High-precision finishing method for narrow-groove channel-cut crystal x-ray monochromator using plasma chemical vaporization machining with wire electrode.

A channel-cut crystal monochromator (CCM) is a popular and powerful device for producing monochromatic x-ray beams with extreme angular stability at a nano-radian level. Narrowing the groove width of CCMs has various benefits; for example, it is made possible to design more compact CCMs with an equivalent working energy range and to reduce the optical delay and the amount of beam shift, enhancing compatibility with various experimental techniques. An obstacle to the use of narrow-groove CCMs is the lack of a high-precision finishing method for the inner-wall reflecting surfaces, which imposes the distortion of x-ray wavefronts and spectral purity. We propose a new, damage-free surface-finishing method for silicon CCMs with a narrow groove of 1 mm or less with a localized etching technique using plasma generated with a wire electrode of 50 µm diameter under atmospheric pressure. Repeating plasma-on and plasma-off periods with a pulsed power supply, we reduce the concentration of reaction products through self-diffusion during the plasma-off periods and minimize the redeposition of the products on the processed surface that deteriorates the surface roughness. Under optimized conditions, we processed a CCM with a groove width of 1.2 mm, which has uniform reflection profiles and a nearly ideal reflectivity behavior for coherent monochromatic x rays.

X-ray adaptive zoom condenser utilizing an intermediate virtual focus.

We propose an extended X-ray adaptive zoom condenser that can form an intermediate virtual focus. The system comprises two deformable mirrors for focusing within a single dimension and can vary its numerical aperture (NA) without changing the positions of the light source, mirrors, or final focus. The desired system NA is achieved simply by controlling the mirror surfaces, which enables conversion between convex and concave forms, by varying the position of the intermediate virtual focus. A feasibility test at SPring-8 under a photon energy of 10 keV demonstrated that the beam size can be varied between 134 and 1010 nm.

Optimal deformation procedure for hybrid adaptive x-ray mirror based on mechanical and piezo-driven bending system.

A hybrid deformable x-ray mirror consisting of a mechanical bender and a bimorph deformable mirror has been developed to realize adaptive optical systems, such as zoom condenser optics, for synchrotron-radiation-based x-ray microscopy. In the developed system, both bending mechanisms comprehensively contribute to the formation of the target mirror shape and can narrow the role of piezoelectric actuators, thereby enabling a more stable operation. In this study, the behavior of the bimorph mirror under the clamped condition was investigated, and the sharing of the deformation amount for each bending mechanism was optimized to minimize the amplitude of the voltage distribution of the bimorph mirror.

High-throughput deterministic plasma etching using array-type plasma generator system.

A deterministic processing method is a high-precision finishing method, where the to-be-removed amount of material at each point of the work surface is calculated based on an accurately measured present surface shape and is removed precisely using a numerically controlled (NC) processing system. Although this method has achieved nanometer-scale accuracy, the method requires considerable time to scan the work surface, leading to low productivity. Therefore, using an individual on-off controllable array-type plasma generator covering the entire work surface, enabling simultaneous NC plasma processing is proposed herein. A novel intermittent gas flow system was constructed using cyclic on-off control of the gas supply and exhaust valves instead of the commonly used continuous gas flow to achieve uniform in-plane plasma etching. It was found that uniform removal could be achieved by combining it with a pulse-modulated high-frequency power supply and setting the plasma generation time in one cycle to be sufficiently short. Furthermore, a power control approach was developed for maintaining a constant plasma state, even while varying the plasma-generating array elements, which resulted in a demonstration experiment of NC plasma etching that successfully reduced the thickness variation of a silicon substrate.

High-resolution micro channel-cut crystal monochromator processed by plasma chemical vaporization machining for a reflection self-seeded X-ray free-electron laser.

