Propagation-based phase-contrast imaging method for full-field X-ray microscopy using advanced Kirkpatrick-Baez mirrors.

We demonstrate a propagation-based phase-contrast imaging method for full-field X-ray microscopy based on advanced Kirkpatrick-Baez (AKB) mirrors to achieve high-contrast observations of weak phase objects and correct field curvature aberrations. Through a demonstration performed at SPring-8, the phase contrast of weak phase objects such as polystyrene spheres and chemically fixed cells was successfully observed with high sensitivity (∼0.03 rad). Furthermore, the field of view of the AKB mirrors was expanded to the full area of the obtained images (25 × 30 µm) by correcting the field curvature aberration using reconstructed complex wavefields.

Femtosecond Reduction of Atomic Scattering Factors Triggered by Intense X-Ray Pulse.

X-ray diffraction of silicon irradiated with tightly focused femtosecond x-ray pulses (photon energy, 11.5 keV; pulse duration, 6 fs) was measured at various x-ray intensities up to 4.6×10^{19} W/cm^{2}. The measurement reveals that the diffraction intensity is highly suppressed when the x-ray intensity reaches of the order of 10^{19} W/cm^{2}. With a dedicated simulation, we confirm that the observed reduction of the diffraction intensity can be attributed to the femtosecond change in individual atomic scattering factors due to the ultrafast creation of highly ionized atoms through photoionization, Auger decay, and subsequent collisional ionization. We anticipate that this ultrafast reduction of atomic scattering factor will be a basis for new x-ray nonlinear techniques, such as pulse shortening and contrast variation x-ray scattering.

Wide field-of-view x-ray imaging optical system using grazing-incidence mirrors.

A field-curvature-corrected imaging optical system for x-ray microscopy using only grazing-incidence mirrors is proposed. It combines a Wolter type I (WO1) mirror pair, which forms a real image, with field curvature correction (FCC) optics-a convex hyperbolic mirror pair-that form a virtual image; compensation of the field curvatures realizes a wide field-of-view (FOV) and high magnification. Ray-tracing and wave-optics simulations verified the efficacy of the design, for which a FOV width was 111 µm-4.7 times larger than that for the uncorrected WO1 design. The addition of FCC optics also produced a 2.3-fold increase in magnification.

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.

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.

Focus characterization of an X-ray free-electron laser by intensity correlation measurement of X-ray fluorescence.

This paper proposes and demonstrates a simple method using the intensity correlation of X-ray fluorescence to evaluate the focused beam size of an X-ray free-electron laser (XFEL). This method was applied to the sub-micrometre focused XFEL beam at the SPring-8 Angstrom Compact Free Electron Laser, and the beam size evaluated using the proposed method was consistent with that measured using the knife-edge scan method. The proposed method is readily applicable to extremely small X-ray spots and can be applied for the precise diagnostics of sub-10 nm focused X-ray beams which have recently emerged.

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.

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.

High surface laser-induced damage threshold of SrB4O7 single crystals under 266-nm (DUV) laser irradiation.

Under 266-nm (deep ultraviolet, DUV) laser irradiation, an SrB4O7 (SBO) single crystal has been found to exhibit a surface laser-induced damage threshold (LIDT) of ∼ 16.4 J/cm2, which is higher than those of a synthetic silica glass (4.8 J/cm2) and a calcium fluoride (CaF2) crystal (11.4 J/cm2). By catalyst-referred etching (CARE), the LIDT of an SBO crystal can also be improved to around 24.1 J/cm2, which is 1.4 and 6.0 times higher compared to an unetched crystal and a silica glass, respectively. With high surface LIDTs, SBO single crystals can then be used as optical window materials for high-power DUV laser systems.

X-Ray Single-Grating Interferometry for Wavefront Measurement and Correction of Hard X-Ray Nanofocusing Mirrors.

X-ray single-grating interferometry was applied to conduct accurate wavefront corrections for hard X-ray nanofocusing mirrors. Systematic errors in the interferometer, originating from a grating, a detector, and alignment errors of the components, were carefully examined. Based on the measured wavefront errors, the mirror shapes were directly corrected using a differential deposition technique. The corrected X-ray focusing mirrors with a numerical aperture of 0.01 attained two-dimensionally diffraction-limited performance. The results of the correction indicate that the uncertainty of the wavefront measurement was less than λ/72 in root-mean-square value.

