Focused ion beam preparation of samples for X‐ray nanotomography

The preparation of hard material samples with the necessary size and shape is critical to successful material analysis. X‐ray nanotomography requires that samples are sufficiently thin for X‐rays to pass through the sample during rotation for tomography. One method for producing samples that fit the criteria for X‐ray nanotomography is focused ion beam/scanning electron microscopy (FIB/SEM) which uses a focused beam of ions to selectively mill around a region of interest and then utilizes a micromanipulator to remove the milled‐out sample from the bulk material and mount it on a sample holder. In this article the process for preparing X‐ray nanotomography samples in multiple shapes and sizes is discussed. Additionally, solid‐oxide fuel cell anode samples prepared through the FIB/SEM technique underwent volume‐independence studies for multiple properties such as volume fraction, average particle size, tortuosity and contiguity to observe the characteristics of FIB/SEM samples in X‐ray nanotomography.     

Direct nano‐scale patterning of Ag films using hard X‐ray induced oxidation

The morphological change of silver nano‐particles (AgNPs) exposed to an intense synchrotron X‐ray beam was investigated for the purpose of direct nano‐scale patterning of metal thin films. AgNPs irradiated by hard X‐rays in oxygen ambient were oxidized and migrated out of the illuminated region. The observed X‐ray induced oxidation was utilized to fabricate nano‐scale metal line patterns using sectioned WSi₂/Si multilayers as masks. Lines with a width as small as 21 nm were successfully fabricated on Ag films on silicon nitride. Au/Ag nano‐lines were also fabricated using the proposed method.     

Status of the hard X‐ray microprobe beamline ID22 of the European Synchrotron Radiation Facility

The ESRF synchrotron beamline ID22, dedicated to hard X‐ray microanalysis and consisting of the combination of X‐ray fluorescence, X‐ray absorption spectroscopy, diffraction and 2D/3D X‐ray imaging techniques, is one of the most versatile instruments in hard X‐ray microscopy science. This paper describes the present beamline characteristics, recent technical developments, as well as a few scientific examples from recent years of the beamline operation. The upgrade plans to adapt the beamline to the growing needs of the user community are briefly discussed.     

Point spread function measurement of an X‐ray beam focused by a multilayer zone plate with narrow annular aperture

The experimental procedure for obtaining the point spread function (PSF) of a focusing beam generated using an X‐ray multilayer zone plate (MZP) with a narrow annular aperture has been developed. It was possible to reconstruct the PSF by applying the tomographic process to the measured dataset consisting of line spread functions (LSFs) in every radial direction on the focal plane. The LSFs were measured by a knife‐edge scanning method of detecting scattered intensity. In the experimental work, quasi‐monochromatic undulator radiation with a first harmonic energy of 20 keV was directly focused without a monochromator by the MZP, and the PSF was measured using this procedure. As a result, a near diffraction‐limited focused beam size of 46 nm full width at half‐maximum was obtained.     

Confocal full‐field X‐ray microscope for novel three‐dimensional X‐ray imaging

A confocal full‐field X‐ray microscope has been developed for use as a novel three‐dimensional X‐ray imaging method. The system consists of an X‐ray illuminating `sheet‐beam' whose beam shape is micrified only in one dimension, and an X‐ray full‐field microscope whose optical axis is normal to the illuminating sheet beam. An arbitral cross‐sectional region of the object is irradiated by the sheet‐beam, and secondary X‐ray emission such as fluorescent X‐rays from this region is imaged simultaneously using the full‐field microscope. This system enables a virtual sliced image of a specimen to be obtained as a two‐dimensional magnified image, and three‐dimensional observation is available only by a linear translation of the object along the optical axis of the full‐field microscope. A feasibility test has been carried out at beamline 37XU of SPring‐8. Observation of the three‐dimensional distribution of metallic inclusions in an artificial diamond was performed.     

Silicon nitride transmission X‐ray mirrors

Transmission X‐ray mirrors have been fabricated from 300–400 nm‐thick low‐stress silicon nitride windows of size 0.6 mm × 85 mm. The windows act as a high‐pass energy filter at grazing incidence in an X‐ray beam for the beam transmitted through the window. The energy cut‐off can be selected by adjusting the incidence angle of the transmission mirror, because the energy cut‐off is a function of the angle of the window with respect to the beam. With the transmission mirror at the target angle of 0.22°, a 0.3 mm × 0.3 mm X‐ray beam was allowed to pass through the mirror with a cut‐off energy of 10 keV at the Cornell High Energy Synchrotron Source. The energy cut‐off can be adjusted from 8 to 12 keV at an angle of 0.26° to 0.18°, respectively. The observed mirror transmittance was above 80% for a 300 nm‐thick film.     

