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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

A Bragg beam splitter for hard x-ray free-electron lasers.

We report a Bragg beam splitter developed for utilization of hard x-ray free-electron lasers. The splitter is based on an ultrathin silicon crystal operating in the symmetric Bragg geometry to provide high reflectivity and transmissivity simultaneously. We fabricated frame-shaped Si(511) and (110) crystals with thicknesses below 10 µm by a reactive dry etching method using atmospheric-pressure plasma. The thickness variation over an illuminated area is less than 300 nm peak-to-valley. High crystalline perfection was verified by topographic and diffractometric measurements. The crystal thickness was evaluated from the period of the Pendellösung beats measured with a highly monochromatic and collimated x-ray probe. The crystals provide two replica pulses with uniform wavefront [(<1/50)λ] and low spatial intensity variation (<5%). These Bragg beam splitters will play an important role in innovating XFEL applications.

Hard-X-ray imaging optics based on four aspherical mirrors with 50 nm resolution.

Ultraprecise imaging optics, which consists of two sets of elliptical mirrors and hyperbolic mirrors aligned perpendicular to each other (i.e., advanced Kirkpatrick-Baez mirrrors), is developed to realize high-resolution and achromatic full-field hard-X-ray microscopy. Experiments to form a demagnified image (with horizontal and vertical demagnification factors of 385 and 210, respectively) are conducted to evaluate the optical system at an X-ray energy of 11.5 keV at SPring-8. Results show that the imaging system can form a demagnified image with nearly diffraction-limited resolutions of ~50 nm in the horizontal and vertical directions. The field of view is also experimentally estimated to be ~12 × ~14 µm(2) when used as a magnification imaging system.

Shape correction of optical surfaces using plasma chemical vaporization machining with a hemispherical tip electrode.

We propose a plasma chemical vaporization machining device with a hemispherical tip electrode for optical fabrication. Radio-frequency plasma is generated close to the electrode under atmospheric conditions, and a workpiece is scanned relative to the stationary electrode under three-axis motion control to remove target areas on a workpiece surface. Experimental results demonstrate that surface removal progresses although process gas is not forcibly supplied to the plasma. The correction of shape errors on conventionally polished spheres is performed. As a result, highly accurate smooth surfaces with the desired rms shape accuracy of 3 nm are successfully obtained, which confirms that the device is effective for the fabrication of optics.

Evaluation of Schottky barrier diodes fabricated directly on processed 4H-SiC(0001) surfaces.

Silicon carbide (SiC) is a suitable substrate for low-power-consumption power devices and high-temperature applications. However, this material is difficult to machine because of its hardness and chemical inertness, and many machining methods have been studied intensively in recent years. In this paper, we present a simple method to evaluate the electrical properties of the processed surface using the ideal factor n of a Schottky barrier diode (SBD) fabricated directly on the processed surface. Upon comparing the values of n for SBDs fabricated on a damaged SiC surface and a non-damaged SiC surface, we found that there is a significant difference in the dispersion and magnitude of n. Furthermore, by combining this technique with slope etching, we were able to estimate the thickness of the damaged sub-surface layer.

Electroforming for replicating nanometer-level smooth surface.

We proposed and developed a new electroforming process for the replication of surfaces having nanometer-level smoothness. In the electroforming process, the separation method plays an important role in preventing the degradation of the surface morphology. The key point in this process is the fabrication of a metal film as an electrode on the master surface. Cr atoms are deposited by an arc plasma deposition method and act as a binding material. Subsequently, a nickel film is fabricated by electron beam deposition to form an electrode. Electrodeposition is then carried out in a nickel sulfamate bath. By controlling the density of Cr atoms on the master surface, the binding strength between the nickel film and master surface can be adjusted, which makes it possible to separate the metal film from the master surface smoothly. As a result, a surface roughness of 0.22 nm (root mean square) has been achieved in a 64 microm x 48 microm area of a replicated surface.

Improved optical and electrical characteristics of free-standing GaN substrates by chemical polishing utilizing photo-electrochemical method.

The optical and electrical properties of GaN(0001) surfaces treated by a novel chemical polishing method are described. Scanning microscopic photoluminescence images reveal that the polished GaN surface shows improved luminescence properties compared to the untreated surface. Current-voltage measurements of Schottky barriers formed using the GaN substrates show that the polished GaN surface has a lower reverse leakage current, and that the barrier height and ideality factor are improved after the polishing treatment.

Dependence of process characteristics on atomic-step density in catalyst-referred etching of 4H-SiC(0001) surface.

Catalyst-referred etching (CARE) is a novel abrasive-free planarization method. CARE-processed 4H-SiC(0001) surfaces are extremely flat and undamaged over the whole wafer. They consist of single-bilayer-height atomic steps and atomically flat terraces. This suggests that the etching properties depend principally on the atomic-step density of the substrate surface. We used on-axis and 8 degrees off-axis substrates to investigate the processing characteristics that affect the atomic-step density of these substrates. We found a strong correlation between the removal rate and the atomic-step density of the two substrates. For the on-axis substrate, the removal rate increased with increasing surface roughness, which increases with an increasing atomic-step density. The removal rate ratio is approximately the same as the atomic-step density ratio of the two substrates.

Efficient wet etching of GaN (0001) substrate with subsurface damage layer.

Photoenhanced chemical (PEC) etching is applicable for processing an n-GaN (0001) surface rapidly. In this process, the surface oxidation is enhanced by photo-generated holes and the resulting oxide can dissolve into solutions. In current work, we conduct bias-assisted PEC etching in a KOH solution with a positively biased wafer, to remove the crystallographically highly damaged layer. The employed substrate was mechanically polished with diamond slurry of sub-micrometer particle size. Without the positive bias, the rate of PEC etching was quite low because the photogenerated holes were quickly depleted by the recombination process at the crystallographic defects and they could not contribute to the oxidation. On the other hand, in the case where the bias was applied, the photogenerated holes and electrons are separated forcibly in the band-bended surface, which effectively contributed to surface oxidation. As a result, a high removal rate was realized even on the damaged surface.

Structure and magnetic properties of mono- and bi-layer graphene films on ultraprecision figured 4H-SiC(0001) surfaces.

Monolayer and bilayer graphene films with a few hundred nm domain size were grown on ultraprecision figured 4H-SiC(0001) on-axis and 8 degrees -off surfaces by annealing in ultra-high vacuum. Using X-ray photoelectron spectroscopy (XPS), atomic force microscopy, reflection high-energy electron diffraction, low-energy electron diffraction (LEED), Raman spectroscopy, and scanning tunneling microscopy, we investigated the structure, number of graphene layers, and chemical bonding of the graphene surfaces. Moreover, the magnetic property of the monolayer graphene was studied using in-situ surface magneto-optic Kerr effect at 40 K. LEED spots intensity distribution and XPS spectra for monolayer and bilayer graphene films could become an obvious and accurate fingerprint for the determination of graphene film thickness on SiC surface.