.