A sub‐micrometer resolution hard X‐ray microprobe system of BL8C at Pohang Light Source

A microprobe system has been installed on the nanoprobe/XAFS beamline (BL8C) at PLS‐II, South Korea. Owing to the reproducible switch of the gap of the in‐vacuum undulator (IVU), the intense and brilliant hard X‐ray beam of an IVU can be used in X‐ray fluorescence (XRF) and X‐ray absorption fine‐structure (XAFS) experiments. For high‐spatial‐resolution microprobe experiments a Kirkpatrick–Baez mirror system has been used to focus the millimeter‐sized X‐ray beam to a micrometer‐sized beam. The performance of this system was examined by a combination of micro‐XRF imaging and micro‐XAFS of a beetle wing. These results indicate that the microprobe system of the BL8C can be used to obtain the distributions of trace elements and chemical and structural information of complex materials.     

Polarization control of an X‐ray free‐electron laser with a diamond phase retarder

A diamond phase retarder was applied to control the polarization states of a hard X‐ray free‐electron laser (XFEL) in the photon energy range 5–20 keV. The horizontal polarization of the XFEL beam generated from the planar undulators of the SPring‐8 Angstrom Compact Free‐Electron Laser (SACLA) was converted into vertical or circular polarization of either helicity by adjusting the angular offset of the diamond crystal from the exact Bragg condition. Using a 1.5 mm‐thick crystal, a high degree of circular polarization, 97%, was obtained for 11.56 keV monochromatic X‐rays, whereas the degree of vertical polarization was 67%, both of which agreed with the estimations including the energy bandwidth of the Si 111 beamline monochromator.     

X‐ray focusing by the system of refractive lens(es) placed inside asymmetric channel‐cut crystals

An X‐ray one‐dimensionally focusing system, a refracting–diffracting lens (RDL), composed of Bragg double‐asymmetric‐reflecting two‐crystal plane parallel plates and a double‐concave cylindrical parabolic lens placed in the gap between the plates is described. It is shown that the focal length of the RDL is equal to the focal distance of the separate lens multiplied by the square of the asymmetry factor. One can obtain RDLs with different focal lengths for certain applications. Using the point‐source function of dynamic diffraction, as well as the Green function in a vacuum with parabolic approximation, an expression for the double‐diffracted beam amplitude for an arbitrary incident wave is presented. Focusing of the plane incident wave and imaging of a point source are studied. The cases of non‐absorptive and absorptive lenses are discussed. The intensity distribution in the focusing plane and on the focusing line, and its dependence on wavelength, deviation from the Bragg angle and magnification is studied. Geometrical optical considerations are also given. RDLs can be applied to focus radiation from both laboratory and synchrotron X‐ray sources, for X‐ray imaging of objects, and for obtaining high‐intensity beams. RDLs can also be applied in X‐ray astronomy.     

Ultra‐thin optical grade scCVD diamond as X‐ray beam position monitor

Results of measurements made at the SIRIUS beamline of the SOLEIL synchrotron for a new X‐ray beam position monitor based on a super‐thin single crystal of diamond grown by chemical vapor deposition (CVD) are presented. This detector is a quadrant electrode design processed on a 3 µm‐thick membrane obtained by argon–oxygen plasma etching the central area of a CVD‐grown diamond plate of 60 µm thickness. The membrane transmits more than 50% of the incident 1.3 keV energy X‐ray beam. The diamond plate was of moderate purity (～1 p.p.m. nitrogen), but the X‐ray beam induced current (XBIC) measurements nevertheless showed a photo‐charge collection efficiency approaching 100% for an electric field of 2 V µm^?1, corresponding to an applied bias voltage of only 6 V. XBIC mapping of the membrane showed an inhomogeneity of more than 10% across the membrane, corresponding to the measured variation in the thickness of the diamond plate before the plasma etching process. The measured XBIC signal‐to‐dark‐current ratio of the device was greater than 10⁵, and the X‐ray beam position resolution of the device was better than a micrometer for a 1 kHz sampling rate.     

