Multi-frame x-ray radiography and image tracking for quantification of expansion in laser-driven tin ejecta microjets.

One regime of experimental particle-laden flow study involves ejecta microjets-often defined as a stream of micrometer-scale particles generated through shock interaction with a non-uniform surface and generally travel above 1 km/s. In order to capture the change in characteristics as a function of propagation time, we apply a multi-frame x-ray radiography platform to observe and track the jet transport dynamics. A synchrotron x-ray source allows us to perform quantitative analyses and comparisons between the eight images captured by the imaging system.

Investigating the electronic structure of high explosives with X-ray Raman spectroscopy.

We investigate the sensitivity and potential of a synergistic experiment-theory X-ray Raman spectroscopy (XRS) methodology on revealing and following the static and dynamic electronic structure of high explosive molecular materials. We show that advanced ab-initio theoretical calculations accounting for the core-hole effect based on the Bethe-Salpeter Equation (BSE) approximation are critical for accurately predicting the shape and the energy position of the spectral features of C and N core-level spectra. Moreover, the incident X-ray dose typical XRS experiments require can induce, in certain unstable structures, a prominent radiation damage at room temperature.

Submicrosecond Aggregation during Detonation Synthesis of Nanodiamond.

Detonation nanodiamond (DND) is known to form aggregates that significantly reduce their unique nanoscale properties and require postprocessing to separate. How and when DND aggregates is an important question that has not been answered experimentally and could provide the foundation for approaches to limit aggregation. To answer this question, time-resolved small-angle X-ray scattering was performed during the detonation of high-explosives that are expected to condense particulates in the diamond, graphite, and liquid regions of the carbon phase diagram.

Controlling interdependent meso-nanosecond dynamics and defect generation in metal 3D printing.

State-of-the-art metal 3D printers promise to revolutionize manufacturing, yet they have not reached optimal operational reliability. The challenge is to control complex laser-powder-melt pool interdependency (dependent upon each other) dynamics. We used high-fidelity simulations, coupled with synchrotron experiments, to capture fast multitransient dynamics at the meso-nanosecond scale and discovered new spatter-induced defect formation mechanisms that depend on the scan strategy and a competition between laser shadowing and expulsion.

Detonation synthesis of carbon nano-onions via liquid carbon condensation.

Transit through the carbon liquid phase has significant consequences for the subsequent formation of solid nanocarbon detonation products. We report dynamic measurements of liquid carbon condensation and solidification into nano-onions over ∽200 ns by analysis of time-resolved, small-angle X-ray scattering data acquired during detonation of a hydrogen-free explosive, DNTF (3,4-bis(3-nitrofurazan-4-yl)furoxan). Further, thermochemical modeling predicts a direct liquid to solid graphite phase transition for DNTF products ~200 ns post-detonation.

Use of small-angle X-ray scattering to resolve intracellular structure changes of cells induced by antibiotic treatment.

The application of small-angle X-ray scattering (SAXS) to whole cells is challenging owing to the variety of internal constituents. To resolve their contributions, the outer shape was captured by ultra-small-angle X-ray scattering and combined with the internal structure resolved by SAXS. Building on these data, a model for the major structural components of was developed.

Structure of Carbon Nanotube Porins in Lipid Bilayers: An in Situ Small-Angle X-ray Scattering (SAXS) Study.

Carbon nanotube porins (CNTPs), small segments of carbon nanotubes capable of forming defined pores in lipid membranes, are important future components for bionanoelectronic devices as they could provide a robust analog of biological membrane channels. In order to control the incorporation of these CNT channels into lipid bilayers, it is important to understand the structure of the CNTPs before and after insertion into the lipid bilayer as well as the impact of such insertion on the bilayer structure. Here we employed a noninvasive in situ probe, small-angle X-ray scattering, to study the integration of CNT porins into dioleoylphosphatidylcholine bilayers.

In Situ Real-Time Radiographic Study of Thin Film Formation Inside Rotating Hollow Spheres.

