Hard X-ray full-field nanoimaging using a direct photon-counting detector.

Full-field X-ray nanoimaging is a widely used tool in a broad range of scientific areas. In particular, for low-absorbing biological or medical samples, phase contrast methods have to be considered. Three well established phase contrast methods at the nanoscale are transmission X-ray microscopy with Zernike phase contrast, near-field holography and near-field ptychography.

Real-time insight into nanostructure evolution during the rapid formation of ultra-thin gold layers on polymers.

Ultra-thin metal layers on polymer thin films attract tremendous research interest for advanced flexible optoelectronic applications, including organic photovoltaics, light emitting diodes and sensors. To realize the large-scale production of such metal-polymer hybrid materials, high rate sputter deposition is of particular interest. Here, we witness the birth of a metal-polymer hybrid material by quantifying in situ with unprecedented time-resolution of 0.

Following the Evolution of Morphology and Optical Properties during Printing of Thin Films for Application in Non-Fullerene Acceptor Based Organic Solar Cells.

printing gives insight into the evolution of morphology and optical properties during slot-die coating of active layers for application in organic solar cells and enables an upscaling and optimization of the thin film deposition process and the photovoltaic performance. Active layers based on the conjugated polymer donor with benzodithiophene units PBDB-T-2Cl and the non-fullerene small-molecule acceptor IT-4F are printed with a slot-die coating technique and probed with grazing incidence small-angle X-ray scattering, grazing incidence wide-angle X-ray scattering, and ultraviolet/visible light spectroscopy. The formation of the morphology is followed from the liquid state to the final dry film for different printing conditions (at 25 and 35 °C), and five regimes of film formation are determined.

Fast-current-heating devices to study in situ phase formation in metallic glasses by using high-energy synchrotron radiation.

Details of fast-resistive-heating setups, controlled heating ranging from ∼10 K s to ∼10 K s, to study in situ phase transformations (on heating and on cooling) in metallic glasses by high-energy synchrotron x-ray diffraction are discussed. Both setups were designed and custom built at the Leibniz Institute for Solid State and Materials Research Dresden (IFW Dresden) and have been implemented at the P02.1 Powder Diffraction and Total Scattering Beamline and the P21.

Crystal growth rates in supercooled atomic liquid mixtures.

Crystallization is a fundamental process in materials science, providing the primary route for the realization of a wide range of new materials. Crystallization rates are also considered to be useful probes of glass-forming ability. At the microscopic level, crystallization is described by the classical crystal nucleation and growth theories, yet in general solid formation is a far more complex process.

Structure-Function Correlations in Sputter Deposited Gold/Fluorocarbon Multilayers for Tuning Optical Response.

A new strategy to nanoengineer gold/fluorocarbon multilayer (ML) nanostructures is reported. We have investigated the morphological changes occurring at the metal-polymer interface in ML structures with varying volume fraction of gold (Au) and the kinetic growth aspect of the microscale properties of nano-sized Au in plasma polymer fluorocarbon (PPFC). Investigations were carried out at various temperatures and annealing times by means of grazing incidence small-angle and wide-angle X-ray scattering (GISAXS and GIWAXS).

New dynamic diamond anvil cells for tera-pascal per second fast compression x-ray diffraction experiments.

Fast compression experiments performed using dynamic diamond anvil cells (dDACs) employing piezoactuators offer the opportunity to study compression-rate dependent phenomena. In this paper, we describe an experimental setup which allows us to perform time-resolved x-ray diffraction during the fast compression of materials using improved dDACs. The combination of the high flux available using a 25.

Towards the geometric structure of small supported Au clusters on Si.

Ultra-small clusters containing few atoms are of high interest in both fundamental research and applications due to their specific functional, magnetic or chemical properties which depend on size and composition. The experimental results of the morphology of the size-selected clusters, consisting of few atoms can be an ideal benchmark for sophisticated theoretical models. With this motivation we have investigated the geometrical structure of mass-selected Au clusters deposited on a silicon substrate prepared by soft-landing conditions.

Parallel and Perpendicular Alignment of Anisotropic Particles in Free Liquid Microjets and Emerging Microdroplets.

Liquid microjets play a key role in fiber spinning, inkjet printing, and coating processes. In all of these applications, the liquid jets carry dispersed particles whose spatial and orientational distributions within the jet critically influence the properties of the fabricated structures. Despite its importance, there is currently no knowledge about the orientational distribution of particles within microjets and droplets.

Transmission zone plates as analyzers for efficient parallel 2D RIXS-mapping.

We have implemented and successfully tested an off-axis transmission Fresnel zone plate as spectral analyzer for resonant inelastic X-ray scattering (RIXS). The imaging capabilities of zone plates allow for advanced two-dimensional (2D) mapping applications. By varying the photon energy along a line focus on the sample, we were able to simultaneously record the emission spectra over a range of excitation energies.

