Phase Transition Dynamics in a Complex Oxide Heterostructure.

Understanding the behavior of defects in the complex oxides is key to controlling myriad ionic and electronic properties in these multifunctional materials. The observation of defect dynamics, however, requires a unique probe-one sensitive to the configuration of defects as well as its time evolution. Here, we present measurements of oxygen vacancy ordering in epitaxial thin films of SrCoO_{x} and the brownmillerite-perovskite phase transition employing x-ray photon correlation spectroscopy.

pyXPCSviewer: an open-source interactive tool for X-ray photon correlation spectroscopy visualization and analysis.

pyXPCSviewer, a Python-based graphical user interface that is deployed at beamline 8-ID-I of the Advanced Photon Source for interactive visualization of XPCS results, is introduced. pyXPCSviewer parses rich X-ray photon correlation spectroscopy (XPCS) results into independent PyQt widgets that are both interactive and easy to maintain. pyXPCSviewer is open-source and is open to customization by the XPCS community for ingestion of diversified data structures and inclusion of novel XPCS techniques, both of which are growing demands particularly with the dawn of near-diffraction-limited synchrotron sources and their dedicated XPCS beamlines.

Evolution of single gyroid photonic crystals in bird feathers.

Vivid, saturated structural colors are conspicuous and important features of many animals. A rich diversity of three-dimensional periodic photonic nanostructures is found in the chitinaceous exoskeletons of invertebrates. Three-dimensional photonic nanostructures have been described in bird feathers, but they are typically quasi-ordered.

20 µs-resolved high-throughput X-ray photon correlation spectroscopy on a 500k pixel detector enabled by data-management workflow.

The performance of the new 52 kHz frame rate Rigaku XSPA-500k detector was characterized on beamline 8-ID-I at the Advanced Photon Source at Argonne for X-ray photon correlation spectroscopy (XPCS) applications. Due to the large data flow produced by this detector (0.2 PB of data per 24 h of continuous operation), a workflow system was deployed that uses the Advanced Photon Source data-management (DM) system and high-performance software to rapidly reduce area-detector data to multi-tau and two-time correlation functions in near real time, providing human-in-the-loop feedback to experimenters.

Focusing a round coherent beam by spatial filtering the horizontal source.

This paper illustrates the use of spatial filtering with a horizontal slit near the source to enlarge the horizontal coherence in an experimental station and produce a diffraction-limited round focus at an insertion device beamline for X-ray photon correlation spectroscopy experiments. Simple expressions are provided to guide the optical layout, and wave propagation simulations confirm their applicability. The two-dimensional focusing performance of Be compound refractive lenses to produce a round diffraction-limited focus at 11 keV capable of generating a high-contrast speckle pattern of an aerogel sample is demonstrated.

Brilliant angle-independent structural colours preserved in weevil scales from the Swiss Pleistocene.

Extant weevils exhibit a remarkable colour palette that ranges from muted monochromatic tones to rainbow-like iridescence, with the most vibrant colours produced by three-dimensional photonic nanostructures housed within cuticular scales. Although the optical properties of these nanostructures are well understood, their evolutionary history is not fully resolved, in part due to a poor knowledge of their fossil record. Here, we report three-dimensional photonic nanostructures preserved in brightly coloured scales of two weevils, belonging to the genus or , from the Pleistocene (16-10 ka) of Switzerland.

Evolution of structure and dynamics of thermo-reversible nanoparticle gels-A combined XPCS and rheology study.

A combined X-ray photon correlation spectroscopy and rheology study is carried out to capture the evolution of structure, fast particle-scale dynamics, and moduli (elastic and loss) at early times of gel formation near the fluid-gel boundary of a suspension of nanoparticles. The system is comprised of moderately concentrated suspensions of octadecyl silica in decalin (ϕ = 0.2) undergoing thermoreversible gelation.

Sub-microsecond-resolved multi-speckle X-ray photon correlation spectroscopy with a pixel array detector.

Small-angle X-ray photon correlation spectroscopy (XPCS) measurements spanning delay times from 826 ns to 52.8 s were performed using a photon-counting pixel array detector with a dynamic range of 0-3 (2 bits). Fine resolution and a wide dynamic range of time scales was achieved by combining two modes of operation of the detector: (i) continuous mode, where data acquisition and data readout are performed in parallel with a frame acquisition time of 19.

