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Register a new userSupplemental Material for High Contrast X-ray Speckle from Atomic-Scale Order in Liquids and Glasses
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Added by
Stephan Hruszkewycz
Publication date
2012
fields
Physics
and research's language is
English
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This supplemental material gives additional detail on Experimental Methods and Hard X-ray FEL Source Characteristics, Calculation of Maximum Speckle Contrast, Extracting Contrast of Weak Speckle Patterns, Estimated Temperature Increase from X-ray Absorption, Split-Pulse XPCS Feasibility, and Sample Disturbance During Single Pulses.
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The availability of ultrafast pulses of coherent hard x-rays from the Linac Coherent Light Source opens new opportunities for studies of atomic-scale dynamics in amorphous materials. Here we show that single ultrafast coherent x-ray pulses can be used to observe the speckle contrast in the high-angle diffraction from liquid Ga and glassy Ni2Pd2P and B2O3. We determine the thresholds above which the x-ray pulses disturb the atomic arrangements. Furthermore, high contrast speckle is observed in scattering patterns from the glasses integrated over many pulses, demonstrating that the source and optics are sufficiently stable for x-ray photon correlation spectroscopy studies of dynamics over a wide range of time scales.
Structure factors for Cax/2AlxSi1-xO2 glasses (x=0,0.25,0.5,0.67) extended to a wave vector of magnitude Q= 40 1/A have been obtained by high-energy x-ray diffraction. For the first time, it is possible to resolve the contributions of Si-O, Al-O and Ca-O coordination polyhedra to the experimental atomic pair distribution functions (PDF). It has been found that both Si and Al are four-fold coordinated and so participate in a continuous tetrahedral network at low values of x. The number of network breaking defects in the form of non-bridging oxygens (NBOs) increases slowly with x until x=0.5 (NBOs ~ 10% at x=0.5). By x=0.67 the network breaking defects become significant as evidenced by the significant drop in the average coordination number of Si. By contrast, Al-O tetrahedra remain free of NBOs and fully integrated in the Al/Si-O network for all values of x. Calcium maintains a rather uniform coordination sphere of approximately 5 oxygen atoms for all values of x. The results suggest that not only Si/Al-O tetrahedra but Ca-O polyhedra, too, play a role in determining the glassy structure.
Hybrid glasses connect emerging fields of metal-organic frameworks (MOFs) with the glass-formation, amorphization, and melting processes of these structurally diverse and chemically versatile systems. Most zeolites, including MOFs, amorphize around the glass transition, devitrifying and then melting at much higher temperatures. The relationship between the two processes has so far not been investigated. Herein we show how heating first results in a low density perfect glass, following an order-order transition, leading to a super-strong liquid of low fragility that dynamically controls MOF collapse. A subsequent order-disorder transition creates a high density liquid of greater fragility. After crystallization and melting, subsequent cooling results in a stable glass virtually identical to the high density phase. Furthermore, the wide-ranging melting temperatures of different MOFs suggest these can be differentiated by topology. Our research provides new insight into the stability and functionality of these novel ductile crystalline materials, including the possibility of melt-casting MOFs.
Nowadays powerful X-ray sources like synchrotrons and free-electron lasers are considered as ultimate tools for probing microscopic properties in materials. However, the correct interpretation of such experiments requires a good understanding on how the beam affects the properties of the sample, knowledge that is currently lacking for intense X-rays. Here we use X-ray photon correlation spectroscopy to probe static and dynamic properties of oxide and metallic glasses. We find that although the structure does not depend on the flux, strong fluxes do induce a non-trivial microscopic motion in oxide glasses, whereas no such dependence is found for metallic glasses. These results show that high fluxes can alter dynamical properties in hard materials, an effect that needs to be considered in the analysis of X-ray data but which also gives novel possibilities to study materials properties since the beam can not only be used to probe the dynamics but also to pump it.
Photometric and astrometric monitoring of directly imaged exoplanets will deliver unique insights into their rotational periods, the distribution of cloud structures, weather, and orbital parameters. As the host star is occulted by the coronagraph, a speckle grid (SG) is introduced to serve as astrometric and photometric reference. Speckle grids are implemented as diffractive pupil-plane optics that generate artificial speckles at known location and brightness. Their performance is limited by the underlying speckle halo caused by evolving uncorrected wavefront errors. The speckle halo will interfere with the coherent SGs, affecting their photometric and astrometric precision. Our aim is to show that by imposing opposite amplitude or phase modulation on the opposite polarization states, a SG can be instantaneously incoherent with the underlying halo, greatly increasing the precision. We refer to these as vector speckle grids (VSGs). We derive analytically the mechanism by which the incoherency arises and explore the performance gain in idealised simulations under various atmospheric conditions. We show that the VSG is completely incoherent for unpolarized light and that the fundamental limiting factor is the cross-talk between the speckles in the grid. In simulation, we find that for short-exposure images the VSG reaches a $sim$0.3-0.8% photometric error and $sim$$3-10cdot10^{-3}$ $lambda/D$ astrometric error, which is a performance increase of a factor $sim$20 and $sim$5, respectively. Furthermore, we outline how VSGs could be implemented using liquid-crystal technology to impose the geometric phase on the circular polarization states. The VSG is a promising new method for generating a photometric and astrometric reference SG that has a greatly increased astrometric and photometric precision.
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