Feasibility study of propagation‐based phase‐contrast X‐ray lung imaging on the Imaging and Medical beamline at the Australian Synchrotron

Propagation‐based phase‐contrast X‐ray imaging (PB‐PCXI) using synchrotron radiation has achieved high‐resolution imaging of the lungs of small animals both in real time and in vivo. Current studies are applying such imaging techniques to lung disease models to aid in diagnosis and treatment development. At the Australian Synchrotron, the Imaging and Medical beamline (IMBL) is well equipped for PB‐PCXI, combining high flux and coherence with a beam size sufficient to image large animals, such as sheep, due to a wiggler source and source‐to‐sample distances of over 137 m. This study aimed to measure the capabilities of PB‐PCXI on IMBL for imaging small animal lungs to study lung disease. The feasibility of combining this technique with computed tomography for three‐dimensional imaging and X‐ray velocimetry for studies of airflow and non‐invasive lung function testing was also investigated. Detailed analysis of the role of the effective source size and sample‐to‐detector distance on lung image contrast was undertaken as well as phase retrieval for sample volume analysis. Results showed that PB‐PCXI of lung phantoms and mouse lungs produced high‐contrast images, with successful computed tomography and velocimetry also being carried out, suggesting that live animal lung imaging will also be feasible at the IMBL.     

Live small‐animal X‐ray lung velocimetry and lung micro‐tomography at the Australian Synchrotron Imaging and Medical Beamline

The high flux and coherence produced at long synchrotron beamlines makes them well suited to performing phase‐contrast X‐ray imaging of the airways and lungs of live small animals. Here, findings of the first live‐animal imaging on the Imaging and Medical Beamline (IMBL) at the Australian Synchrotron are reported, demonstrating the feasibility of performing dynamic lung motion measurement and high‐resolution micro‐tomography. Live anaesthetized mice were imaged using 30 keV monochromatic X‐rays at a range of sample‐to‐detector propagation distances. A frame rate of 100 frames s^?1 allowed lung motion to be determined using X‐ray velocimetry. A separate group of humanely killed mice and rats were imaged by computed tomography at high resolution. Images were reconstructed and rendered to demonstrate the capacity for detailed, user‐directed display of relevant respiratory anatomy. The ability to perform X‐ray velocimetry on live mice at the IMBL was successfully demonstrated. High‐quality renderings of the head and lungs visualized both large structures and fine details of the nasal and respiratory anatomy. The effect of sample‐to‐detector propagation distance on contrast and resolution was also investigated, demonstrating that soft tissue contrast increases, and resolution decreases, with increasing propagation distance. This new capability to perform live‐animal imaging and high‐resolution micro‐tomography at the IMBL enhances the capability for investigation of respiratory diseases and the acceleration of treatment development in Australia.     

A method to determine the absolute harmonic content of an X‐ray beam using attenuation measurements

We present a new method for determining the absolute harmonic content of an X‐ray beam. The technique is applied to determine the harmonic content of a synchrotron beam to high‐accuracy by measuring the X‐ray attenuation of a large number of aluminium foils with thicknesses varying over several orders of magnitude. Earlier methods always determined relative quantities such as the effective harmonic content, which are dependant on experimental geometry and not transferable between detectors. We use a more fundamental and useful parameter: the harmonic‐photon percentage. Copyright © 2009 John Wiley & Sons, Ltd.     

High‐efficiency coherence‐preserving harmonic rejection with crystal optics

This work reports a harmonic‐rejection scheme based on the combination of Si(111) monochromator and Si(220) harmonic‐rejection crystal optics. This approach is of importance to a wide range of X‐ray applications in all three major branches of modern X‐ray science (scattering, spectroscopy, imaging) based at major facilities, and especially relevant to the capabilities offered by the new diffraction‐limited storage rings. It was demonstrated both theoretically and experimentally that, when used with a synchrotron undulator source over a broad range of X‐ray energies of interest, the harmonic‐rejection crystals transmit the incident harmonic X‐rays on the order of 10^?6. Considering the flux ratio of fundamental and harmonic X‐rays in the incident beam, this scheme achieves a total flux ratio of harmonic radiation to fundamental radiation on the order of 10^?10. The spatial coherence of the undulator beam is preserved in the transmitted fundamental radiation while the harmonic radiation is suppressed, making this scheme suitable not only for current third‐generation synchrotron sources but also for the new diffraction‐limited storage rings where coherence preservation is an even higher priority. Compared with conventional harmonic‐rejection mirrors, where coherence is poorly preserved and harmonic rejection is less effective, this scheme has the added advantage of lower cost and footprint. This approach has been successfully utilized at the ultra‐small‐angle X‐ray scattering instrument at the Advanced Photon Source for scattering, imaging and coherent X‐ray photon correlation spectroscopy experiments. With minor modification, the harmonic rejection can be improved by a further five orders of magnitude, enabling even more performance capabilities.     

