G. Grübel

X-ray cross correlation analysis uncovers hidden local symmetries in disordered matter.

We explore the different local symmetries in colloidal glasses beyond the standard pair correlation analysis. Using our newly developed X-ray cross correlation analysis (XCCA) concept together with brilliant coherent X-ray sources, we have been able to access and classify the otherwise hidden local order within disorder. The emerging local symmetries are coupled to distinct momentum transfer (Q) values, which do not coincide with the maxima of the amorphous structure factor. Four-, 6-, 10- and, most prevalently, 5-fold symmetries are observed. The observation of dynamical evolution of these symmetries forms a connection to dynamical heterogeneities in glasses, which is far beyond conventional diffraction analysis. The XCCA concept opens up a fascinating view into the world of disorder and will definitely allow, with the advent of free electron X-ray lasers, an accurate and systematic experimental characterization of the structure of the liquid and glass states.

Indium-Defect Complexes in Silicon Studied by Perturbed Angular Correlation Spectroscopy

The formation of molecule-like complexes, consisting of a defect and a radioactive111In atom, is studied using the perturbedγγ angular correlation technique (PAC). The complexes are characterized by their defect specific electric field gradients which also contain information on the geometry of the formed complexes. Whereas the complex is formed with the111In atom, its electric field gradient is measured after the decay of the radioactive111In atom to111Cd. Formation and dissolution of the molecule-like complexes is pursued for a variety of different conditions, such as sample temperature, dopant concentration and position of the Fermi level. In particular, the interaction of In atoms with the following defects in Si was investigated: Intrinsic defects, created by particle irradiation; substitutional donor atoms (P, As, Sb, Bi); and interstitial impurity atoms (Li, H, and an unidentified X defect); especially, the latter ones are known to passivate acceptor atoms in Si. Methodology and specific properties of the PAC technique will be illustrated with the help of these examples.

Correlation spectroscopy with coherent X-rays

X-ray photon correlation spectroscopy (XPCS) is a novel technique for the study of slow dynamics in disordered materials. It overcomes limitations of visible light scattering techniques such as multiple scattering or limitations in Q-range by using coherent X-rays from third generation synchrotron radiation sources. Applications to the static and dynamic behavior of complex fluids and to slow dynamics in hard condensed matter systems are reviewed.

ultrafast optical demagnetization manipulates nanoscale spin structure in domain walls

During ultrafast demagnetization of a magnetically ordered solid, angular momentum has to be transferred between the spins, electrons, and phonons in the system on femto- and picosecond timescales. Although the intrinsic spin-transfer mechanisms are intensely debated, additional extrinsic mechanisms arising due to nanoscale heterogeneity have only recently entered the discussion. Here we use femtosecond X-ray pulses from a free-electron laser to study thin film samples with magnetic domain patterns. We observe an infrared-pump-induced change of the spin structure within the domain walls on the sub-picosecond timescale. This domain-topography-dependent contribution connects the intrinsic demagnetization process in each domain with spin-transport processes across the domain walls, demonstrating the importance of spin-dependent electron transport between differently magnetized regions as an ultrafast demagnetization channel. This pathway exists independent from structural inhomogeneities such as chemical interfaces, and gives rise to an ultrafast spatially varying response to optical pump pulses.

Coherent imaging of biological samples with femtosecond pulses at the free-electron laser FLASH

Coherent x-ray imaging represents a new window to imaging non- crystalline, biological specimens at unprecedented resolutions. The advent of free-electron lasers (FEL) allows extremely high flux densities to be delivered to a specimen resulting in stronger scattered signal from these samples to be measured. In the best case scenario, the diffraction pattern is measured before the sample is destroyed by these intense pulses, as the processes involved in radiation damage may be substantially slower than the pulse duration. In this case, the scattered signal can be interpreted and reconstructed to yield a faithful image of the sample at a resolution beyond the conventional radiation damage limit. We employ coherent x-ray diffraction imaging (CXDI) using the free-electron

Small-angle X-ray scattering using coherent undulator radiation at the ESRF.

A simple approach for producing a high-coherent-flux X-ray beam for small-angle-scattering studies used at the Troika beamline of the European Synchrotron Radiation Facility is reported. For such small-angle studies it is permissible to reduce the longitudinal coherence .length of the beam, thus increasing the energy bandpass and intensity of the beam, because there is only a small optical path-length difference. By using mirrors and filters to cut unwanted energies from the undulator harmonic structure, a high-flux beam of >10(9) photons s(-1) through a 5 micron-diameter pinhole at 8.2 keV with a bandpass of 1.3% can be produced. The coherent properties of this beam have been measured by analyzing a static speckle pattern from an aerogel sample imaged by a directly illuminated CCD camera. The speckle size and contrast are compared with the expected values based on a statistical analysis of the intensity distribution of speckle patterns obtained using partially coherent conditions. The expected widths of the spatial autocorrelation are found, but there is an apparent incoherent fraction of the beam which reduces the measured contrast. The method presented is to be used as a tool to optimize conditions for diffraction experiments using coherent X-rays.

Performance of a picosecond x-ray delay line unit at 8.39 keV

A prototype device capable of splitting an x-ray pulse into two adjustable fractions, delaying one of them with the aim to perform x-ray photon correlation spectroscopy and pump-probe type studies, was designed, manufactured, and tested. The device utilizes eight perfect silicon crystals in vertical 90 degrees scattering geometry. Its performance has been verified with 8.39 keV synchrotron radiation. The measured throughput of the device with a Si(333) premonochromator at 8.39 keV under ambient conditions is 0.6%. Time delays up to 2.62 ns have been achieved, detected with a time resolution of 16.7 ps.

In situ observation of nanoparticle ordering at the air-water-substrate boundary in colloidal solutions using x-ray nanobeams

The nanoscale structuring during evaporation of a droplet consisting of an aqueous colloidal solution of 2nm gold nanoparticles in water on a silicon substrate is followed in real time. The authors investigated the transfer of lateral order and vertical layering as a function of time at the three-phase contact line air-solution substrate combining a nanometer-sized x-ray beam with a grazing incidence geometry. A pronounced retardation of vertical ordering is observed with respect to lateral ordering. While individual layers are deposited during evaporation of the solvent, the growth parallel to the substrate shows a strongly nondiffusive behavior.

X‐ray Fraunhofer diffraction patterns from a thin‐film waveguide

We have observed the Fraunhofer diffraction pattern of x‐rays exiting from the end face of a SiO2/polyimide/Si thin‐film waveguide. The measured angular intensity distributions are in excellent agreement with those calculated based on the dimensions and the refractive index profile of the guide. Our measurement confirms that, at the end face of the guide, the wavefront of a single guided mode is fully coherent in the direction normal to the guiding plane. This focused and transversely coherent x‐ray beam may be used as a source for coherence‐based experiments, such as x‐ray photon correlation spectroscopy.

Development of a hard X-ray delay line for X-ray photon correlation spectroscopy and jitter-free pump–probe experiments at X-ray free-electron laser sources

A prototype device capable of splitting an X-ray pulse into two adjustable fractions, delaying one of them with the aim of performing split pulse X-ray photon correlation spectroscopy and pump–probe type studies was designed and manufactured. Time delays up to 2.95 ns have been demonstrated. The achieved contrast values of 56% indicate a feasibility of performing coherence-based experiments with the delay line.