A coded aperture microscope for X-ray fluorescence full-field imaging.

The design and construction of an instrument for full-field imaging of the X-ray fluorescence emitted by a fully illuminated sample are presented. The aim is to produce an X-ray microscope with a few micrometers spatial resolution, which does not need to scan the sample. Since the fluorescence from a spatially inhomogeneous sample may contain many fluorescence lines, the optic which will provide the magnification of the emissions must be achromatic, i.e. its optical properties must be energy-independent. The only optics which fulfill this requirement in the X-ray regime are mirrors and pinholes. The throughput of a simple pinhole is very low, so the concept of coded apertures is an attractive extension which improves the throughput by having many pinholes, and retains the achromatic property. Modified uniformly redundant arrays (MURAs) with 10 µm openings and 50% open area have been fabricated using gold in a lithographic technique, fabricated on a 1 µm-thick silicon nitride membrane. The gold is 25 µm thick, offering good contrast up to 20 keV. The silicon nitride is transparent down into the soft X-ray region. MURAs with various orders, from 19 up to 73, as well as their respective negative (a mask where open and closed positions are inversed compared with the original mask), have been made. Having both signs of mask will reduce near-field artifacts and make it possible to correct for any lack of contrast.

Multicavity x-ray Fabry-Perot resonance with ultrahigh resolution and contrast.

Realization of x-ray Fabry-Perot (FP) resonance in back-Bragg-reflection crystal cavities has been proposed and explored for many years, but to date no satisfactory performance has been achieved. Here we show that single-cavity crystal resonators intrinsically have limited finesse and efficiency. To break this limit, we demonstrate that monolithic multicavity resonators with equal-width cavities and specific plate thickness ratios can generate ultrahigh-resolution FP resonance with high efficiency, steep peak tails, and ultrahigh contrast simultaneously. The resonance mechanism is similar to that of sequentially cascaded single-cavity resonators. The ultranarrow-bandwidth FP resonance is anticipated to have various applications, including modern ultrahigh-resolution or precision x-ray monochromatization, spectroscopy, coherence purification, coherent diffraction, phase contrast imaging, etc.

A bi-prism interferometer for hard X-ray photons.

Micro-fabricated bi-prisms have been used to create an interference pattern from an incident hard X-ray beam, and the intensity of the pattern probed with fluorescence from a 30 nm-thick metal film. Maximum fringe visibility exceeded 0.9 owing to the nano-sized probe and the choice of single-crystal prism material. A full near-field analysis is necessary to describe the fringe field intensities, and the transverse coherence lengths were extracted at APS beamline 8-ID-I. It is also shown that the maximum number of fringes is dependent only on the complex refractive index of the prism material.

Simultaneous XAFS measurements of multiple samples.

A four-channel ionization chamber has been designed, constructed and tested. This ionization chamber allows X-ray absorption spectra to be collected in transmission from up to four samples simultaneously. This results in spectra that are free of systematic uncertainty in relative energy alignment introduced by scan-to-scan stability of the monochromator or of numerical uncertainty associated with a post-processing alignment algorithm, allowing, in a single shot, an absolute measure of edge shift between four samples of different valence. As four samples can be measured in parallel, the time expended over the course of an experiment to cycle the measurement environment between its rest state and the measurement condition is substantially reduced. The ionization chamber is simple in design and could be implemented at virtually any XAFS beamline with a horizontal fan of radiation such as that provided by a bend magnet or wiggler.

X-ray diffuse scattering measurements of nucleation dynamics at femtosecond resolution.

Femtosecond time-resolved small and wide angle x-ray diffuse scattering techniques are applied to investigate the ultrafast nucleation processes that occur during the ablation process in semiconducting materials. Following intense optical excitation, a transient liquid state of high compressibility characterized by large-amplitude density fluctuations is observed and the buildup of these fluctuations is measured in real time. Small-angle scattering measurements reveal snapshots of the spontaneous nucleation of nanoscale voids within a metastable liquid and support theoretical predictions of the ablation process.