Direct Observation of Melting in Shock-Compressed Bismuth With Femtosecond X-ray Diffraction.

The melting of bismuth in response to shock compression has been studied using in situ femtosecond x-ray diffraction at an x-ray free electron laser. Both solid-solid and solid-liquid phase transitions are documented using changes in discrete diffraction peaks and the emergence of broad, liquid scattering upon release from shock pressures up to 14 GPa. The transformation from the solid state to the liquid is found to occur in less than 3 ns, very much faster than previously believed.

The Extreme Conditions Beamline P02.2 and the Extreme Conditions Science Infrastructure at PETRA III.

A detailed description is presented of the Extreme Conditions Beamline P02.2 for micro X-ray diffraction studies of matter at simultaneous high pressure and high/low temperatures at PETRA III, in Hamburg, Germany. This includes performance of the X-ray optics and instrumental resolution as well as an overview of the different sample environments available for high-pressure studies in the diamond anvil cell.

Real-Time Monitoring of Morphology and Optical Properties during Sputter Deposition for Tailoring Metal-Polymer Interfaces.

The reproducible low-cost fabrication of functional metal-polymer nanocomposites with tailored optoelectronic properties for advanced applications remains a major challenge in applied nanotechnology. To obtain full control over the nanostructural evolution at the metal-polymer interface and its impact on optoelectronic properties, we employed combined in situ time-resolved microfocus grazing incidence small angle X-ray scattering (μGISAXS) with in situ UV/vis specular reflectance spectroscopy (SRS) during sputter deposition of gold on thin polystyrene films. On the basis of the temporal evolution of the key scattering features in the real-time μGISAXS experiment, we directly observed four different growth regimes: nucleation, isolated island growth, growth of larger aggregates via partial coalescence, and continuous layer growth.

Size limit on the formation of periodic mesoporous organosilicas (PMOs).

The decrease of the lattice size of periodic mesoporous organosilicas (PMOs) is one important goal in obtaining a microporous material for storage or adsorption of small molecules. To determine the influence of different synthesis parameters in the lattice size, here we performed in situ small-angle X-ray diffraction studies and show that a variation of the surfactant's headgroup size is not directly followed by the lattice parameter of the resulting structure. We show that in the surfactant series of penta-, hexa-, hepta-, octa-, nona-, and decaethylene glycol monododecyl ether (C12(EO)n, n = 5, 6, 7, 8, 9, 10) the lattice size decreases between n = 5 and n = 8 and then increases, while the ordering of the materials is always cubic (space group Fd3m).

Angular momentum sensitive two-center interference.

In quantum mechanics the Young-type double-slit experiment can be performed with electrons either traveling through a double slit or being coherently emitted from two inversion symmetric molecular sites. In the latter one the valence photoionization cross sections of homonuclear diatomic molecules were predicted to oscillate over kinetic energy almost 50 years ago. Beyond the direct proof of the oscillatory behavior of these photoionization cross sections σ, we show that the angular distribution of the emitted electrons reveals hitherto unexplored information on the relative phase shift between the corresponding partial waves through two-center interference patterns.

Single-crystal diffraction at the Extreme Conditions beamline P02.2: procedure for collecting and analyzing high-pressure single-crystal data.

Fast detectors employed at third-generation synchrotrons have reduced collection times significantly and require the optimization of commercial as well as customized software packages for data reduction and analysis. In this paper a procedure to collect, process and analyze single-crystal data sets collected at high pressure at the Extreme Conditions beamline (P02.2) at PETRA III, DESY, is presented.

Aluminum-1,4-cyclohexanedicarboxylates: high-throughput and temperature-dependent in situ EDXRD studies.

The system AlCl3·6H2O/cis-H2CDC/trans-H2CDC/solvent was systematically investigated with high-throughput methods to study the influence of the two 1,4-cyclohexanedicarboxylate isomers (cis- and trans-H2CDC) as flexible aliphatic linker molecules on the formation of new crystalline compounds. Using the cis-isomer, the layered inorganic-organic hybrid compound [Al(OH)(cis-CDC)] (1) is formed. The use of trans-H2CDC leads to the microporous MOF [Al(OH)(trans-CDC)]·H2O (2) denoted CAU-13.

High-throughput microwave-assisted discovery of new metal phosphonates.