Position and flux stabilization of X‐ray beams produced by double‐crystal monochromators for EXAFS scans at the titanium K‐edge

The simultaneous and active feedback stabilization of X‐ray beam position and monochromatic beam flux during EXAFS scans at the titanium K‐edge as produced by a double‐crystal monochromator beamline is reported. The feedback is generated using two independent feedback loops using separate beam flux and position measurements. The flux is stabilized using a fast extremum‐searching algorithm that is insensitive to changes in the synchrotron ring current and energy‐dependent monochromator output. Corrections of beam height are made using an innovative transmissive beam position monitor instrument. The efficacy of the feedback stabilization method is demonstrated by comparing the measurements of EXAFS spectra on inhomogeneous diluted Ti‐containing samples with and without feedback applied.     

Analysis and interpretation of the first monochromatic X‐ray tomography data collected at the Australian Synchrotron Imaging and Medical beamline

The first monochromatic X‐ray tomography experiments conducted at the Imaging and Medical beamline of the Australian Synchrotron are reported. The sample was a phantom comprising nylon line, Al wire and finer Cu wire twisted together. Data sets were collected at four different X‐ray energies. In order to quantitatively account for the experimental values obtained for the Hounsfield (or CT) number, it was necessary to consider various issues including the point‐spread function for the X‐ray imaging system and harmonic contamination of the X‐ray beam. The analysis and interpretation of the data includes detailed considerations of the resolution and efficiency of the CCD detector, calculations of the X‐ray spectrum prior to monochromatization, allowance for the response of the double‐crystal Si monochromator used (via X‐ray dynamical theory), as well as a thorough assessment of the role of X‐ray phase‐contrast effects. Computer simulations relating to the tomography experiments also provide valuable insights into these important issues. It was found that a significant discrepancy between theory and experiment for the Cu wire could be largely resolved in terms of the effect of the point‐spread function. The findings of this study are important in respect of any attempts to extract quantitative information from X‐ray tomography data, across a wide range of disciplines, including materials and life sciences.     

Focusing femtosecond X‐ray free‐electron laser pulses by refractive lenses

The possibility of using a parabolic refractive lens with initial X‐ray free‐electron laser (XFEL) pulses, i.e. without a monochromator, is analysed. It is assumed that the measurement time is longer than 0.3 fs, which is the time duration of a coherent pulse (spike). In this case one has to calculate the propagation of a monochromatic wave and then perform an integration of the intensity over the radiation spectrum. Here a general algorithm for calculating the propagation of time‐dependent radiation in free space and through various objects is presented. Analytical formulae are derived describing the properties of the monochromatic beam focused by a system of one and two lenses. Computer simulations show that the European XFEL pulses can be focused with maximal efficiency, i.e. as for a monochromatic wave. This occurs even for nanofocusing lenses.     

A feasibility study of dynamic stress analysis inside a running internal combustion engine using synchrotron X‐ray beams

The present investigation establishes the feasibility of using synchrotron‐generated X‐ray beams for time‐resolved in situ imaging and diffraction of the interior components of an internal combustion engine during its operation. The demonstration experiment was carried out on beamline I12 (JEEP) at Diamond Light Source, UK. The external hutch of the JEEP instrument is a large‐scale engineering test bed for complex in situ processing and simulation experiments. The hutch incorporates a large capacity translation and rotation table and a selection of detectors for monochromatic and white‐beam diffraction and imaging. These capabilities were used to record X‐ray movies of a motorcycle internal combustion engine running at 1850 r.p.m. and to measure strain inside the connecting rod via stroboscopic X‐ray diffraction measurement. The high penetrating ability and high flux of the X‐ray beam at JEEP allowed the observation of inlet and outlet valve motion, as well as that of the piston, connecting rod and the timing chain within the engine. Finally, the dynamic internal strain within the moving connecting rod was evaluated with an accuracy of ～50 × 10^?6.     