Collimating Montel mirror as part of a multi‐crystal analyzer system for resonant inelastic X‐ray scattering

Advances in resonant inelastic X‐ray scattering (RIXS) have come in lockstep with improvements in energy resolution. Currently, the best energy resolution at the Ir L₃‐edge stands at ～25 meV, which is achieved using a diced Si(844) spherical crystal analyzer. However, spherical analyzers are limited by their intrinsic reflection width. A novel analyzer system using multiple flat crystals provides a promising way to overcome this limitation. For the present design, an energy resolution at or below 10 meV was selected. Recognizing that the angular acceptance of flat crystals is severely limited, a collimating element is essential to achieve the necessary solid‐angle acceptance. For this purpose, a laterally graded, parabolic, multilayer Montel mirror was designed for use at the Ir L₃‐absorption edge. It provides an acceptance larger than 10 mrad, collimating the reflected X‐ray beam to smaller than 100 µrad, in both vertical and horizontal directions. The performance of this mirror was studied at beamline 27‐ID at the Advanced Photon Source. X‐rays from a diamond (111) monochromator illuminated a scattering source of diameter 5 µm, generating an incident beam on the mirror with a well determined divergence of 40 mrad. A flat Si(111) crystal after the mirror served as the divergence analyzer. From X‐ray measurements, ray‐tracing simulations and optical metrology results, it was established that the Montel mirror satisfied the specifications of angular acceptance and collimation quality necessary for a high‐resolution RIXS multi‐crystal analyzer system.     

A miniature X‐ray emission spectrometer (miniXES) for high‐pressure studies in a diamond anvil cell

Core–shell X‐ray emission spectroscopy (XES) is a valuable complement to X‐ray absorption spectroscopy (XAS) techniques. However, XES in the hard X‐ray regime is much less frequently employed than XAS, often as a consequence of the relative scarcity of XES instrumentation having energy resolutions comparable with the relevant core‐hole lifetimes. To address this, a family of inexpensive and easily operated short‐working‐distance X‐ray emission spectrometers has been developed. The use of computer‐aided design and rapid prototype machining of plastics allows customization for various emission lines having energies from ～3 keV to ～10 keV. The specific instrument described here, based on a coarsely diced approximant of the Johansson optic, is intended to study volume collapse in Pr metal and compounds by observing the pressure dependence of the Pr Lα emission spectrum. The collection solid angle is ～50 msr, roughly equivalent to that of six traditional spherically bent crystal analyzers. The miniature X‐ray emission spectrometer (miniXES) methodology will help encourage the adoption and broad application of high‐resolution XES capabilities at hard X‐ray synchrotron facilities.     

A sagittally focusing double‐multilayer monochromator for ultrafast X‐ray imaging applications

The development of a sagittally focusing double‐multilayer monochromator is reported, which produces a spatially extended wide‐bandpass X‐ray beam from an intense synchrotron bending‐magnet source at the Advanced Photon Source, for ultrafast X‐ray radiography and tomography applications. This monochromator consists of two W/B₄C multilayers with a 25 Å period coated on Si single‐crystal substrates. The second multilayer is mounted on a sagittally focusing bender, which can dynamically change the bending radius of the multilayer in order to condense and focus the beam to various points along the beamline. With this new apparatus, it becomes possible to adjust the X‐ray beam size to best match the area detector size and the object size to facilitate more efficient data collection using ultrafast X‐ray radiography and tomography.     

The first microbeam synchrotron X‐ray fluorescence beamline at the Siam Photon Laboratory

The first microbeam synchrotron X‐ray fluorescence (µ‐SXRF) beamline using continuous synchrotron radiation from Siam Photon Source has been constructed and commissioned as of August 2011. Utilizing an X‐ray capillary half‐lens allows synchrotron radiation from a 1.4 T bending magnet of the 1.2 GeV electron storage ring to be focused from a few millimeters‐sized beam to a micrometer‐sized beam. This beamline was originally designed for deep X‐ray lithography (DXL) and was one of the first two operational beamlines at this facility. A modification has been carried out to the beamline in order to additionally enable µ‐SXRF and synchrotron X‐ray powder diffraction (SXPD). Modifications included the installation of a new chamber housing a Si(111) crystal to extract 8 keV synchrotron radiation from the white X‐ray beam (for SXPD), a fixed aperture and three gate valves. Two end‐stations incorporating optics and detectors for µ‐SXRF and SXPD have then been installed immediately upstream of the DXL station, with the three techniques sharing available beam time. The µ‐SXRF station utilizes a polycapillary half‐lens for X‐ray focusing. This optic focuses X‐ray white beam from 5 mm × 2 mm (H × V) at the entrance of the lens down to a diameter of 100 µm FWHM measured at a sample position 22 mm (lens focal point) downstream of the lens exit. The end‐station also incorporates an XYZ motorized sample holder with 25 mm travel per axis, a 5× ZEISS microscope objective with 5 mm × 5 mm field of view coupled to a CCD camera looking to the sample, and an AMPTEK single‐element Si (PIN) solid‐state detector for fluorescence detection. A graphic user interface data acquisition program using the LabVIEW platform has also been developed in‐house to generate a series of single‐column data which are compatible with available XRF data‐processing software. Finally, to test the performance of the µ‐SXRF beamline, an elemental surface profile has been obtained for a piece of ancient pottery from the Ban Chiang archaeological site, a UNESCO heritage site. It was found that the newly constructed µ‐SXRF technique was able to clearly distinguish the distribution of different elements on the specimen.     