Hollow spheres with uniform coatings on the inner surface have applications in optical devices, time- or site-controlled drug release, heat storage devices, and target fabrication for inertial confinement fusion experiments. The fabrication of uniform coatings, which is often critical for the application performance, requires precise understanding and control over the coating process and its parameters. Here, we report on in situ real-time radiography experiments that provide critical spatiotemporal information about the distribution of fluids inside hollow spheres during uniaxial rotation.

Ordering in bio-inorganic hybrid nanomaterials probed by in situ scanning transmission X-ray microscopy.

Phospholipid bilayer coated Si nanowires are one-dimensional (1D) composites that provide versatile bio-nanoelectronic functionality via incorporation of a wide variety of biomolecules into the phospholipid matrix. The physiochemical behaviour of the phospholipid bilayer is strongly dependent on its structure and, as a consequence, substantial modelling and experimental efforts have been directed at the structural characterization of supported bilayers and unsupported phospholipid vesicles; nonetheless, the experimental studies conducted to date have exclusively involved volume-averaged techniques, which do not allow for the assignment of spatially resolved structural variations that could critically impact the performance of the 1D phospholipid-Si NW composites. In this manuscript, we use scanning transmission X-ray microscopy (STXM) to probe bond orientation and bilayer thickness as a function of position with a spatial resolution of ∼30 nm for Δ9-cis 1,2-dioleoyl-sn-glycero-3-phosphocholine layers prepared Si NWs.

Potential-induced electronic structure changes in supercapacitor electrodes observed by in operando soft X-ray spectroscopy.

The dynamic physiochemical response of a functioning graphene-based aerogel supercapacitor is monitored in operando by soft X-ray spectroscopy and interpreted through ab initio atomistic simulations. Unanticipated changes in the electronic structure of the electrode as a function of applied voltage bias indicate structural modifications across multiple length scales via independent pseudocapacitive and electric double layer charge storage channels.

Atomic layer deposition-derived ultra-low-density composite bulk materials with deterministic density and composition.

A universal approach for on-demand development of monolithic metal oxide composite bulk materials with air-like densities (<5 mg/cm(3)) is reported. The materials are fabricated by atomic layer deposition of titania (TiO2) or zinc oxide (ZnO) using the nanoscale architecture of 1 mg/cm(3) SiO2 aerogels formed by self-organization as a blueprint. This approach provides deterministic control over density and composition without affecting the nanoscale architecture of the composite material that is otherwise very difficult to achieve.

X-ray absorption spectroscopy for the structural investigation of self-assembled-monolayer-directed mineralization.

Self-assembled monolayers (SAMs) of organothiol molecules prepared on noble metal substrates are known to exert considerable influence over biomineral nucleation and growth and, as such, offer model templates for investigation of the processes of directed biomineralization. Identifying the structural evolution of SAM/crystal systems is essential for a more comprehensive understanding of the mechanisms by which organic monolayers mediate mineral growth. X-ray absorption spectroscopy (XAS) provides the attractive ability to study SAM structure at critical stages throughout the processes of crystallization in SAM/mineral systems.

Electronic structure differences between H(2)-, Fe-, Co-, and Cu-phthalocyanine highly oriented thin films observed using NEXAFS spectroscopy.

Phthalocyanines, a class of macrocyclic, square planar molecules, are extensively studied as semiconductor materials for chemical sensors, dye-sensitized solar cells, and other applications. In this study, we use angular dependent near-edge x-ray absorption fine structure (NEXAFS) spectroscopy as a quantitative probe of the orientation and electronic structure of H2-, Fe-, Co-, and Cu-phthalocyanine molecular thin films. NEXAFS measurements at both the carbon and nitrogen K-edges reveal that phthalocyanine films deposited on sapphire have upright molecular orientations, while films up to 50 nm thick deposited on gold substrates contain prostrate molecules.

A Temporal Abstraction-based Extract, Transform and Load Process for Creating Registry Databases for Research.

In the CTSA era there is great interest in aggregating and comparing populations across institutions. These sites likely represent data differently in their clinical data warehouses and other databases. Clinical data warehouses frequently are structured in a generalized way that supports many constituencies.