Pixelated transmission‐mode diamond X‐ray detector

Fabrication and testing of a prototype transmission‐mode pixelated diamond X‐ray detector (pitch size 60–100 µm), designed to simultaneously measure the flux, position and morphology of an X‐ray beam in real time, are described. The pixel density is achieved by lithographically patterning vertical stripes on the front and horizontal stripes on the back of an electronic‐grade chemical vapor deposition single‐crystal diamond. The bias is rotated through the back horizontal stripes and the current is read out on the front vertical stripes at a rate of ～1 kHz, which leads to an image sampling rate of ～30 Hz. This novel signal readout scheme was tested at beamline X28C at the National Synchrotron Light Source (white beam, 5–15 keV) and at beamline G3 at the Cornell High Energy Synchrotron Source (monochromatic beam, 11.3 keV) with incident beam flux ranges from 1.8 × 10^?2 to 90 W mm^?2. Test results show that the novel detector provides precise beam position (positional noise within 1%) and morphology information (error within 2%), with an additional software‐controlled single channel mode providing accurate flux measurement (fluctuation within 1%).     

Utilizing broadband X‐rays in a Bragg coherent X‐ray diffraction imaging experiment

A method is presented to simplify Bragg coherent X‐ray diffraction imaging studies of complex heterogeneous crystalline materials with a two‐stage screening/imaging process that utilizes polychromatic and monochromatic coherent X‐rays and is compatible with in situ sample environments. Coherent white‐beam diffraction is used to identify an individual crystal particle or grain that displays desired properties within a larger population. A three‐dimensional reciprocal‐space map suitable for diffraction imaging is then measured for the Bragg peak of interest using a monochromatic beam energy scan that requires no sample motion, thus simplifying in situ chamber design. This approach was demonstrated with Au nanoparticles and will enable, for example, individual grains in a polycrystalline material of specific orientation to be selected, then imaged in three dimensions while under load.     

SUT‐NANOTEC‐SLRI beamline for X‐ray absorption spectroscopy

The SUT‐NANOTEC‐SLRI beamline was constructed in 2012 as the flagship of the SUT‐NANOTEC‐SLRI Joint Research Facility for Synchrotron Utilization, co‐established by Suranaree University of Technology (SUT), National Nanotechnology Center (NANOTEC) and Synchrotron Light Research Institute (SLRI). It is an intermediate‐energy X‐ray absorption spectroscopy (XAS) beamline at SLRI. The beamline delivers an unfocused monochromatic X‐ray beam of tunable photon energy (1.25–10 keV). The maximum normal incident beam size is 13 mm (width) × 1 mm (height) with a photon flux of 3 × 10⁸ to 2 × 10¹⁰ photons s^?1 (100 mA)^?1 varying across photon energies. Details of the beamline and XAS instrumentation are described. To demonstrate the beamline performance, K‐edge XANES spectra of MgO, Al₂O₃, S₈, FeS, FeSO₄, Cu, Cu₂O and CuO, and EXAFS spectra of Cu and CuO are presented.     

Measurement of the X‐ray mass attenuation coefficients of silver in the 5–20 keV range

The X‐ray mass attenuation coefficients of silver were measured in the energy range 5–20 keV with an accuracy of 0.01–0.2% on a relative scale down to 5.3 keV, and of 0.09–1.22% on an absolute scale to 5.0 keV. This analysis confirms that with careful choice of foil thickness and careful correction for systematics, especially including harmonic contents at lower energies, the X‐ray attenuation of high‐Z elements can be measured with high accuracy even at low X‐ray energies (<6 keV). This is the first high‐accuracy measurement of X‐ray mass attenuation coefficients of silver in the low energy range, indicating the possibility of obtaining high‐accuracy X‐ray absorption fine structure down to the L₁ edge (3.8 keV) of silver. Comparison of results reported here with an earlier data set optimized for higher energies confirms accuracy to within one standard error of each data set collected and analysed using the principles of the X‐ray extended‐range technique (XERT). Comparison with theory shows a slow divergence towards lower energies in this region away from absorption edges. The methodology developed can be used for the XAFS analysis of compounds and solutions to investigate structural features, bonding and coordination chemistry.     

Quick X‐ray reflectivity using monochromatic synchrotron radiation for time‐resolved applications

A new technique for the parallel collection of X‐ray reflectivity (XRR) data, compatible with monochromatic synchrotron radiation and flat substrates, is described and applied to the in situ observation of thin‐film growth. The method employs a polycapillary X‐ray optic to produce a converging fan of radiation, incident onto a sample surface, and an area detector to simultaneously collect the XRR signal over an angular range matching that of the incident fan. Factors determining the range and instrumental resolution of the technique in reciprocal space, in addition to the signal‐to‐background ratio, are described in detail. This particular implementation records ～5° in 2gθ and resolves Kiessig fringes from samples with layer thicknesses ranging from 3 to 76 nm. The value of this approach is illustrated by showing in situ XRR data obtained with 100 ms time resolution during the growth of epitaxial La_0.7Sr_0.3MnO₃ on SrTiO₃ by pulsed laser deposition at the Cornell High Energy Synchrotron Source (CHESS). Compared with prior methods for parallel XRR data collection, this is the first method that is both sample‐independent and compatible with the highly collimated, monochromatic radiation typical of third‐generation synchrotron sources. Further, this technique can be readily adapted for use with laboratory‐based sources.     

