Sub-micrometre focusing of intense 100†keV X-rays with multilayer reflective optics.

A high-flux sub-micrometre focusing system was constructed using multilayer focusing mirrors in Kirkpatrick-Baez geometry for 100 keV X-rays. The focusing mirror system had a wide bandwidth of 5% and a high peak reflectivity of 74%. Performance was evaluated at the undulator beamline BL05XU of SPring-8, which produced an intense 100 keV X-ray beam with a bandwidth of 1%. When the light source was focused directly in both vertical and horizontal directions, the beam size was measured to be 0.32 µm (V) × 5.3 µm (H) with a flux of 1 × 1012 photons s-1. However, when a limited horizontal slit was used to form a secondary source, the focusing beam size decreased to 0.25 µm (V) × 0.26 µm (H) with a flux of 6 × 1010 photons s-1. The 200 nm line and space patterns of a Siemens star chart made of tantalum were clearly resolved by the absorption contrast of the focused beam. This 100 keV focusing system is applicable to various fields of nondestructive analyses with sub-micrometre resolutions.

In situ high-pressure pair distribution function measurement of liquid and glass by using 100 keV pink beam.

Understanding the pressure-induced structural changes in liquids and amorphous materials is fundamental in a wide range of scientific fields. However, experimental investigation of the structure of liquid and amorphous material under in situ high-pressure conditions is still limited due to the experimental difficulties. In particular, the range of the momentum transfer (Q) in the structure factor [S(Q)] measurement under high-pressure conditions has been limited at relatively low Q, which makes it difficult to conduct detailed structural analysis of liquid and amorphous material. Here, we show the in situ high-pressure pair distribution function measurement of liquid and glass by using the 100 keV pink beam. Structures of liquids and glasses are measured under in situ high-pressure conditions in the Paris-Edinburgh press by high-energy x-ray diffraction measurement using a double-slit collimation setup with a point detector. The experiment enables us to measure S(Q) of GeO2 and SiO2 glasses and liquid Ge at a wide range of Q up to 20-29 Å-1 under in situ high-pressure and high-temperature conditions, which is almost two times larger than that of the conventional high-pressure angle-dispersive x-ray diffraction measurement. The high-pressure experimental S(Q) precisely determined at a wide range of Q opens the way to investigate detailed structural features of liquids and amorphous materials under in situ high-pressure and high-temperature conditions, as well as ambient pressure study.

Pressure-induced reversal of Peierls-like distortions elicits the polyamorphic transition in GeTe and GeSe.

While polymorphism is prevalent in crystalline solids, polyamorphism draws increasing interest in various types of amorphous solids. Recent studies suggested that supercooling of liquid phase-change materials (PCMs) induces Peierls-like distortions in their local structures, underlying their liquid-liquid transitions before vitrification. However, the mechanism of how the vitrified phases undergo a possible polyamorphic transition remains elusive. Here, using high-energy synchrotron X-rays, we can access the precise pair distribution functions under high pressure and provide clear evidence that pressure can reverse the Peierls-like distortions, eliciting a polyamorphic transition in GeTe and GeSe. Combined with simulations based on machine-learned-neural-network potential, our structural analysis reveals a high-pressure state characterized by diminished Peierls-like distortion, greater coherence length, reduced compressibility, and a narrowing bandgap. Our finding underscores the crucial role of Peierls-like distortions in amorphous octahedral systems including PCMs. These distortions can be controlled through pressure and composition, offering potentials for designing properties in PCM-based devices.

BL09XU: an advanced hard X-ray photoelectron spectroscopy beamline of SPring-8.

The BL09XU beamline of SPring-8 has been reorganized into a beamline dedicated for hard X-ray photoelectron spectroscopy (HAXPES) to provide advanced capabilities with upgraded optical instruments. The beamline has two HAXPES analyzers to cover a wide range of applications. Two sets of double channel-cut crystal monochromators with the Si(220) and (311) reflections were installed to perform resonant HAXPES analyses with a total energy resolution of less than 300 meV over a wide energy range (4.9-12 keV) while achieving a fixed-exit condition. A double-crystal X-ray phase retarder using diamond crystals controls the polarization state with a high degree of polarization over 0.9 in the wide energy range 5.9-9.5 keV. Each HAXPES analyzer is equipped with a focusing mirror to provide a high-flux microbeam. The design and performance of the upgraded instruments are presented.

