Lutz Wiegart

Three-dimensional coherent X-ray diffractive imaging of whole frozen-hydrated cells

Since its first experimental demonstration in 1999, coherent diffractive imaging (CDI) has been applied to image a broad range of samples using advanced synchrotron radiation, X-ray free-electron lasers, high harmonic generation and electrons. Here, the first experimental demonstration of cryogenic CDI for quantitative three-dimensional imaging of whole frozen-hydrated cells is reported. As a proof of principle, the three-dimensional mass density of the sub-cellular organization of a Neospora caninum cell is determined based on its natural contrast.

Salt Effects in the Formation of Self-Assembled Lithocholate Helical Ribbons and Tubes

The formation of self-assembled nanotubes is usually accounted for by anisotropic elastic properties of membranelike precursors. We present experimental data as evidence of the role played by electrostatics in the formation of self-assembled tubes in alkaline aqueous suspensions of lithocholic acid (LCA). Striking salt effects are characterized by comparing the rheological, dynamical, and scattering properties of systems prepared either in stoichiometric neutralization conditions (SC) of LCA or in a large excess of sodium hydroxide (EOC, experimentally optimized conditions) and finally, in two steps: stoichiometric neutralization followed by an appropriate addition of NaCl (AISC). The SC liquid system is originally made up of loose helical ribbons (previous transmission electron microscopy data), and upon aging they exhibit both intra- and interordering processes. Initially, the helical ribbons are loose and progressively wind around a cylinder (R = 330 Å) with their edges exposed to the solvent. They can be temporarily organized in a centered rectangular two-dimensional lattice (pgg, a = 224 Å, b = 687 Å). Upon further aging, the ribbons wind into more compact helical ribbons (or tubes with helical grooves): their edges are less-exposed and their ordering vanishes. Upon addition of NaCl salt (as in the AISC systems), the specific screening of the intra-aggregate electrostatic repulsions induces the closure of the ribbons into tubes (R(ext) = 260 Å, R(int) = 245 Å as in the EOC systems). Simultaneously with the closure of the ribbons into plain tubes, a drastic enhancement of their interconnectivity through van der Waals attractions develops. Eventually, gels are obtained with networks having hexagonal bundles of tubes.

Photon statistics and speckle visibility spectroscopy with partially coherent X-rays.

A new approach is proposed for measuring structural dynamics in materials from multi-speckle scattering patterns obtained with partially coherent X-rays. Coherent X-ray scattering is already widely used at high-brightness synchrotron lightsources to measure dynamics using X-ray photon correlation spectroscopy, but in many situations this experimental approach based on recording long series of images (i.e. movies) is either not adequate or not practical. Following the development of visible-light speckle visibility spectroscopy, the dynamic information is obtained instead by analyzing the photon statistics and calculating the speckle contrast in single scattering patterns. This quantity, also referred to as the speckle visibility, is determined by the properties of the partially coherent beam and other experimental parameters, as well as the internal motions in the sample (dynamics). As a case study, Brownian dynamics in a low-density colloidal suspension is measured and an excellent agreement is found between correlation functions measured by X-ray photon correlation spectroscopy and the decay in speckle visibility with integration time obtained from the analysis presented here.

Robust X-ray angular correlations for the study of meso-structures

As self-assembling nanomaterials become more sophisticated, it is becoming increasingly important to measure the structural order of finite-sized assemblies of nano-objects. These mesoscale clusters represent an acute challenge to conventional structural probes, owing to the range of implicated size scales (10 nm to several micrometres), the weak scattering signal and the dynamic nature of meso-clusters in native solution environments. The high X-ray flux and coherence of modern synchrotrons present an opportunity to extract structural information from these challenging systems, but conventional ensemble X-ray scattering averages out crucial information about local particle configurations. Conversely, a single meso-cluster scatters too weakly to recover the full diffraction pattern. Using X-ray angular cross-correlation analysis, it is possible to combine multiple noisy measurements to obtain robust structural information. This paper explores the key theoretical limits and experimental challenges that constrain the application of these methods to probing structural order in real nanomaterials. A metric is presented to quantify the signal-to-noise ratio of angular correlations, and it is used to identify several experimental artifacts that arise. In particular, it is found that background scattering, data masking and inter-cluster interference profoundly affect the quality of correlation analyses. A robust workflow is demonstrated for mitigating these effects and extracting reliable angular correlations from realistic experimental data.