Characteristics of a tapered undulator for the X‐ray absorption fine‐structure technique at PLS‐II

An in‐vacuum undulator (IVU) with a tapered configuration was installed in the 8C nanoprobe/XAFS beamlime (BL8C) of the Pohang Light Source in Korea for hard X‐ray nanoprobe and X‐ray absorption fine‐structure (XAFS) experiments. It has been operated in planar mode for the nanoprobe experiments, while gap‐scan and tapered modes have been used alternatively for XAFS experiments. To examine the features of the BL8C IVU for XAFS experiments, spectral distributions were obtained theoretically and experimentally as functions of the gap and gap taper. Beam profiles at a cross section of the X‐ray beam were acquired using a slit to visualize the intensity distributions which depend on the gap, degree of tapering and harmonic energies. To demonstrate the effect of tapering around the lower limit of the third‐harmonic energy, V K‐edge XAFS spectra were obtained in each mode. Owing to the large X‐ray intensity variation around this energy, XAFS spectra of the planar and gap‐scan modes show considerable spectral distortions in comparison with the tapered mode. This indicates that the tapered mode, owing to the smooth X‐ray intensity profile at the expense of the highest and most stable intensity, can be an alternative for XAFS experiments where the gap‐scan mode gives a considerable intensity variation; it is also suitable for quick‐XAFS scanning.     

Upgrade of MacCHESS facility for X‐ray scattering of biological macromolecules in solution

X‐ray scattering of biological macromolecules in solution is an increasingly popular tool for structural biology and benefits greatly from modern high‐brightness synchrotron sources. The upgraded MacCHESS BioSAXS station is now located at the 49‐pole wiggler beamline G1. The 20‐fold improved flux over the previous beamline F2 provides higher sample throughput and autonomous X‐ray scattering data collection using a unique SAXS/WAXS dual detectors configuration. This setup achieves a combined q‐range from 0.007 to 0.7 Å^?1, enabling better characterization of smaller molecules, while opening opportunities for emerging wide‐angle scattering methods. In addition, a facility upgrade of the positron storage ring to continuous top‐up mode has improved beam stability and eliminated beam drift over the course of typical BioSAXS experiments. Single exposure times have been reduced to 2 s for 3.560 mg ml^?1 lysozyme with an average quality factor I/σ of 20 in the Guinier region. A novel disposable plastic sample cell design that incorporates lower background X‐ray window material provides users with a more pristine sample environment than previously available. Systematic comparisons of common X‐ray window materials bonded to the cell have also been extended to the wide‐angle regime, offering new insight into best choices for various q‐space ranges. In addition, a quantitative assessment of signal‐to‐noise levels has been performed on the station to allow users to estimate necessary exposure times for obtaining usable signals in the Guinier regime. Users also have access to a new BioSAXS sample preparation laboratory which houses essential wet‐chemistry equipment and biophysical instrumentation. User experiments at the upgraded BioSAXS station have been on‐going since commissioning of the beamline in Summer 2013. A planned upgrade of the G1 insertion device to an undulator for the Winter 2014 cycle is expected to further improve flux by an order of magnitude.     

Simple dose rate measurements for a very high synchrotron X‐ray flux

Dose measurements based on methylene blue (MB) bleaching, widely used for ultraviolet light, can also be applied to X‐rays including very high flux levels. This method has been tested by using both MB bleaching and Fricke dosimetry for a conventional monochromatic X‐ray source and then for `white‐beam' synchrotron radiation. The results show that MB bleaching dosimetry can easily measure X‐ray doses up to at least 10⁵ Gy s^?1, as long as the MB concentration is sufficiently high. This condition can be verified from the deviations from linearity of the bleaching versus exposure time.     

X‐ray position‐sensitive duo‐lateral diamond detectors at SOLEIL

The performance of a diamond X‐ray beam position monitor is reported. This detector consists of an ionization solid‐state chamber based on a thin single‐crystal chemical‐vapour‐deposition diamond with position‐sensitive resistive electrodes in a duo‐lateral configuration. The detector's linearity, homogeneity and responsivity were studied on beamlines at Synchrotron SOLEIL with various beam sizes, intensities and energies. These measurements demonstrate the large and homogeneous (absorption variation of less than 0.7% over 500 µm × 500 µm) active area of the detector, with linear responses independent of the X‐ray beam spatial distribution. Due to the excellent charge collection efficiency (approaching 100%) and intensity sensitivity (0.05%), the detector allows monitoring of the incident beam flux precisely. In addition, the in‐beam position resolution was compared with a theoretical analysis providing an estimation of the detector's beam position resolution capability depending on the experimental conditions (X‐ray flux, energy and readout acquisition time).     

