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.     

Submicrometer hard X‐ray focusing using a single‐bounce ellipsoidal capillary combined with a Fresnel zone plate

A single‐bounce capillary with an ellipsoidal shape has been used for two‐step focusing in combination with a Fresnel zone plate (FZP). The FZP serves as a first microfocusing element and produces a demagnified micrometer image of the source, before the elliptical capillary makes a last final compression of the beam. With 15 keV X‐rays from the European Synchrotron Radiation Facility BM5 bending magnet, the two‐step demagnification system produced a focus of about 250 nm with a gain of more than 1000. The use of an ellipsoidal capillary as a micro‐mirror under off‐axis illumination using micro‐prefocusing optics might open up new opportunities in nanofocusing developments.     

Optical sectioning using single‐plane‐illumination Raman imaging

Confocal Raman imaging is widely used for optical sectioning of materials. However, for biological applications it often suffers from poor axial resolution, photodamage to the sample of interest, substrate interference, and long acquisition times. We have applied the principles of light sheet microscopy to Raman imaging and show for the first time that optically sectioned Raman images can be obtained in significantly lower acquisition times. Copyright © 2010 John Wiley & Sons, Ltd.     

Correlations in single‐photon experiments

Correlations of detection events in two photodetectors placed at the opposite sides of a beam splitter are studied in the frame of classical probability theory. It is assumed that there is always only one photon present in the measuring apparatus during one elementary experiment (one measurement act). Due to the conservation of energy, there is always a strict anticorrelation in one elementary experiment, because the photon cannot excite both of the detectors at the same time. It is explicitely shown in several examples that the “bunching” and “anti‐bunching” of the counts in serieses of elementary single‐photon experiments is governed by the statistical properties of grouping the sequences of the elementary measurements.     

Finite‐element modelling of multilayer X‐ray optics

Multilayer optical elements for hard X‐rays are an attractive alternative to crystals whenever high photon flux and moderate energy resolution are required. Prediction of the temperature, strain and stress distribution in the multilayer optics is essential in designing the cooling scheme and optimizing geometrical parameters for multilayer optics. The finite‐element analysis (FEA) model of the multilayer optics is a well established tool for doing so. Multilayers used in X‐ray optics typically consist of hundreds of periods of two types of materials. The thickness of one period is a few nanometers. Most multilayers are coated on silicon substrates of typical size 60 mm × 60 mm × 100–300 mm. The high aspect ratio between the size of the optics and the thickness of the multilayer (10⁷) can lead to a huge number of elements for the finite‐element model. For instance, meshing by the size of the layers will require more than 10¹⁶ elements, which is an impossible task for present‐day computers. Conversely, meshing by the size of the substrate will produce a too high element shape ratio (element geometry width/height > 10⁶), which causes low solution accuracy; and the number of elements is still very large (10⁶). In this work, by use of ANSYS layer‐functioned elements, a thermal‐structural FEA model has been implemented for multilayer X‐ray optics. The possible number of layers that can be computed by presently available computers is increased considerably.     

High‐energy X‐ray optics with silicon saw‐tooth refractive lenses

Silicon saw‐tooth refractive lenses have been in successful use for vertical focusing and collimation of high‐energy X‐rays (50–100 keV) at the 1‐ID undulator beamline of the Advanced Photon Source. In addition to presenting an effectively parabolic thickness profile, as required for aberration‐free refractive optics, these devices allow high transmission and continuous tunability in photon energy and focal length. Furthermore, the use of a single‐crystal material (i.e. Si) minimizes small‐angle scattering background. The focusing performance of such saw‐tooth lenses, used in conjunction with the 1‐ID beamline's bent double‐Laue monochromator, is presented for both short (～1:0.02) and long (～1:0.6) focal‐length geometries, giving line‐foci in the 2 µm–25 µm width range with 81 keV X‐rays. In addition, a compound focusing scheme was tested whereby the radiation intercepted by a distant short‐focal‐length lens is increased by having it receive a collimated beam from a nearer (upstream) lens. The collimation capabilities of Si saw‐tooth lenses are also exploited to deliver enhanced throughput of a subsequently placed small‐angular‐acceptance high‐energy‐resolution post‐monochromator in the 50–80 keV range. The successful use of such lenses in all these configurations establishes an important detail, that the pre‐monochromator, despite being comprised of vertically reflecting bent Laue geometry crystals, can be brilliance‐preserving to a very high degree.     

Nanocomposite‐based stretchable optics

Stretchable and conformable optical devices open up very exciting perspectives for the fabrication of systems incorporating diffracting and optical power in a single element. Supersonic cluster beam implantation of silver nanoparticles in an elastomeric substrate grooved by molding allows effective fabrication of cheap and simple stretchable optical elements able to withstand thousands of deformations and stretching cycles without any degradation of their optical properties. The nanocomposite‐based reflective optical devices were characterized both morphologically and optically showing excellent performances and stability compared to similar devices fabricated with standard techniques. The nanocomposite‐based devices can therefore be applied to arbitrary curved nonoptical grade surfaces in order to achieve optical power and to minimize aberrations like astigmatism. The high resilience of the nanocomposite material on which the devices are based allows them to be peeled and reused multiple times.     