Distributed X-ray photon correlation spectroscopy data reduction using Hadoop MapReduce.

Multi-speckle X-ray photon correlation spectroscopy (XPCS) is a powerful technique for characterizing the dynamic nature of complex materials over a range of time scales. XPCS has been successfully applied to study a wide range of systems. Recent developments in higher-frame-rate detectors, while aiding in the study of faster dynamical processes, creates large amounts of data that require parallel computational techniques to process in near real-time.

Stress relaxation in quasi-two-dimensional self-assembled nanoparticle monolayers.

We experimentally probed the stress relaxation of a monolayer of iron oxide nanoparticles at the water-air interface. Upon drop-casting onto a water surface, the nanoparticles self-assembled into islands of two-dimensional hexagonally close packed crystalline domains surrounded by large voids. When compressed laterally, the voids gradually disappeared as the surface pressure increased.

Hard-sphere-like dynamics in highly concentrated alpha-crystallin suspensions.

The dynamics of concentrated suspensions of the eye-lens protein alpha crystallin have been measured using x-ray photon correlation spectroscopy. Measurements were made at wave vectors corresponding to the first peak in the hard-sphere structure factor and volume fractions close to the critical volume fraction for the glass transition. Langevin dynamics simulations were also performed in parallel to the experiments.

Unraveling the Role of Order-to-Disorder Transition in Shear Thickening Suspensions.

Using high-resolution in situ small angle x-ray scattering in conjunction with oscillatory shear on highly monodisperse silica suspensions, we demonstrate that an order-to-disorder transition leads to a dynamic shear thickening in a lower stress regime than the standard steady shear thickening. We show that the order-to-disorder transition is controlled by strain, which is distinguishably different from steady shear thickening, which is a stress-related phenomenon. The appearance of this two-step shear thinning and thickening transition is also influenced by the particle size, monodispersity, and measurement conditions (i.

Dynamic Scaling of Colloidal Gel Formation at Intermediate Concentrations.

We have examined the formation and dissolution of gels composed of intermediate volume-fraction nanoparticles with temperature-dependent short-range attractions using small-angle x-ray scattering, x-ray photon correlation spectroscopy, and rheology to obtain nanoscale and macroscale sensitivity to structure and dynamics. Gel formation after temperature quenches to the vicinity of the rheologically determined gel temperature, T_{gel}, was characterized via the slowdown of dynamics and changes in microstructure observed in the intensity autocorrelation functions and structure factor, respectively, as a function of quench depth (ΔT=T_{quench}-T_{gel}), wave vector, and formation time t_{f}. We find the wave-vector-dependent dynamics, microstructure, and rheology at a particular ΔT and t_{f} map to those at other ΔTs and t_{f}s via an effective scaling temperature, T_{s}.

Thermal Fluctuations of Ferroelectric Nanodomains in a Ferroelectric-Dielectric PbTiO_{3}/SrTiO_{3} Superlattice.

Ferroelectric-dielectric superlattices consisting of alternating layers of ferroelectric PbTiO_{3} and dielectric SrTiO_{3} exhibit a disordered striped nanodomain pattern, with characteristic length scales of 6 nm for the domain periodicity and 30 nm for the in-plane coherence of the domain pattern. Spatial disorder in the domain pattern gives rise to coherent hard x-ray scattering patterns exhibiting intensity speckles. We show here using variable-temperature Bragg-geometry x-ray photon correlation spectroscopy that x-ray scattering patterns from the disordered domains exhibit a continuous temporal decorrelation due to spontaneous domain fluctuations.

Exploring the relationship between nanoscale dynamics and macroscopic rheology in natural polymer gums.

We report a study connecting the nanoscale and macroscale structure and dynamics of Acacia mearnsii gum as probed by small-angle X-ray scattering (SAXS), X-ray photon correlation spectroscopy (XPCS) and rheology. Acacia gum, in general, is a complex polysaccharide used extensively in industry. Over the analyzed concentration range (15 to 30 wt%) the A.

Submillisecond X-ray photon correlation spectroscopy from a pixel array detector with fast dual gating and no readout dead-time.

Small-angle scattering X-ray photon correlation spectroscopy (XPCS) studies were performed using a novel photon-counting pixel array detector with dual counters for each pixel. Each counter can be read out independently from the other to ensure there is no readout dead-time between the neighboring frames. A maximum frame rate of 11.