High-fluence and high-gain multilayer focusing optics to enhance spatial resolution in femtosecond X-ray laser imaging.

With the emergence of X-ray free-electron lasers (XFELs), coherent diffractive imaging (CDI) has acquired a capability for single-particle imaging (SPI) of non-crystalline objects under non-cryogenic conditions. However, the single-shot spatial resolution is limited to ~5 nanometres primarily because of insufficient fluence. Here, we present a CDI technique whereby high resolution is achieved with very-high-fluence X-ray focusing using multilayer mirrors with nanometre precision. The optics can focus 4-keV XFEL down to 60 nm × 110 nm and realize a fluence of >3 × 105 J cm-2 pulse-1 or >4 × 1012 photons µm-2 pulse-1 with a tenfold increase in the total gain compared to conventional optics due to the high demagnification. Further, the imaging of fixed-target metallic nanoparticles in solution attained an unprecedented 2-nm resolution in single-XFEL-pulse exposure. These findings can further expand the capabilities of SPI to explore the relationships between dynamic structures and functions of native biomolecular complexes.

Double-multilayer monochromators for high-energy and large-field X-ray imaging applications with intense pink beams at SPring-8 BL20B2.

In this study, double-multilayer monochromators that generate intense, high-energy, pink X-ray beams are designed, installed and evaluated at the SPring-8 medium-length (215 m) bending-magnet beamline BL20B2 for imaging applications. Two pairs of W/B4C multilayer mirrors are designed to utilize photon energies of 110 keV and 40 keV with bandwidths of 0.8% and 4.8%, respectively, which are more than 100 times larger when compared with the Si double-crystal monochromator (DCM) with a bandwidth of less than 0.01%. At an experimental hutch located 210 m away from the source, a large and uniform beam of size 14 mm (V) × 300 mm (H) [21 mm (V) × 300 mm (H)] was generated with a high flux density of 1.6 × 109 photons s-1 mm-2 (6.9 × 1010 photons s-1 mm-2) at 110 keV (40 keV), which marked a 300 (190) times increase in the photon flux when compared with a DCM with Si 511 (111) diffraction. The intense pink beams facilitate advanced X-ray imaging for large-sized objects such as fossils, rocks, organs and electronic devices with high speed and high spatial resolution.

Experimental evidence of tetrahedral symmetry breaking in SiO2 glass under pressure.

Bimodal behavior in the translational order of silicon's second shell in SiO2 liquid at high temperatures and high pressures has been recognized in theoretical studies, and the fraction of the S state with high tetrahedrality is considered as structural origin of the anomalous properties. However, it has not been well identified in experiment. Here we show experimental evidence of a bimodal behavior in the translational order of silicon's second shell in SiO2 glass under pressure. SiO2 glass shows tetrahedral symmetry structure with separation between the first and second shells of silicon at low pressures, which corresponds to the S state structure reported in SiO2 liquid. On the other hand, at high pressures, the silicon's second shell collapses onto the first shell, and more silicon atoms locate in the first shell. These observations indicate breaking of local tetrahedral symmetry in SiO2 glass under pressure, as well as SiO2 liquid.

Stable sub-micrometre high-flux probe for soft X-ray ARPES using a monolithic Wolter mirror.

A focusing optics that can provide a sub-micrometre high-flux probe for soft X-ray micrometre-scale angle-resolved photoemission spectroscopy (ARPES) is proposed. A monolithic Wolter-type mirror with a large acceptance, achromatism and small comatic aberration was designed and evaluated. A focused beam size of 0.4 µm (vertical) × 4 µm (horizontal), a high throughput of 59% and a high tolerance of 1.6 mrad to the pitching error were realized at a photon energy of 1000 eV. A Wolter-type mirror can be practically employed as a stable sub-micrometre focusing mirror with high throughput in ARPES applications.