Carrier-density-dependent lattice stability in InSb.

The ultrafast decay of the x-ray diffraction intensity following laser excitation of an InSb crystal has been utilized to observe carrier dependent changes in the potential energy surface. For the first time, an abrupt carrier dependent onset for potential energy surface softening and the appearance of accelerated atomic disordering for a very high average carrier density have been observed. Inertial dynamics dominate the early stages of crystal disordering for a wide range of carrier densities between the onset of crystal softening and the appearance of accelerated atomic disordering.

Ultrafast bond softening in bismuth: mapping a solid's interatomic potential with X-rays.

Intense femtosecond laser excitation can produce transient states of matter that would otherwise be inaccessible to laboratory investigation. At high excitation densities, the interatomic forces that bind solids and determine many of their properties can be substantially altered. Here, we present the detailed mapping of the carrier density-dependent interatomic potential of bismuth approaching a solid-solid phase transition. Our experiments combine stroboscopic techniques that use a high-brightness linear electron accelerator-based x-ray source with pulse-by-pulse timing reconstruction for femtosecond resolution, allowing quantitative characterization of the interatomic potential energy surface of the highly excited solid.

Observation of structural anisotropy and the onset of liquidlike motion during the nonthermal melting of InSb.

The melting dynamics of laser excited InSb have been studied with femtosecond x-ray diffraction. These measurements observe the delayed onset of diffusive atomic motion, signaling the appearance of liquidlike dynamics. They also demonstrate that the root-mean-squared displacement in the [111] direction increases faster than in the [110] direction after the first 500 fs. This structural anisotropy indicates that the initially generated fluid differs significantly from the equilibrium liquid.

Clocking femtosecond X rays.

Linear-accelerator-based sources will revolutionize ultrafast x-ray science due to their unprecedented brightness and short pulse duration. However, time-resolved studies at the resolution of the x-ray pulse duration are hampered by the inability to precisely synchronize an external laser to the accelerator. At the Sub-Picosecond Pulse Source at the Stanford Linear-Accelerator Center we solved this problem by measuring the arrival time of each high energy electron bunch with electro-optic sampling. This measurement indirectly determined the arrival time of each x-ray pulse relative to an external pump laser pulse with a time resolution of better than 60 fs rms.

Atomic-scale visualization of inertial dynamics.

The motion of atoms on interatomic potential energy surfaces is fundamental to the dynamics of liquids and solids. An accelerator-based source of femtosecond x-ray pulses allowed us to follow directly atomic displacements on an optically modified energy landscape, leading eventually to the transition from crystalline solid to disordered liquid. We show that, to first order in time, the dynamics are inertial, and we place constraints on the shape and curvature of the transition-state potential energy surface. Our measurements point toward analogies between this nonequilibrium phase transition and the short-time dynamics intrinsic to equilibrium liquids.

A lamellar model for the X-ray rocking curves of sagittally bent Laue crystals.

The use of sagittally bent asymmetric Laue crystals in horizontally focusing monochromators for high-energy synchrotron X-rays necessitates simulation of the X-ray reflectivity by such crystals. Based on the theory of the lattice distortion in the diffraction plane of sagittally bent Laue crystals, a lamellar model was developed to predict their rocking curves. The model was experimentally verified by rocking-curve measurements from various reflections on silicon crystals of four representative orientations, sagittally bent to various radii, using X-rays of 67 keV energy.

Rocking-curve width of sagittally bent Laue crystals.

The use of bent asymmetric Laue crystals to sagittally focus high-energy synchrotron X-rays calls for an understanding of the mechanisms affecting X-ray diffraction by such crystals. The rocking-curve width, a measurable quantity directly related to the distortion of the lattice planes, is the necessary first step towards such an understanding. A model is formulated for assessing the rocking-curve widths of sagittally bent Laue crystals, considering the elastic anisotropy. A method for depth-resolved measurement of the rocking curves was also developed to verify the model. The model successfully explains the wide range of rocking-curve widths of a large number of reflections from silicon crystals with two different orientations.