Synthesis and characterization of a nanocrystalline diamond aerogel.

Aerogel materials have myriad scientific and technological applications due to their large intrinsic surface areas and ultralow densities. However, creating a nanodiamond aerogel matrix has remained an outstanding and intriguing challenge. Here we report the high-pressure, high-temperature synthesis of a diamond aerogel from an amorphous carbon aerogel precursor using a laser-heated diamond anvil cell.

High Surface Area, sp(2)-Cross-Linked Three-Dimensional Graphene Monoliths.

Developing three-dimensional (3D) graphene assemblies with properties similar to those individual graphene sheets is a promising strategy for graphene-based electrodes. Typically, the synthesis of 3D graphene assemblies relies on van der Waals forces for holding the graphene sheets together, resulting in bulk properties that do not reflect those reported for individual graphene sheets. Here, we report the use of sol-gel chemistry to introduce chemical bonding between the graphene sheets and control the bulk properties of graphene-based aerogels.

Preparation of iron and gold silicide nanodomains on silicon (111) by the reaction of gold, iron-gold core-shell, and alloy nanoparticles with triethylsilane.

This study describes a strategy to use composite colloidal nanoparticles and triethylsilane as precursors to synthesize nanometer size structures on single-crystal silicon substrate. The concept is demonstrated by depositing gold, iron-gold alloy, and iron-gold core-shell nanoparticles on silicon (111). Upon heating, the nanoparticles form new crystalline phases on the Si (111) surface.

Unanticipated C=C bonds in covalent monolayers on silicon revealed by NEXAFS.

Interfaces are crucial to material properties. In the case of covalent organic monolayers on silicon, molecular structure at the interface controls the self-assembly of the monolayers, which in turn influences the optical properties and electrical transport. These properties intrinsically affect their application in biology, tribology, optics, and electronics.

Three-dimensional coherent x-ray diffraction imaging of a ceramic nanofoam: determination of structural deformation mechanisms.

Ultralow density polymers, metals, and ceramic nanofoams are valued for their high strength-to-weight ratio, high surface area, and insulating properties ascribed to their structural geometry. We obtain the labrynthine internal structure of a tantalum oxide nanofoam by x-ray diffractive imaging. Finite-element analysis from the structure reveals mechanical properties consistent with bulk samples and with a diffusion-limited cluster aggregation model, while excess mass on the nodes discounts the dangling fragments hypothesis of percolation theory.

Near-edge X-ray absorption fine structure spectroscopy of diamondoid thiol monolayers on gold.

Diamondoids, hydrocarbon molecules with cubic-diamond-cage structures, have unique properties with potential value for nanotechnology. The availability and ability to selectively functionalize this special class of nanodiamond materials opens new possibilities for surface modification, for high-efficiency field emitters in molecular electronics, as seed crystals for diamond growth, or as robust mechanical coatings. The properties of self-assembled monolayers (SAMs) of diamondoids are thus of fundamental interest for a variety of emerging applications.

Structural development of mercaptophenol self-assembled monolayers and the overlying mineral phase during templated CaCO3 crystallization from a transient amorphous film.

Formation of biomineral structures is increasingly attributed to directed growth of a mineral phase from an amorphous precursor on an organic matrix. While many in vitro studies have used calcite formation on organothiol self-assembled monolayers (SAMs) as a model system to investigate this process, they have generally focused on the stability of amorphous calcium carbonate (ACC) or maximizing control over the order of the final mineral phase. Little is known about the early stages of mineral formation, particularly the structural evolution of the SAM and mineral.

Monochromatic electron photoemission from diamondoid monolayers.

We found monochromatic electron photoemission from large-area self-assembled monolayers of a functionalized diamondoid, [121]tetramantane-6-thiol. Photoelectron spectra of the diamondoid monolayers exhibited a peak at the low-kinetic energy threshold; up to 68% of all emitted electrons were emitted within this single energy peak. The intensity of the emission peak is indicative of diamondoids being negative electron affinity materials.