A high-resolution micro channel-cut crystal monochromator (µCCM) composed of an Si(220) crystal is developed for the purpose of narrowing the bandwidth of a reflection self-seeded X-ray free-electron laser. Subsurface damage on the monochromator, which distorts the wavefront and broadens the bandwidth of the monochromatic seed beam, was removed by using a plasma etching technique. High diffraction performance of the monochromator was confirmed through evaluation with coherent X-rays. Reflection self-seeding operation was tested with the Si(220) µCCM at SPring-8 Angstrom Compact free-electron laser. A narrow average bandwidth of 0.6 eV, which is five times narrower than the value previously reported [I. Inoue et al., Nat. Photonics13, 319 (2019)10.1038/s41566-019-0365-y], was successfully obtained at 9 keV. The narrow-band X-ray beams with high intensity realized in this study will further expand the capabilities of X-ray free-electron lasers.

An abrasive-free chemical polishing method assisted by nickel catalyst generated by in situ electrochemical plating.

An abrasive-free polishing method using water and a Pt catalyst, called catalyst-referred etching (CARE), has been developed for the finishing of optical and semiconductor surfaces. This method realizes well-ordered surfaces with a smoothness of several tens of picometers without crystallographic disturbance. In this study, we propose a new CARE method using a Ni catalyst with in situ electrochemical plating and dissolution, which enable enhancing the catalytic capability of Ni. This method has advantages to realize more than ten times higher removal rate and better stability compared with the conventional CARE method.

A micro channel-cut crystal X-ray monochromator for a self-seeded hard X-ray free-electron laser.

A channel-cut Si(111) crystal with a channel width of 90 µm was developed for achieving reflection self-seeding in hard X-ray free-electron lasers (XFELs). With the crystal a monochromatic seed pulse is produced from a broadband XFEL pulse generated in the first undulator section with an optical delay of 119 fs at 10 keV. The small optical delay allows a temporal overlap between the seed optical pulse and the electron bunch by using a small magnetic chicane for the electron beam placed between two undulator sections. Peak reflectivity reached 67%, which is reasonable compared with the theoretical value of 81%. By using this monochromator, a monochromatic seed pulse without broadband background in the spectrum was obtained at SACLA with a conversion efficiency from a broadband XFEL pulse of 2 × 10-2, which is ∼10 times higher than the theoretical efficiency of transmission self-seeding using a thin diamond (400) monochromator.

Catalyzed chemical polishing of SiO2 glasses in pure water.

A catalytically assisted etching system was developed for the ultra-precision fabrication of optical components, such as X-ray mirrors and extreme-ultraviolet mask blanks. This study demonstrates that an atomically smooth surface with a sub-Angstrom root-mean-square roughness could be achieved on a SiO2 glass substrate using pure water and Pt as the etching solution and catalyst, respectively. Density functional theory calculations confirmed that the mechanistic pathway was involved in catalyzed hydrolysis. The significant roles of the catalyst were clarified to be the dissociation of water molecules and the stabilization of a meta-stable state, in which a hypervalent silicate state is induced, and the Si-O backbond is elongated and loosened. To confirm the role of the catalyst, the Pt metal was replaced by Au, and the observed drastic difference in the removal rate was attributed to the degree of stabilization of the metastable state.

X-ray optics for advanced ultrafast pump-probe X-ray experiments at SACLA.

X-ray optics were implemented for advanced ultrafast X-ray experiments with different techniques at the hard X-ray beamline BL3 of SPring-8 Ångstrom Compact free-electron LAser. A double channel-cut crystal monochromator (DCCM) and compound refractive lenses (CRLs) were installed to tailor the beam conditions. These X-ray optics can work simultaneously with an arrival-timing monitor that compensates for timing jitter and drift. Inner-walls of channel-cut crystals (CCs) in the DCCM were processed by plasma chemical vaporization machining to remove crystallographic damage. Four-bounced reflection profiles of the CCs were investigated and excellent diffraction qualities were achieved. The use of CRLs enabled two-dimensional X-ray focusing with a spot size of ∼1.5 µm × 1.5 µm full width at half-maximum, while keeping reasonable throughputs for a wide photon energy range of 5-15 keV.

