Michael Sprung

Beyond simple exponential correlation functions and equilibrium dynamics in x-ray photon correlation spectroscopy

We discuss the complex dynamics in condensed matter studied with x-ray photon correlation spectroscopy (XPCS) in which non-exponential correlation functions and dispersion relations deviating from the simple diffusion law are observed. Results are presented for two systems whose dynamics are characterized by compressed, faster-than-exponential correlation functions associated with hyper-diffusive motion. In the first case, the microscopic response of an aerogel following sectioning is investigated. In the second, the out-of-equilibrium dynamics in a dense colloidal gel recovering from shear is analyzed. In both cases, the dynamics, which can be associated with relaxation of internal stress, exhibits ageing. Included in the analyses are calculations of two-time correlation functions and the variance of the instantaneous degree of correlation, yielding the dynamical susceptibility.

Direct measurement of antiferromagnetic domain fluctuations

Measurements of magnetic noise emanating from ferromagnets owing to domain motion were first carried out nearly 100 years ago, and have underpinned much science and technology. Antiferromagnets, which carry no net external magnetic dipole moment, yet have a periodic arrangement of the electron spins extending over macroscopic distances, should also display magnetic noise. However, this must be sampled at spatial wavelengths of the order of several interatomic spacings, rather than the macroscopic scales characteristic of ferromagnets. Here we present a direct measurement of the fluctuations in the nanometre-scale superstructure of spin- and charge-density waves associated with antiferromagnetism in elemental chromium. The technique used is X-ray photon correlation spectroscopy, where coherent X-ray diffraction produces a speckle pattern that serves as a ‘fingerprint’ of a particular magnetic domain configuration. The temporal evolution of the patterns corresponds to domain walls advancing and retreating over micrometre distances. This work demonstrates a useful measurement tool for antiferromagnetic domain wall engineering, but also reveals a fundamental finding about spin dynamics in the simplest antiferromagnet: although the domain wall motion is thermally activated at temperatures above 100 K, it is not so at lower temperatures, and indeed has a rate that saturates at a finite value—consistent with quantum fluctuations—on cooling below 40 K.

Capturing the Crystalline Phase of Two-Dimensional Nanocrystal Superlattices in Action

Critical photonic, electronic, and magnetic applications of two-dimensional nanocrystal superlattices often require nanostructures in perfect single-crystal phases with long-range order and limited defects. Here we discovered a crystalline phase with quasi-long-range positional order for two-dimensional nanocrystal superlattice domains self-assembled at the liquid-air interface during droplet evaporation, using in situ time-resolved X-ray scattering along with rigorous theories on two dimensional crystal structures. Surprisingly, it was observed that drying these superlattice domains preserved only an orientational order but not a long-range positional order, also supported by quantitative analysis of transmission electron microscopy images.

Sub-10 nm beam confinement by X-ray waveguides: design, fabrication and characterization of optical properties

Optimized X-ray waveguides have been fabricated and characterized in terms of transmission, angular acceptance, farfield pattern and imaging applications. Beam confinement down to sub-10 nm in two orthogonal directions has been demonstrated, at the nano-focus endstation at P10 of PETRA III at HASYLAB/DESY.

Diamond kinoform hard X-ray refractive lenses: design, nanofabrication and testing.

Motivated by the anticipated advantageous performance of diamond kinoform refractive lenses for synchrotron X-ray radiation studies, this report focuses on progress in designing, nanofabricating and testing of their focusing performance. The method involves using lift-off and plasma etching to reproduce a planar definition of numerically determined kinoform refractive optics. Tests of the focusing action of a diamond kinoform refractive lens at the APS 8-ID-I beamline demonstrate angular control of the focal spot.

Compound focusing mirror and X-ray waveguide optics for coherent imaging and nano-diffraction

A compound optical system for coherent focusing and imaging at the nanoscale is reported, realised by high-gain fixed-curvature elliptical mirrors in combination with X-ray waveguide optics or different cleaning apertures. The key optical concepts are illustrated, as implemented at the Göttingen Instrument for Nano-Imaging with X-rays (GINIX), installed at the P10 coherence beamline of the PETRA III storage ring at DESY, Hamburg, and examples for typical applications in biological imaging are given. Characteristic beam configurations with the recently achieved values are also described, meeting the different requirements of the applications, such as spot size, coherence or bandwidth. The emphasis of this work is on the different beam shaping, filtering and characterization methods.