Generation of an X-ray nanobeam of a free-electron laser using reflective optics with speckle interferometry.

Ultimate focusing of an X-ray free-electron laser (XFEL) enables the generation of ultrahigh-intensity X-ray pulses. Although sub-10 nm focusing has already been achieved using synchrotron light sources, the sub-10 nm focusing of XFEL beams remains difficult mainly because the insufficient stability of the light source hinders the evaluation of a focused beam profile. This problem is specifically disadvantageous for the Kirkpatrick-Baez (KB) mirror focusing system, in which a slight misalignment of ∼300 nrad can degrade the focused beam. In this work, an X-ray nanobeam of a free-electron laser was generated using reflective KB focusing optics combined with speckle interferometry. The speckle profiles generated by 2 nm platinum particles were systematically investigated on a single-shot basis by changing the alignment of the multilayer KB mirror system installed at the SPring-8 Angstrom Compact Free-Electron Laser, in combination with computer simulations. It was verified that the KB mirror alignments were optimized with the required accuracy, and a focused vertical beam of 5.8 nm (±1.2 nm) was achieved after optimization. The speckle interferometry reported in this study is expected to be an effective tool for optimizing the alignment of nano-focusing systems and for generating an unprecedented intensity of up to 1022 W cm-2 using XFEL sources.

Arrival timing diagnostics at a soft X-ray free-electron laser beamline of SACLA BL1.

An arrival timing monitor for the soft X-ray free-electron laser (XFEL) beamline of SACLA BL1 has been developed. A small portion of the soft XFEL pulse is branched using the wavefront-splitting method. The branched FEL pulse is one-dimensionally focused onto a GaAs wafer to induce a transient reflectivity change. The beam branching method enables the simultaneous operation of the arrival timing diagnostics and experiments. The temporal resolution evaluated from the imaging system is ∼22 fs in full width at half-maximum, which is sufficient considering the temporal durations of the soft XFEL and the optical laser pulses.

Systematic-error-free wavefront measurement using an X-ray single-grating interferometer.

In this study, the systematic errors of an X-ray single-grating interferometer based on the Talbot effect were investigated in detail. Non-negligible systematic errors induced by an X-ray camera were identified and a method to eliminate the systematic error was proposed. Systematic-error-free measurements of the wavefront error produced by multilayer focusing mirrors with large numerical apertures were demonstrated at the SPring-8 Angstrom Compact free electron LAser. Consequently, wavefront aberration obtained with two different cameras was found to be consistent with an accuracy better than λ/12.

A soft X-ray free-electron laser beamline at SACLA: the light source, photon beamline and experimental station.

The design and performance of a soft X-ray free-electron laser (FEL) beamline of the SPring-8 Compact free-electron LAser (SACLA) are described. The SPring-8 Compact SASE Source test accelerator, a prototype machine of SACLA, was relocated to the SACLA undulator hall for dedicated use for the soft X-ray FEL beamline. Since the accelerator is operated independently of the SACLA main linac that drives the two hard X-ray beamlines, it is possible to produce both soft and hard X-ray FEL simultaneously. The FEL pulse energy reached 110 µJ at a wavelength of 12.4 nm (i.e. photon energy of 100 eV) with an electron beam energy of 780 MeV.

Ellipsoidal mirror for two-dimensional 100-nm focusing in hard X-ray region.

Cutting-edge hard X-ray microscopy strongly depends on sophisticated focusing optics and ultrabright X-ray sources at synchrotron-radiation and X-ray free-electron laser (XFEL) facilities. These facilities typically provide two-dimensional nanofocusing X-ray beams by combining one-dimensional focusing mirrors. However, single-reflecting two-dimensional focusing mirrors with an ellipsoidal surface, which are well-known to possess high efficiency, have limited microfocusing applications. In this paper, we present an ultrahigh-precision ellipsoidal mirror for two-dimensional X-ray nanofocusing by overcoming the difficulties faced in the manufacturing process of its aspherical surface, including the surface-processing methods and surface metrology. The developed mirror has nanoscale accuracy, and it achieves focus size of 85 nm × 125 nm (full width at half maximum) using 7-keV X-rays. Two-dimensional focus was demonstrated in the same focal plane by resolving 50-nm test structures by scanning X-ray microscopy using a focusing beam. These achievements represent an important first step toward realizing two-dimensional aspherical mirrors with complex designs, in addition to ultralow loss and unprecedented small focusing property for extensive optical applications in synchrotron-radiation and XFEL facilities as well as in other scientific fields that require ultraprecision optical surfaces.