Compact reflective imaging optics in hard X-ray region based on concave and convex mirrors.

We demonstrated that the combination of a hyperbolic convex and elliptical concave mirrors works as a compact reflective X-ray imaging system with a short optical focal length and large magnification factor. We performed an experiment to form a one-dimensional demagnified image with a demagnification factor of 321 within an approximately 2-m-long optical setup at an X-ray energy of 10 keV. The results showed that this imaging optics system is capable of providing a resolution of ~40 nm. From wavefront analysis, it was confirmed that the optics possessed a wide field-of-view with a significant reduction of comatic aberration.

Nearly diffraction-limited hard X-ray line focusing with hybrid adaptive X-ray mirror based on mechanical and piezo-driven deformation.

We have developed the new hybrid adaptive X-ray mirror based on mechanical and piezo-driven deformation to realize precise shape controllability on a long-length mirror. The mechanical bender approximately provides the required ellipse, while the piezoelectric actuators attached to the mirror correct very small residual errors to satisfy the diffraction-limited condition. The mechanical bender significantly reduces the role of the piezoelectric actuator, resulting in the suppression of accuracy degradation due to the drift and/or junction effect of the piezoelectric actuators. In addition, line focusing was demonstrated with two different numerical apertures at SPring-8, and the obtained beam sizes were 127 and 253 nm (FWHM), which agree well with the diffraction-limited sizes.

Performance of a hard X-ray split-and-delay optical system with a wavefront division.

The performance of a hard X-ray split-and-delay optical (SDO) system with a wavefront division scheme was investigated at the hard X-ray free-electron laser facility SACLA. For the wavefront division, beam splitters made of edge-polished perfect Si(220) crystals were employed. We characterized the beam properties of the SDO system, and investigated its capabilities for beam manipulation and diagnostics. First, it was confirmed that shot-to-shot non-invasive diagnostics of pulse energies for both branches in the SDO system was feasible. Second, nearly ideal and identical focal profiles for both branches were obtained with a spot size of ∼1.5 µm in full width at half-maximum. Third, a spatial overlap of the two focused beams with a sub-µm accuracy was achieved by fine tuning of the SDO system. Finally, a reliable tunability of the delay time between two pulses was confirmed. The time interval was measured with an X-ray streak camera by changing the path length of the variable-delay branch. Errors from the fitted line were evaluated to be as small as ±0.4 ps over a time range of 60 ps.

Characterization of temporal coherence of hard X-ray free-electron laser pulses with single-shot interferograms.

Temporal coherence is one of the most fundamental characteristics of light, connecting to spectral information through the Fourier transform relationship between time and frequency. Interferometers with a variable path-length difference (PLD) between the two branches have widely been employed to characterize temporal coherence properties for broad spectral regimes. Hard X-ray interferometers reported previously, however, have strict limitations in their operational photon energies, due to the specific optical layouts utilized to satisfy the stringent requirement for extreme stability of the PLD at sub-ångström scales. The work presented here characterizes the temporal coherence of hard X-ray free-electron laser (XFEL) pulses by capturing single-shot interferograms. Since the stability requirement is drastically relieved with this approach, it was possible to build a versatile hard X-ray interferometer composed of six separate optical elements to cover a wide photon energy range from 6.5 to 11.5 keV while providing a large variable delay time of up to 47 ps at 10 keV. A high visibility of up to 0.55 was observed at a photon energy of 10 keV. The visibility measurement as a function of time delay reveals a mean coherence time of 5.9 ±â€…0.7 fs, which agrees with that expected from the single-shot spectral information. This is the first result of characterizing the temporal coherence of XFEL pulses in the hard X-ray regime and is an important milestone towards ultra-high energy resolutions at micro-electronvolt levels in time-domain X-ray spectroscopy, which will open up new opportunities for revealing dynamic properties in diverse systems on timescales from femto-seconds to nanoseconds, associated with fluctuations from ångström to nanometre spatial scales.

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.

Simulation of concave-convex imaging mirror system for development of a compact and achromatic full-field x-ray microscope.