Coherent amplification of X-ray scattering from meso-structures

A new technique is presented to allow the measurement of weakly scattering samples despite a high-background environment. Coherent interference between the sample and a nanofabricated ‘amplifier’ structure generates a strong interference scattering pattern, which can be analyzed using angular correlation functions to reconstruct the sample’s symmetry.

Simulation of experiments with partially coherent x-rays using Synchrotron Radiation Workshop

High-accuracy physical optics calculation methods used in the “Synchrotron Radiation Workshop” (SRW) allow for multiple applications of this code in different areas, covering development, commissioning, diagnostics and operation of X-ray instruments at light source facilities. This presentation focuses on the application of the SRW code for the simulation of experiments at these facilities. The most complete and most detailed simulation of experiments with SRW is possible in the area of elastic coherent scattering, where the interaction of radiation with samples can be described with the same transmission-type “propagators” that are used for the simulation of fully- and partially-coherent radiation propagation through X-ray optical elements of beamlines. A complete “source-to-detector” simulation of such an experiment for a lithographic sample is described here together with comparisons of the simulated coherent scattering data with actual measurements results, obtained at the Coherent Hard X-ray (CHX) beamline of the National Synchrotron Light Source II (NSLS-II). Particular attention is paid to the analysis of visibility of speckles and intensity levels in the scattered radiation patterns at different degrees of coherence of the radiation entering the sample.

Initial performances of first undulator-based hard x-ray beamlines of NSLS-II compared to simulations

Commissioning of the first X-ray beamlines of NSLS-II included detailed measurements of spectral and spatial distributions of the radiation at different locations of the beamlines, from front-ends to sample positions. Comparison of some of these measurement results with high-accuracy calculations of synchrotron (undulator) emission and wavefront propagation through X-ray transport optics, performed using SRW code, is presented.

Software tools for X-ray photon correlation and X-ray speckle visibility spectroscopy

A set of new data analysis software tools have been developed for the study of structural dynamics of materials using coherent scattering and photon correlation techniques. The new software tools can readily process high-throughput, multidimensional data, enabling studies of slow and fast dynamics of materials using X-ray Speckle Visibility Spectroscopy and X-ray Photon Correlation Spectroscopy techniques. They support a wide range of user expertise, from novice to developer, and are available in Scikit-beam python package which is available at https://github.com/scikit-beam/scikit-beam.

New aspects of longitudinal instabilities in electron storage rings

Novel features of the longitudinal instability of a single electron bunch circulating in a low-emittance electron storage ring are discussed. Measurements and numerical simulations, performed both in time and frequency domain, show a non-monotonic increase of the electron beam energy spread as a function of single bunch current, characterized by the presence of local minima and maxima, where a local minimum of the energy spread is interpreted as a higher-order microwave instability threshold. It is also shown that thresholds related to the same zero-intensity bunch length depend linearly on the accelerating radio frequency voltage. The observed intensity-dependent features of the energy spread, confirmed by measurements with two independent diagnostics methods, i.e. horizontal beam profile measurements by a synchrotron light monitor and photon energy spectrum measurements of undulator radiation, are given a theoretical interpretation by applying a novel eigenvalue analysis based on the linearized Vlasov equation.

Main functions, recent updates, and applications of Synchrotron Radiation Workshop code

The paper presents an overview of the main functions and new application examples of the “Synchrotron Radiation Workshop” (SRW) code. SRW supports high-accuracy calculations of different types of synchrotron radiation, and simulations of propagation of fully-coherent radiation wavefronts, partially-coherent radiation from a finite-emittance electron beam of a storage ring source, and time-/frequency-dependent radiation pulses of a free-electron laser, through X-ray optical elements of a beamline. An extended library of physical-optics “propagators” for different types of reflective, refractive and diffractive X-ray optics with its typical imperfections, implemented in SRW, enable simulation of practically any X-ray beamline in a modern light source facility. The high accuracy of calculation methods used in SRW allows for multiple applications of this code, not only in the area of development of instruments and beamlines for new light source facilities, but also in areas such as electron beam diagnostics, commissioning and performance benchmarking of insertion devices and individual X-ray optical elements of beamlines. Applications of SRW in these areas, facilitating development and advanced commissioning of beamlines at the National Synchrotron Light Source II (NSLS-II), are described.