Dynamic fracture of tantalum under extreme tensile stress.

The understanding of fracture phenomena of a material at extremely high strain rates is a key issue for a wide variety of scientific research ranging from applied science and technological developments to fundamental science such as laser-matter interaction and geology. Despite its interest, its study relies on a fine multiscale description, in between the atomic scale and macroscopic processes, so far only achievable by large-scale atomic simulations. Direct ultrafast real-time monitoring of dynamic fracture (spallation) at the atomic lattice scale with picosecond time resolution was beyond the reach of experimental techniques. We show that the coupling between a high-power optical laser pump pulse and a femtosecond x-ray probe pulse generated by an x-ray free electron laser allows detection of the lattice dynamics in a tantalum foil at an ultrahigh strain rate of [Formula: see text] ~2 × 108 to 3.5 × 108 s-1. A maximal density drop of 8 to 10%, associated with the onset of spallation at a spall strength of ~17 GPa, was directly measured using x-ray diffraction. The experimental results of density evolution agree well with large-scale atomistic simulations of shock wave propagation and fracture of the sample. Our experimental technique opens a new pathway to the investigation of ultrahigh strain-rate phenomena in materials at the atomic scale, including high-speed crack dynamics and stress-induced solid-solid phase transitions.

Damage threshold of coating materials on x-ray mirror for x-ray free electron laser.

We evaluated the damage threshold of coating materials such as Mo, Ru, Rh, W, and Pt on Si substrates, and that of uncoated Si substrate, for mirror optics of X-ray free electron lasers (XFELs). Focused 1 µm (full width at half maximum) XFEL pulses with the energies of 5.5 and 10 keV, generated by the SPring-8 angstrom compact free electron laser (SACLA), were irradiated under the grazing incidence condition. The damage thresholds were evaluated by in situ measurements of X-ray reflectivity degradation during irradiation by multiple pulses. The measured damage fluences below the critical angles were sufficiently high compared with the unfocused SACLA beam fluence. Rh coating was adopted for two mirror systems of SACLA. One system was a beamline transport mirror system that was partially coated with Rh for optional utilization of a pink beam in the photon energy range of more than 20 keV. The other was an improved version of the 1 µm focusing mirror system, and no damage was observed after one year of operation.

Stitching interferometry for ellipsoidal x-ray mirrors.

Ellipsoidal mirrors, which can efficiently produce a two-dimensional focusing beam with a single mirror, are superior x-ray focusing optics, especially when compared to elliptical-cylinder mirrors in the Kirkpatrick-Baez geometry. However, nano-focusing ellipsoidal mirrors are not commonly used for x-ray optics because achieving the accuracy required for the surface metrology of nano-focusing ellipsoidal mirrors is difficult due to their small radius of curvature along the short ellipsoidal axis. Here, we developed a surface metrology system for nano-focusing ellipsoidal mirrors using stitching interferometric techniques. The developed system simultaneously measures sub-aperture shapes with a microscopic interferometer and the tilt angles of the sub-aperture shapes with a large Fizeau interferometer. After correcting the systematic errors included in the sub-aperture shapes, the entire mirror shape is calculated by stitching the sub-aperture shapes based on the obtained relative angles between partially overlapped sub-apertures. In this study, we developed correction methods for systematic errors in sub-aperture shapes that originated from off-axis aberrations produced in the optics of the microscopic interferometer. The systematic errors on an ellipsoidal mirror were estimated by measuring a series of tilted plane substrates and the ellipsoidal substrate. From measurements of an ellipsoidal mirror with a 3.6-mm radius of curvature at the mirror center, we obtained a measurement repeatability of 0.51 nm (root-mean-square) in an assessment area of 0.5 mm × 99.18 mm. This value satisfies the requirements for surface metrology of nano-focusing x-ray mirrors. Thus, the developed metrology system should be applicable for fabricating nano-focusing ellipsoidal mirrors.