A systematic study was carried out to investigate the influence of linker geometry, metal ionic radius as well as the nature of the counter ions on the structure formation of metal tetraphosphonates. Two tetraphosphonic acids p- and m-(H2O3PCH2)2N-CH2-C6H4-CH2-N(CH2PO3H2)2, six metal ions (Ca(2+), Mn(2+), Co(2+), Ni(2+), Zn(2+), and Cd(2+)) and two different counter ions (Cl(-) and NO3(-)) were employed using high throughput methods. Microwave (MW)-assisted heating led to the discovery of ten new metal-phosphonates which crystallize in three different crystal structures.

From atoms to layers: in situ gold cluster growth kinetics during sputter deposition.

The adjustment of size-dependent catalytic, electrical and optical properties of gold cluster assemblies is a very significant issue in modern applied nanotechnology. We present a real-time investigation of the growth kinetics of gold nanostructures from small nuclei to a complete gold layer during magnetron sputter deposition with high time resolution by means of in situ microbeam grazing incidence small-angle X-ray scattering (μGISAXS). We specify the four-stage growth including their thresholds with sub-monolayer resolution and identify phase transitions monitored in Yoneda intensity as a material-specific characteristic.

Copper phosphonatoethanesulfonates: temperature dependent in situ energy dispersive X-ray diffraction study and influence of the pH on the crystal structures.

The system Cu(2+)/H2O3P-C2H4-SO3H/NaOH was investigated using in situ energy dispersive X-ray diffraction (EDXRD) to study the formation and temperature induced phase transformation of previously described copper phosphonosulfonates. Thus, the formation of [Cu2(O3P-C2H4-SO3)(OH)(H2O)]·3H2O (4) at 90 °C is shown to proceed via a previously unknown intermediate [Cu2(O3P-C2H4-SO3)(OH)(H2O)]·4H2O (6), which could be structurally characterized from high resolution powder diffraction data. Increase of the reaction temperature to 150 °C led to a rapid phase transformation to [Cu2(O3P-C2H4-SO3)(OH)(H2O)]·H2O (1), which was also studied by in situ EDXRD.

P03, the microfocus and nanofocus X-ray scattering (MiNaXS) beamline of the PETRA III storage ring: the microfocus endstation.

The P03 beamline, also called the microfocus and nanofocus X-ray scattering (MiNaXS) beamline, exploits the excellent photon beam properties of the low-emittance source PETRA III to provide a microfocused/nanofocused beam with ultra-high intensity for time-resolved X-ray scattering experiments. The beamline has been designed to perform X-ray scattering in both transmission and reflection geometries. The microfocus endstation started user operation in May 2011.

Two- and Three-Dimensional Network of Nanoparticles via Polymer-Mediated Self-Assembly.

We show a route to produce a two- and three-dimensional network of nanoparticles via polymer-mediated self-assembly. A negatively charged polymer, CO-functionalized poly (-phenyleneethylene) (PPE-CO), is used to build this network of iron-platinum (Fe-Pt) nanoparticles. The nanoparticles arrange locally in hexagonal and cubic lattice type network structures.

In situ observation of cluster formation during nanoparticle solution casting on a colloidal film.

We present a real-time study of the nanostructuring and cluster formation of gold nanoparticles deposited in aqueous solution on top of a pre-structured polystyrene colloidal thin film. Cluster formation takes place at different length scales, from the agglomerations of the gold nanoparticles to domains of polystyrene colloids. By combining in situ imaging ellipsometry and microbeam grazing incidence small-angle x-ray scattering, we are able to identify different stages of nanocomposite formation, namely diffusion, roughness increase, layer build-up and compaction.

Time-resolved ultrathin cobalt film growth on a colloidal polymer template.

Cobalt (Co) sputter deposition onto a colloidal polymer template is investigated using grazing incidence small-angle X-ray scattering (GISAXS), scanning electron microscopy (SEM), and atomic force microscopy (AFM). SEM and AFM data picture the sample topography, GISAXS the surface and near-surface film structure. A two-phase model is proposed to describe the time evolution of the Co growth.

Systematic and in situ energy dispersive X-ray diffraction investigations on the formation of lanthanide phosphonatobutanesulfonates: Ln(O(3)P-C(4)H(8)-SO(3))(H(2)O) (Ln = La-Gd).

Using the flexible linker H(2)O(3)P-C(4)H(8)-SO(3)H (H(3)L) and rare earth ions Ln(3+) (Ln = La, Ce, Pr, Nd, Sm, Eu, Gd) we were able to synthesize the new isostructural inorganic organic hybrid compounds Ln(O(3)P-C(4)H(8)-SO(3))(H(2)O). High-throughput experiments were employed to study the influence of the molar ratios Ln:H(3)L and pH on the product formation. The crystal structure of the compounds Sm(O(3)P-C(4)H(8)-SO(3))(H(2)O) (1) and Pr(O(3)P-C(4)H(8)-SO(3))(H(2)O) (2) were determined by single crystal diffraction.