Low-dose three-dimensional hard x-ray imaging of bacterial cells

We have imaged the three-dimensional density distribution of unstained and unsliced, freeze-dried cells of the gram-positive bacterium Deinococcus radiodurans by tomographic x-ray propagation microscopy, i.e. projection tomography with phase contrast formation by free space propagation. The work extends previous x-ray imaging of biological cells in the simple in-line holography geometry to full three-dimensional reconstruction, based on a fast iterative phase reconstruction algorithm which circumvents the usual twin-image problem. The sample is illuminated by the highly curved wave fronts emitted from a virtual quasi-point source with 10 nm cross section, realized by two crossed x-ray waveguides. The experimental scheme allows for a particularly dose efficient determination of the 3D density distribution in the cellular structure.

Diffusive dynamics during the high-to-low density transition in amorphous ice

Significance The importance of a molecular-level understanding of the properties, structure, and dynamics of liquid water is recognized in many scientific fields. It has been debated whether the observed high- and low-density amorphous ice forms are related to two distinct liquid forms. Here, we study experimentally the structure and dynamics of high-density amorphous ice as it relaxes into the low-density form. The unique aspect of this work is the combination of two X-ray methods, where wide-angle X-ray scattering provides the evidence for the structure at the atomic level and X-ray photon-correlation spectroscopy provides insight about the motion at the nanoscale, respectively. The observed motion appears diffusive, indicating liquid-like dynamics during the relaxation from the high-to low-density form. Water exists in high- and low-density amorphous ice forms (HDA and LDA), which could correspond to the glassy states of high- (HDL) and low-density liquid (LDL) in the metastable part of the phase diagram. However, the nature of both the glass transition and the high-to-low-density transition are debated and new experimental evidence is needed. Here we combine wide-angle X-ray scattering (WAXS) with X-ray photon-correlation spectroscopy (XPCS) in the small-angle X-ray scattering (SAXS) geometry to probe both the structural and dynamical properties during the high-to-low-density transition in amorphous ice at 1 bar. By analyzing the structure factor and the radial distribution function, the coexistence of two structurally distinct domains is observed at T = 125 K. XPCS probes the dynamics in momentum space, which in the SAXS geometry reflects structural relaxation on the nanometer length scale. The dynamics of HDA are characterized by a slow component with a large time constant, arising from viscoelastic relaxation and stress release from nanometer-sized heterogeneities. Above 110 K a faster, strongly temperature-dependent component appears, with momentum transfer dependence pointing toward nanoscale diffusion. This dynamical component slows down after transition into the low-density form at 130 K, but remains diffusive. The diffusive character of both the high- and low-density forms is discussed among different interpretations and the results are most consistent with the hypothesis of a liquid–liquid transition in the ultraviscous regime.

Surface X-Ray Speckles: Coherent Surface Diffraction from Au(001)

We present coherent speckled x-ray diffraction patterns obtained from a monolayer of surface atoms. We measured both the specular anti-Bragg reflection and the off-specular hexagonal reconstruction peak for the Au(001) surface reconstruction. We observed fluctuations of the speckle patterns even when the integrated intensity appears static. By autocorrelating the speckle patterns, we were able to identify two qualitatively different surface dynamic behaviors of the hex reconstruction depending on the sample temperature.

Setup for in situ surface investigations of the liquid/glass transition with (coherent) x rays

A dedicated setup comprising an efficient cryogenic device for the in situ preparation of large surface areas of prototypical organic glass formers in a wide temperature range (170–340 K) is presented. This setup provides the necessary temperature and vibrational stability for surface x-ray and neutron scattering experiments, including the extremely sensitive technique of x-ray photon correlation spectroscopy (XPCS). XPCS is an emerging method which is made possible by the high coherent photon flux produced by third-generation synchrotrons. We demonstrate that microscopic motion at the surface can be studied in a direct way in the liquid and supercooled state using XPCS. In addition, we have used a charge-coupled-device detector to record two-dimensional images of static speckle patterns forming on surfaces in the glassy state.