We propose the use of two pairs of concave-convex mirrors as imaging optics for the compact full-field x-ray microscope with high resolution and magnification factors. The optics consists of two pairs of hyperbolic convex and elliptical concave mirrors with the principal surface near the object, consequently enabling the focal length to be 10 times shorter than conventional advanced Kirkpatrick-Baez mirror optics. This paper describes characteristics of the optics calculated by ray-tracing and wave-optical simulators. The expected spatial resolution is approximately 40 nm with a wide field of view of more than 10 µm and a total length of about 2 m, which may lead to the possibility of laboratory-sized, achromatic, and high-resolution full-field x-ray microscopes.

Development of speckle-free channel-cut crystal optics using plasma chemical vaporization machining for coherent x-ray applications.

We have developed a method of fabricating speckle-free channel-cut crystal optics with plasma chemical vaporization machining, an etching method using atmospheric-pressure plasma, for coherent X-ray applications. We investigated the etching characteristics to silicon crystals and achieved a small surface roughness of less than 1 nm rms at a removal depth of >10 µm, which satisfies the requirements for eliminating subsurface damage while suppressing diffuse scattering from rough surfaces. We applied this method for fabricating channel-cut Si(220) crystals for a hard X-ray split-and-delay optical system and confirmed that the crystals provided speckle-free reflection profiles under coherent X-ray illumination.

Wavelength-tunable split-and-delay optical system for hard X-ray free-electron lasers.

We developed a hard X-ray split-and-delay optical (SDO) system based on Bragg diffraction in crystal optics for generating two split pulses with a variable temporal separation. To achieve both high stability and operational flexibility, the SDO system was designed to include variable-delay and fixed-delay branches. As key optical elements, we fabricated high quality thin crystals and channel-cut crystals by applying the plasma chemical vaporization machining technique. The SDO system using Si(220) crystals covered a photon energy range of 6.5-11.5keV and a delay time range from a negative value to > 45 ps over the photon energy range (up to 220 ps at 6.5 keV). A simple alignment method for realizing a spatial overlap between the split pulses was developed. The SDO system was tested at a SPring-8 beamline in combination with a focusing system. We achieved an excellent overlap with an accuracy of 30 nm for ∼ 200 nm focused beams in both the horizontal and vertical directions. This achievement is an important progress towards the realization of time-resolved studies using multiple X-ray pulses with a time range from femtosecond to subnanosecond scales at X-ray free-electron laser facilities.

Nearly diffraction-limited X-ray focusing with variable-numerical-aperture focusing optical system based on four deformable mirrors.

Unlike the electrostatic and electromagnetic lenses used in electron microscopy, most X-ray focusing optical systems have fixed optical parameters with constant numerical apertures (NAs). This lack of adaptability has significantly limited application targets. In the research described herein, we developed a variable-NA X-ray focusing system based on four deformable mirrors, two sets of Kirkpatrick-Baez-type focusing mirrors, in order to control the focusing size while keeping the position of the focus unchanged. We applied a mirror deformation procedure using optical/X-ray metrology for offline/online adjustments. We performed a focusing test at a SPring-8 beamline and confirmed that the beam size varied from 108 nm to 560 nm (165 nm to 1434 nm) in the horizontal (vertical) direction by controlling the NA while maintaining diffraction-limited conditions.

Damage threshold of platinum/carbon multilayers under hard X-ray free-electron laser irradiation.

We evaluated the irradiation damage induced by hard X-ray free-electron lasers to platinum/carbon multilayers intended for use in a focusing reflective mirror. In order to determine the damage threshold, we compared X-ray reflectivities before and after irradiation at the first-order Bragg angle using a focused X-ray free-electron laser with a beam size of approximately 1 µm and a pulse energy ranging from 0.01 to 10 µJ at a photon energy of 10 keV. We confirmed that the damage threshold of the platinum/carbon multilayer with a bilayer period of 3 nm was 0.051 µJ/µm(2), which is sufficiently higher than that in practical applications.