High‐power‐load DCLM monochromator for a computed tomography program at BMIT at energies of 25–150 keV

The research program at the biomedical imaging facility requires a high‐flux hard‐X‐ray monochromator that can also provide a wide beam. A wide energy range is needed for standard radiography, phase‐contrast imaging, K‐edge subtraction imaging and monochromatic beam therapy modalities. The double‐crystal Laue monochromator, developed for the BioMedical Imaging and Therapy facility, is optimized for the imaging of medium‐ and large‐scale samples at high energies with the resolution reaching 4 µm. A pair of 2 mm‐thick Si(111) bent Laue‐type crystals were used in fixed‐exit beam mode with a 16 mm vertical beam offset and the first crystal water‐cooled. The monochromator operates at energies from 25 to 150 keV, and the measured size of the beam is 189 mm (H) × 8.6 mm (V) at 55 m from the source. This paper presents our approach in developing a complete focusing model of the monochromator. The model uses mechanical properties of crystals and benders to obtain a finite‐element analysis of the complete assembly. The modeling results are compared and calibrated with experimental measurements. Using the developed analysis, a rough estimate of the bending radius and virtual focus (image) position of the first crystal can be made, which is also the real source for the second crystal. On the other hand, by measuring the beam height in several points in the SOE‐1 hutch, the virtual focus of the second crystal can be estimated. The focusing model was then calibrated with measured mechanical properties, the values for the force and torque applied to the crystals were corrected, and the actual operating parameters of the monochromator for fine‐tuning were provided.     

High‐flux hard X‐ray microbeam using a single‐bounce capillary with doubly focused undulator beam

A pre‐focused X‐ray beam at 12 keV and 9 keV has been used to illuminate a single‐bounce capillary in order to generate a high‐flux X‐ray microbeam. The BioCAT undulator X‐ray beamline 18ID at the Advanced Photon Source was used to generate the pre‐focused beam containing 1.2 × 10¹³ photons s^?1 using a sagittal‐focusing double‐crystal monochromator and a bimorph mirror. The capillary entrance was aligned with the focal point of the pre‐focused beam in order to accept the full flux of the undulator beam. Two alignment configurations were tested: (i) where the center of the capillary was aligned with the pre‐focused beam (`in‐line') and (ii) where one side of the capillary was aligned with the beam (`off‐line'). The latter arrangement delivered more flux (3.3 × 10¹² photons s^?1) and smaller spot sizes (≤10 µm FWHM in both directions) for a photon flux density of 4.2 × 10¹⁰ photons s^?1µm^?2. The combination of the beamline main optics with a large‐working‐distance (approximately 24 mm) capillary used in this experiment makes it suitable for many microprobe fluorescence applications that require a micrometer‐size X‐ray beam and high flux density. These features are advantageous for biological samples, where typical metal concentrations are in the range of a few ng cm^?2. Micro‐XANES experiments are also feasible using this combined optical arrangement.     

BioCARS: a synchrotron resource for time‐resolved X‐ray science

BioCARS, a NIH‐supported national user facility for macromolecular time‐resolved X‐ray crystallography at the Advanced Photon Source (APS), has recently completed commissioning of an upgraded undulator‐based beamline optimized for single‐shot laser‐pump X‐ray‐probe measurements with time resolution as short as 100 ps. The source consists of two in‐line undulators with periods of 23 and 27 mm that together provide high‐flux pink‐beam capability at 12 keV as well as first‐harmonic coverage from 6.8 to 19 keV. A high‐heat‐load chopper reduces the average power load on downstream components, thereby preserving the surface figure of a Kirkpatrick–Baez mirror system capable of focusing the X‐ray beam to a spot size of 90 µm horizontal by 20 µm vertical. A high‐speed chopper isolates single X‐ray pulses at 1 kHz in both hybrid and 24‐bunch modes of the APS storage ring. In hybrid mode each isolated X‐ray pulse delivers up to ～4 × 10¹⁰ photons to the sample, thereby achieving a time‐averaged flux approaching that of fourth‐generation X‐FEL sources. A new high‐power picosecond laser system delivers pulses tunable over the wavelength range 450–2000 nm. These pulses are synchronized to the storage‐ring RF clock with long‐term stability better than 10 ps RMS. Monochromatic experimental capability with Biosafety Level 3 certification has been retained.