Bias‐driven super‐insulating state in prismane single‐molecule contacts

Quantum transport in a single‐molecule contact made of a prismane cluster C₈ attached to quasi‐one‐dimensional gold (100) electrodes is calculated using the ab initio methodology based on the density‐functional theory and the nonequilibrium Green's functions formalism. Varying the junction length L we calculate the length dependence of the zero‐bias conductance G (L) and, for a set of the interelectrode distances, the current–voltage (I –V) characteristics. It is shown that the G (L) dependence is strongly nonmonotonic with a sharp dip at some value of L. With increase in L, the I –V curves change their shape from monotonic curves to curves with a negative differential resistance area and, for a larger L, the junction exhibits the super‐insulating state, i.e., within some applied bias voltage range the current through the junctions is about two orders of magnitude less than the current outside this bias range. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Development of a single‐cell X‐ray fluorescence flow cytometer

An X‐ray fluorescence flow cytometer that can determine the total metal content of single cells has been developed. Capillary action or pressure was used to load cells into hydrophilic or hydrophobic capillaries, respectively. Once loaded, the cells were transported at a fixed vertical velocity past a focused X‐ray beam. X‐ray fluorescence was then used to determine the mass of metal in each cell. By making single‐cell measurements, the population heterogeneity for metals in the µM to mM concentration range on fL sample volumes can be directly measured, a measurement that is difficult using most analytical methods. This approach has been used to determine the metal composition of 936 individual bovine red blood cells (bRBC), 31 individual 3T3 mouse fibroblasts (NIH3T3) and 18 Saccharomyces cerevisiae (yeast) cells with an average measurement frequency of ～4 cells min^?1. These data show evidence for surprisingly broad metal distributions. Details of the device design, data analysis and opportunities for further sensitivity improvement are described.     

Atomic spectroscopy and quantum optics in hollow‐core waveguides

Atomic spectroscopy is a well‐established, integral part of the physicist's toolbox with an extremely broad range of applications ranging from astronomy to single atom quantum optics. While highly desirable, miniaturization of atomic spectroscopy techniques on the chip scale was hampered by the apparent incompatibility of conventional solid‐state integrated optics and gaseous media. Here, the state of the art of atomic spectroscopy in hollow‐core optical waveguides is reviewed The two main approaches to confining light in low index atomic vapors are described: hollow‐core photonic crystal fiber (HC‐PCF) and planar antiresonant reflecting optical waveguides (ARROWs). Waveguide design, fabrication, and characterization are reviewed along with the current performance as compact atomic spectroscopy devices. The article specifically focuses on the realization of quantum interference effects in alkali atoms which may enable radically new optical devices based on low‐level nonlinear interactions on the single photon level for frequency standards and quantum communication systems.     

I19, the small‐molecule single‐crystal diffraction beamline at Diamond Light Source

The dedicated small‐molecule single‐crystal X‐ray diffraction beamline (I19) at Diamond Light Source has been operational and supporting users for over three years. I19 is a high‐flux tunable‐wavelength beamline and its key details are described in this article. Much of the work performed on the beamline involves structure determination from small and weakly diffracting crystals. Other experiments that have been supported to date include structural studies at high pressure, studies of metastable species, variable‐temperature crystallography, studies involving gas exchange in porous materials and structural characterizations that require analysis of the diffuse scattering between Bragg reflections. A range of sample environments to facilitate crystallographic studies under non‐ambient conditions are available as well as a number of options for automation. An indication of the scope of the science carried out on the beamline is provided by the range of highlights selected for this paper.     

X‐ray collimation by crystals with precise parabolic holes based on diffractive–refractive optics

Two crystals with precise parabolic holes were used to demonstrate sagittal beam collimation by means of a diffractive–refractive double‐crystal monochromator. A new approach is introduced and beam collimation is demonstrated. Two Si(333) crystals with an asymmetry angle of α = 15° were prepared and arranged in a dispersive position (+,?,?,+). Based on theoretical calculations, this double‐crystal set‐up should provide tunable beam collimation within an energy range of 6.3–18.8 keV (Θ_B = 71–18.4°). An experiment study was performed on BM05 at ESRF. Using 8.97 keV energy, the beam profile at various distances was measured. The experimental results are in good agreement with theoretical predictions. Owing to insufficient harmonic suppression, the collimated (333) beam was overlapped by horizontally diverging (444) and (555) beams.     

Refraction and ultra‐small‐angle scattering of X‐rays in a single‐crystal diamond compound refractive lens

In this work a double‐crystal setup is employed to study compound refractive lenses made of single‐crystal diamond. The point spread function of the lens is calculated taking into account the lens transmission, the wavefront aberrations, and the ultra‐small‐angle broadening of the X‐ray beam. It is shown that, similarly to the wavefront aberrations, the ultra‐small‐angle scattering effects can significantly reduce the intensity gain and increase the focal spot size. The suggested approach can be particularly useful for the characterization of refractive X‐ray lenses composed of many tens of unit lenses.     