Synchrotron X-ray reciprocal-space mapping, topography and diffraction resolution studies of macromolecular crystal quality.

A comprehensive study of microgravity and ground-grown chicken egg-white lysozyme crystals is presented using synchrotron X-ray reciprocal-space mapping, topography techniques and diffraction resolution. Microgravity crystals displayed reduced intrinsic mosaicities on average, but no differences in terms of strain over their ground-grown counterparts. Topographic analysis revealed that in the microgravity case the majority of the crystal was contributing to the peak of the reflection at the appropriate Bragg angle. In the ground-control case only a small volume of the crystal contributed to the intensity at the diffraction peak. The techniques prove to be highly complementary, with the reciprocal-space mapping providing a quantitative measure of the crystal mosaicity and strain (or variation in lattice spacing) and the topography providing a qualitative overall assessment of the crystal in terms of its X-ray diffraction properties. Structural data collection was also carried out at the synchrotron.

Microcontroller-based servo for two-crystal X-ray monochromators.

Microcontrollers have become increasingly easy to incorporate into instruments as the architectures and support tools have developed. The PIC series is particularly easy to use, and this paper describes a controller used to stabilize the output of a two-crystal X-ray monochromator at a given offset from its peak intensity position, as such monochromators are generally used.

Transmission-type X-ray linear polarizer with perfect crystals.

Even though conventional X-ray polarizers with multiple-reflection channel-cut structures perform well, they suffer from the disadvantage that the polarized beam is non-stationary as the energy is scanned. In this paper the possibility of using a thin Bragg reflector as a polarizing filter is investigated, so that the transmitted beam (rather than the Bragg-reflected beam) is used. Consequently, the position and direction of the transmitted beam are unchanged as the energy is changed, or even when the polarization direction to be filtered out is changed. Theoretical considerations as well as experimental results on the performance characteristics of the proposed transmission-type X-ray linear polarizer are presented. A polarization ratio, defined as I(H)/I(V), higher than 10(5) was obtained.

X-ray topography of tetragonal lysozyme grown by the temperature-controlled technique.

Growth-induced defects in lysozyme crystals were observed by white-beam and monochromatic X-ray topography at the National Synchrotron Light Source (NSLS) at the Brookhaven National Laboratory (BNL). The topographic methods were non-destructive to the extent that traditional diffraction data collection could be performed to high resolution after topography. It was found that changes in growth parameters, defect concentration as detected by X-ray topography, and the diffraction quality obtainable from the crystals were all strongly correlated. In addition, crystals with fewer defects showed lower mosaicity and higher diffraction resolution as expected.

Silicon Detector System for High Rate EXAFS Applications.

A multichannel silicon pad detector for EXAFS (Extended X-ray Absorption Fine Structure) applications has been designed and built. The X-ray spectroscopic measurements demonstrate that an adequate energy resolution of 230 eV FWHM (corresponding to 27 rms electrons in silicon) can be achieved reliably at -35 °C. A resolution of 190 eV FWHM (corresponding to 22 rms electrons) has been obtained from individual pads at -35 °C. At room temperature (25 °C) an average energy resolution of 380 eV FWHM is achieved and a resolution of 350 eV FWHM (41 rms electrons) is the best performance. A simple cooling system constituted of Peltier cells is sufficient to reduce the reverse currents of the pads and their related shot noise contribution, in order to achieve resolutions better than 300 eV FWHM which is adequate for the EXAFS applications.

Two-mirror wave-front-dividing interferometer for infrared synchrotron radiation.

We describe what is to our knowledge the first instrument specifically designed for use with infrared synchrotron radiation that takes advantage of the spatial coherence of this radiation. Beam splitting is achieved by wave-front division. We show data taken with the instrument over the wavelength region from 10 to 1000 microm (1-mm wavelengths) and discuss the advantages of this instrument over a conventional one.