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.

Full-field X-ray fluorescence microscope based on total-reflection advanced Kirkpatrick-Baez mirror optics.

A novel full-field X-ray fluorescence microscope based on total-reflection advanced Kirkpatrick-Baez mirror optics was developed. The total-reflection imaging mirror optics arrangement, with four reflections, has the advantage of being able to function both as a powerful low-pass energy filter, completely rejecting incident excitation X-rays, and as an achromatic optical imaging system. Isolated X-ray fluorescence signals can be imaged, avoiding imaging-detector saturation, with low background noise. A prototype fluorescence microscope constructed at SPring-8 demonstrated the capability to simultaneously image elemental distributions using various X-ray fluorescence signals (Ni, Cu, Zn, Ge, and Bi). A half-period spatial resolution of ~0.5-1 µm (1000-500 LP/mm) was achieved, owing to the achromaticity of the imaging mirrors and the photon-counting scheme of the CCD camera used for fluorescence detection.

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.

Generation of apodized X-ray illumination and its application to scanning and diffraction microscopy.

X-ray science has greatly benefited from the progress in X-ray optics. Advances in the design and the manufacturing techniques of X-ray optics are key to the success of various microscopic and spectroscopic techniques practiced today. Here the generation of apodized X-ray illumination using a two-stage deformable Kirkpatrick-Baez mirror system is presented. Such apodized illumination is marked by the suppression of the side-lobe intensities of the focused beam. Thus generated apodized illumination was employed to improve the image quality in scanning X-ray fluorescence microscopy. Imaging of a non-isolated object by coherent X-ray diffractive imaging with apodized illumination in a non-scanning mode is also presented.

Imaging of intracellular fatty acids by scanning X-ray fluorescence microscopy.

Fatty acids are taken up by cells and incorporated into complex lipids such as neutral lipids and glycerophospholipids. Glycerophospholipids are major constituents of cellular membranes. More than 1000 molecular species of glycerophospholipids differ in their polar head groups and fatty acid compositions. They are related to cellular functions and diseases and have been well analyzed by mass spectrometry. However, intracellular imaging of fatty acids and glycerophospholipids has not been successful due to insufficient resolution using conventional methods. Here, we developed a method for labeling fatty acids with bromine (Br) and applied scanning X-ray fluorescence microscopy (SXFM) to obtain intracellular Br mapping data with submicrometer resolution. Mass spectrometry showed that cells took up Br-labeled fatty acids and metabolized them mainly into glycerophospholipids in CHO cells. Most Br signals observed by SXFM were in the perinuclear region. Higher resolution revealed a spot-like distribution of Br in the cytoplasm. The current method enabled successful visualization of intracellular Br-labeled fatty acids. Single-element labeling combined with SXFM technology facilitates the intracellular imaging of fatty acids, which provides a new tool to determine dynamic changes in fatty acids and their derivatives at the single-cell level.-Shimura, M., Shindou, H., Szyrwiel, L., Tokuoka, S. M., Hamano, F., Matsuyama, S., Okamoto, M., Matsunaga, A., Kita, Y., Ishizaka, Y., Yamauchi, K., Kohmura, Y., Lobinski, R., Shimizu, I., Shimizu, T. Imaging of intracellular fatty acids by scanning X-ray fluorescence microscopy.

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.

Nanofocusing of X-ray free-electron lasers by grazing-incidence reflective optics.

Total-reflection mirror devices for X-ray free-electron laser focusing are discussed in terms of optical design, mirror-fabrication technology, a wavefront diagnosis method and radiation-damage testing, as a review of the present status of the focusing optics at the SPring-8 angstrom compact free-electron laser (SACLA). Designed beam sizes of 1 µm and 50 nm, and spot sizes almost matching prediction have been achieved and used to explore topics at the forefront of natural science. The feasibility of these devices is determined to be sufficient for long-term and stable operation at SACLA by investigating the radiation-damage threshold and achievable accuracies in the mirror figure and alignment.