Kinoform optics applied to X‐ray photon correlation spectroscopy

Moderate‐demagnification higher‐order silicon kinoform focusing lenses have been fabricated to facilitate small‐angle X‐ray photon correlation spectroscopy (XPCS) experiments. The geometric properties of such lenses, their focusing performance and their applicability for XPCS measurements are described. It is concluded that one‐dimensional vertical X‐ray focusing via silicon kinoform lenses significantly increases the usable coherent flux from third‐generation storage‐ring light sources for small‐angle XPCS experiments.     

Optimizing the accuracy and precision of the single‐pulse Laue technique for synchrotron photo‐crystallography

The accuracy that can be achieved in single‐pulse pump‐probe Laue experiments is discussed. It is shown that with careful tuning of the experimental conditions a reproducibility of the intensity ratios of equivalent intensities obtained in different measurements of 3–4% can be achieved. The single‐pulse experiments maximize the time resolution that can be achieved and, unlike stroboscopic techniques in which the pump‐probe cycle is rapidly repeated, minimize the temperature increase due to the laser exposure of the sample.     

Phase‐space analysis and experimental results for secondary focusing at X‐ray beamlines

Micro‐focusing optical devices at synchrotron beamlines usually have a limited acceptance, but more flux can be intercepted if such optics are used to focus secondary sources created by the primary optics. Flux throughput can be maximized by placing the secondary focusing optics close to or exactly at the secondary source position. However, standard methods of beamline optics analysis, such as the lens equation or matching the mirror surface to an ellipse, work poorly when the source‐to‐optics distance is very short. In this paper the general characteristics of the focusing of beams with Gaussian profiles by a `thin lens' are analysed under the paraxial approximation in phase space, concluding that the focusing of a beam with a short source‐to‐optics distance is distinct from imaging the source; slope errors are successfully included in all the formulas so that they can be used to calculate beamline focusing with good accuracy. A method is also introduced to use the thin‐lens result to analyse the micro‐focusing produced by an elliptically bent trapezoid‐shaped Kirkpatrick–Baez mirror. The results of this analysis are in good agreement with ray‐tracing simulations and are confirmed by the experimental results of the secondary focusing at the 18‐ID Bio‐CAT beamline (at the APS). The result of secondary focusing carried out at 18‐ID using a single‐bounce capillary can also be explained using this phase‐space analysis. A discussion of the secondary focusing results is presented at the end of this paper.     

Simulations of X‐ray diffraction of shock‐compressed single‐crystal tantalum with synchrotron undulator sources

Polychromatic synchrotron undulator X‐ray sources are useful for ultrafast single‐crystal diffraction under shock compression. Here, simulations of X‐ray diffraction of shock‐compressed single‐crystal tantalum with realistic undulator sources are reported, based on large‐scale molecular dynamics simulations. Purely elastic deformation, elastic–plastic two‐wave structure, and severe plastic deformation under different impact velocities are explored, as well as an edge release case. Transmission‐mode diffraction simulations consider crystallographic orientation, loading direction, incident beam direction, X‐ray spectrum bandwidth and realistic detector size. Diffraction patterns and reciprocal space nodes are obtained from atomic configurations for different loading (elastic and plastic) and detection conditions, and interpretation of the diffraction patterns is discussed.     

New figuring model based on surface slope profile for grazing‐incidence reflective optics

Surface slope profile is widely used in the metrology of grazing‐incidence reflective optics instead of surface height profile. Nevertheless, the theoretical and experimental model currently used in deterministic optical figuring processes is based on surface height, not on surface slope. This means that the raw slope profile data from metrology need to be converted to height profile to perform the current height‐based figuring processes. The inevitable measurement noise in the raw slope data will introduce significant cumulative error in the resultant height profiles. As a consequence, this conversion will degrade the determinism of the figuring processes, and will have an impact on the ultimate surface figuring results. To overcome this problem, an innovative figuring model is proposed, which directly uses the raw slope profile data instead of the usual height data as input for the deterministic process. In this paper, first the influence of the measurement noise on the resultant height profile is analyzed, and then a new model is presented; finally a demonstration experiment is carried out using a one‐dimensional ion beam figuring process to demonstrate the validity of our approach.     

Tracking X‐ray‐derived redox changes in crystals of a methylamine dehydrogenase/amicyanin complex using single‐crystal UV/Vis microspectrophotometry

X‐ray exposure during crystallographic data collection can result in unintended redox changes in proteins containing functionally important redox centers. In order to directly monitor X‐ray‐derived redox changes in trapped oxidative half‐reaction intermediates of Paracoccus denitrificans methylamine dehydrogenase, a commercially available single‐crystal UV/Vis microspectrophotometer was installed on‐line at the BioCARS beamline 14‐BM‐C at the Advanced Photon Source, Argonne, USA. Monitoring the redox state of the intermediates during X‐ray exposure permitted the creation of a general multi‐crystal data collection strategy to generate true structures of each redox intermediate.