First experimental feasibility study of VIPIC: a custom-made detector for X-ray speckle measurements.

The Vertically Integrated Photon Imaging Chip (VIPIC) was custom-designed for X-ray photon correlation spectroscopy, an application in which occupancy per pixel is low but high time resolution is needed. VIPIC operates in a sparsified streaming mode in which each detected photon is immediately read out as a time- and position-stamped event. This event stream can be fed directly to an autocorrelation engine or accumulated to form a conventional image.

Pushing x-ray photon correlation spectroscopy beyond the continuous frame rate limit.

We demonstrate delayed-frame X-ray Photon Correlation Spectroscopy with 120 microsecond time resolution, limited only by sample scattering rates, with a prototype Pixel-array detector capable of taking two image frames separated by 153 ns or less. Although the overall frame rate is currently limited to about 4 frame pairs per second, we easily measured millisecond correlation functions. This technology, coupled to the use of brighter synchrotrons such as Petra III or the NSLS-II should enable X-ray Photon Correlation Spectroscopy on microsecond time scales on a wider variety of materials.

Charge-induced equilibrium dynamics and structure at the Ag(001)-electrolyte interface.

The applied potential dependent rate of atomic step motion of the Ag(001) surface in weak NaF electrolyte has been measured using a new extension of the technique of X-ray Photon Correlation Spectroscopy (XPCS). For applied potentials between hydrogen evolution and oxidation, the surface configuration completely changes on timescales of 10(2)-10(4) seconds depending upon the applied potential. These dynamics, directly measured over large areas of the sample surface simultaneously, are related to the surface energy relative to over or under potential.

Structural Diversity of Arthropod Biophotonic Nanostructures Spans Amphiphilic Phase-Space.

Many organisms, especially arthropods, produce vivid interference colors using diverse mesoscopic (100-350 nm) integumentary biophotonic nanostructures that are increasingly being investigated for technological applications. Despite a century of interest, precise structural knowledge of many biophotonic nanostructures and the mechanisms controlling their development remain tentative, when such knowledge can open novel biomimetic routes to facilely self-assemble tunable, multifunctional materials. Here, we use synchrotron small-angle X-ray scattering and electron microscopy to characterize the photonic nanostructure of 140 integumentary scales and setae from ∼127 species of terrestrial arthropods in 85 genera from 5 orders.

Hidden motion made known - rotational X-ray tracking reveals spinning colloids.

Rotational x-ray tracking (RXT) is demonstrated as a promising new tool for investigating previously unobservable motion in crystalline nanoscale colloids. Its potential utility is demonstrated by applying it to measurements of the local viscoelastic properties of a gel-colloid nanocomposite.

X-ray speckle visibility spectroscopy in the single-photon limit.

The technique of speckle visibility spectroscopy has been employed for the measurement of dynamics using coherent X-ray scattering. It is shown that the X-ray contrast within a single exposure can be related to the relaxation time of the intermediate scattering function, and this methodology is applied to the diffusion of 72 nm-radius latex spheres in glycerol. Data were collected with exposure times as short as 2 ms by employing a resonant shutter.

The dedicated high-resolution grazing-incidence X-ray scattering beamline 8-ID-E at the Advanced Photon Source.

As an increasingly important structural-characterization technique, grazing-incidence X-ray scattering (GIXS) has found wide applications for in situ and real-time studies of nanostructures and nanocomposites at surfaces and interfaces. A dedicated beamline has been designed, constructed and optimized at beamline 8-ID-E at the Advanced Photon Source for high-resolution and coherent GIXS experiments. The effectiveness and applicability of the beamline and the scattering techniques have been demonstrated by a host of experiments including reflectivity, grazing-incidence static and kinetic scattering, and coherent surface X-ray photon correlation spectroscopy.

X-ray photon correlation spectroscopy during homogenous shear flow.

We report x-ray photon correlation spectroscopy measurements of advective and diffusive dynamics in a dispersion of colloidal particles subjected to homogeneous shear flow in a rotating-disk shear cell. Intensity autocorrelation functions from scattering data collected using homodyne detection respond to the variation in velocity across the scattering volume when the scattering vector has a component parallel to the flow direction. Theoretical expressions for the impact of homogenous shear flow on the correlation function provide a quantitative prediction of the dependence of correlation functions on the scattering vector and shear rate.