A beam branching method for timing and spectral characterization of hard X-ray free-electron lasers.

We report a method for achieving advanced photon diagnostics of x-ray free-electron lasers (XFELs) under a quasi-noninvasive condition by using a beam-splitting scheme. Here, we used a transmission grating to generate multiple branches of x-ray beams. One of the two primary diffracted branches (+1st-order) is utilized for spectral measurement in a dispersive scheme, while the other (-1st-order) is dedicated for arrival timing diagnostics between the XFEL and the optical laser pulses. The transmitted x-ray beam (0th-order) is guided to an experimental station. To confirm the validity of this timing-monitoring scheme, we measured the correlation between the arrival timings of the -1st and 0th branches. The observed error was as small as 7.0 fs in root-mean-square. Our result showed the applicability of the beam branching scheme to advanced photon diagnostics, which will further enhance experimental capabilities of XFEL.

3D visualization of XFEL beam focusing properties using LiF crystal X-ray detector.

Here, we report, that by means of direct irradiation of lithium fluoride a (LiF) crystal, in situ 3D visualization of the SACLA XFEL focused beam profile along the propagation direction is realized, including propagation inside photoluminescence solid matter. High sensitivity and large dynamic range of the LiF crystal detector allowed measurements of the intensity distribution of the beam at distances far from the best focus as well as near the best focus and evaluation of XFEL source size and beam quality factor M(2). Our measurements also support the theoretical prediction that for X-ray photons with energies ~10 keV the radius of the generated photoelectron cloud within the LiF crystal reaches about 600 nm before thermalization. The proposed method has a spatial resolution ~0.4-2.0 µm for photons with energies 6-14 keV and potentially could be used in a single shot mode for optimization of different focusing systems developed at XFEL and synchrotron facilities.

Atomic inner-shell laser at 1.5-ångström wavelength pumped by an X-ray free-electron laser.

Since the invention of the first lasers in the visible-light region, research has aimed to produce short-wavelength lasers that generate coherent X-rays; the shorter the wavelength, the better the imaging resolution of the laser and the shorter the pulse duration, leading to better temporal resolution in probe measurements. Recently, free-electron lasers based on self-amplified spontaneous emission have made it possible to generate a hard-X-ray laser (that is, the photon energy is of the order of ten kiloelectronvolts) in an ångström-wavelength regime, enabling advances in fields from ultrafast X-ray spectrosopy to X-ray quantum optics. An atomic laser based on neon atoms and pumped by a soft-X-ray (that is, a photon energy of less than one kiloelectronvolt) free-electron laser has been achieved at a wavelength of 14 nanometres. Here, we use a copper target and report a hard-X-ray inner-shell atomic laser operating at a wavelength of 1.5 ångströms. X-ray free-electron laser pulses with an intensity of about 10(19) watts per square centimetre tuned to the copper K-absorption edge produced sufficient population inversion to generate strong amplified spontaneous emission on the copper Kα lines. Furthermore, we operated the X-ray free-electron laser source in a two-colour mode, with one colour tuned for pumping and the other for the seed (starting) light for the laser.

Saturable absorption of intense hard X-rays in iron.

In 1913, Maurice de Broglie discovered the presence of X-ray absorption bands of silver and bromine in photographic emulsion. Over the following century, X-ray absorption spectroscopy was established as a standard basis for element analysis, and further applied to advanced investigation of the structures and electronic states of complex materials. Here we show the first observation of an X-ray-induced change of absorption spectra of the iron K-edge for 7.1-keV ultra-brilliant X-ray free-electron laser pulses with an extreme intensity of 10(20) W cm(-2). The highly excited state yields a shift of the absorption edge and an increase of transparency by a factor of 10 with an improvement of the phase front of the transmitted X-rays. This finding, the saturable absorption of hard X-rays, opens a promising path for future innovations of X-ray science by enabling novel attosecond active optics, such as lasing and dynamical spatiotemporal control of X-rays.