A method of hard X‐ray phase‐shifting digital holography

A new method of phase‐shifting digital holography is demonstrated in the hard X‐ray region. An in‐line‐type phase‐shifting holography setup was installed in a 6.80 keV hard X‐ray synchrotron beamline. By placing a phase plate consisting of a hole and a band at the focusing point of a Fresnel lens, the relative phase of the reference and objective beams could be successfully shifted for use with a three‐step phase‐shift algorithm. The system was verified by measuring the shape of a gold test pattern and a silica sphere.     

Beam‐shaping condenser lenses for full‐field transmission X‐ray microscopy

A new type of diffractive X‐ray optical elements is reported, which have been used as beam‐shaping condenser lenses in full‐field transmission X‐ray microscopes. These devices produce a square‐shaped flat‐top illumination on the sample matched to the field of view. The size of the illumination can easily be designed depending on the geometry and requirements of the specific experimental station. Gold and silicon beam‐shapers have been fabricated and tested in full‐field microscopes in the hard and soft X‐ray regimes, respectively.     

Application of kinoform lens for X‐ray reflectivity analysis

In this paper the first practical application of kinoform lenses for the X‐ray reflectivity characterization of thin layered materials is demonstrated. The focused X‐ray beam generated from a kinoform lens, a line of nominal size ～50 µm × 2 µm, provides a unique possibility to measure the X‐ray reflectivities of thin layered materials in sample scanning mode. Moreover, the small footprint of the X‐ray beam, generated on the sample surface at grazing incidence angles, enables one to measure the absolute X‐ray reflectivities. This approach has been tested by analyzing a few thin multilayer structures. The advantages achieved over the conventional X‐ray reflectivity technique are discussed and demonstrated by measurements.     

X‐ray dynamical diffraction Fraunhofer holography

An X‐ray dynamical diffraction Fraunhofer holographic scheme is proposed. Theoretically it is shown that the reconstruction of the object image by visible light is possible. The spatial and temporal coherence requirements of the incident X‐ray beam are considered. As an example, the hologram recording as well as the reconstruction by visible light of an absolutely absorbing wire are discussed.     

XDS: a flexible beamline for X‐ray diffraction and spectroscopy at the Brazilian synchrotron

The majority of the beamlines at the Brazilian Synchrotron Light Source Laboratory (LNLS) use radiation produced in the storage‐ring bending magnets and are therefore currently limited in the flux that can be used in the harder part of the X‐ray spectrum (above ～10 keV). A 4 T superconducting multipolar wiggler (SCW) was recently installed at LNLS in order to improve the photon flux above 10 keV and fulfill the demands set by the materials science community. A new multi‐purpose beamline was then installed at the LNLS using the SCW as a photon source. The XDS is a flexible beamline operating in the energy range between 5 and 30 keV, designed to perform experiments using absorption, diffraction and scattering techniques. Most of the work performed at the XDS beamline concentrates on X‐ray absorption spectroscopy at energies above 18 keV and high‐resolution diffraction experiments. More recently, new setups and photon‐hungry experiments such as total X‐ray scattering, X‐ray diffraction under high pressures, resonant X‐ray emission spectroscopy, among others, have started to become routine at XDS. Here, the XDS beamline characteristics, performance and a few new experimental possibilities are described.     

A novel monochromator for experiments with ultrashort X‐ray pulses

Aiming at advancing storage‐ring‐based ultrafast X‐ray science, over the past few years many upgrades have been undertaken to continue improving beamline performance and photon flux at the Femtoslicing facility at BESSY II. In this article the particular design upgrade of one of the key optical components, the zone‐plate monochromator (ZPM) beamline, is reported. The beamline is devoted to optical pump/soft X‐ray probe applications with 100 fs (FWHM) X‐ray pulses in the soft X‐ray range at variable polarization. A novel approach consisting of an array of nine off‐axis reflection zone plates is used for a gapless coverage of the spectral range between 410 and 1333 eV at a designed resolution of E/ΔE = 500 and a pulse elongation of only 30 fs. With the upgrade of the ZPM the following was achieved: a smaller focus, an improved spectral resolution and bandwidth as well as excellent long‐term stability. The beamline will enable a new class of ultrafast applications with variable optical excitation wavelength and variable polarization.