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.

Hyperuniformity in amorphous silicon based on the measurement of the infinite-wavelength limit of the structure factor.

We report the results of highly sensitive transmission X-ray scattering measurements performed at the Advanced Photon Source, Argonne National Laboratory, on nearly fully dense high-purity amorphous-silicon (a-Si) samples for the purpose of determining their degree of hyperuniformity. A perfectly hyperuniform structure has complete suppression of infinite-wavelength density fluctuations, or, equivalently, the structure factor S(q→0) = 0; the smaller the value of S(0), the higher the degree of hyperuniformity. Annealing was observed to increase the degree of hyperuniformity in a-Si where we found S(0) = 0.0075 (±0.0005), which is significantly below the computationally determined lower bound recently suggested by de Graff and Thorpe [de Graff AMR, Thorpe MF (2010) Acta Crystallogr A 66(Pt 1):22-31] based on studies of continuous random network models, but consistent with the recently proposed nearly hyperuniform network picture of a-Si. Increasing hyperuniformity is correlated with narrowing of the first diffraction peak and extension of the range of oscillations in the pair distribution function.

Highly ordered noncrystalline metallic phase.

We report the characterization of a unique metallic glass that, during rapid cooling of an Al-Fe-Si melt, forms by nucleation, followed by growth normal to a moving interface between the solid and melt with partitioning of the chemical elements. We determine experimentally that this is not a polycrystalline composite with nanometer-sized grains, and conclude that this may be a new kind of structure: an atomically ordered, isotropic, noncrystalline solid, possessing no long-range translational symmetry.

Structure and dynamics studies of concentrated micrometer-sized colloidal suspensions.

We present an experimental study of the structural and dynamical properties of concentrated suspensions of different sized polystyrene microspheres dispersed in glycerol for volume fraction concentrations between 10% and 20%. The static structure, probed with ultrasmall-angle X-ray scattering, shows a behavior very similar to that of hard spheres. The equilibrium dynamics is probed with ultrasmall-angle X-ray scattering-X-ray photon correlation spectroscopy, a new technique that overcomes the limits of visible light-scattering techniques imposed by multiple scattering and is suitable for studies of optically opaque materials containing micrometer-sized structures. We found that the intensity autocorrelation functions are better described by a stretched exponential function and microspheres in a concentrated suspension move collectively. We also found that the inverse of the effective diffusion coefficients displays a peak with respect to the scattering vector that resembles the peaks in the static structure factors, which indicates that a long-lived, low free-energy state exists. The relaxation time is approximately inversely related to scattering vector, a behavior consistent with models that describe the dynamics in terms of random, local structural arrangements in disordered media.

Quantitative measurement of nanoparticle halo formation around colloidal microspheres in binary mixtures.

A new colloidal stabilization mechanism, known as nanoparticle "haloing" (Tohver, V.; Smay, J. E.; Braem, A.; Braun, P. V.; Lewis, J. A. Proc. Natl. Acad. Sci. U.S.A. 2001, 98, (16), 8950-8954), has been predicted theoretically and inferred experimentally in microsphere-nanoparticle mixtures that possess high charge and size asymmetry. The term "halo" implies the existence of a nonzero separation distance between the highly charged nanoparticles and the negligibly charged microspheres that they surround. By means of ultrasmall-angle X-ray scattering, we have quantified the microsphere-nanoparticle separation distance as well as the number of nanoparticles and their lateral separation distance within the self-organized halos that form in these binary mixtures.