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Macromolecules 55(19), 8757 - 8765 (2022). doi:10.1021/acs.macromol.2c01326, Dynamics of nanoparticles (NPs) in microscopic networks, in particular, localization and transport, play a key role in designing new functional nanocomposites and drug delivery systems. To this aim, it is crucial to understand the interplay between the network structure and dynamics on the microscopic scale which determines NP diffusion. Here, we study the localization and transport of spherical NPs in photorheological wormlike micellar nanocomposites where the mobility of the NPs is controlled by the network mesh size and the micelle length, which can be tuned by UV-illumination. The macroscopic viscoelastic properties are measured by classical rheology, while X-ray photon correlation spectroscopy and nanorheology provide information on the microscopic NP dynamics on length scales on the order of the network mesh size. On long time scales, the data reveal that transport through the network is determined by the ratio between the NP size and the network mesh size, while upon UV illumination, the NP mobility is drastically enhanced. On shorter time scales, the influence of the dynamical and structural micelle properties on the NP dynamics under confinement is explored and indicates an anomalous speed-up of the dynamics, which is discussed in the context of changes in the local structure and non-linear phenomena such as strain stiffening and hopping motion., Published by Soc., Washington, DC

Hydrated proteins undergo a transition in the deeply supercooled regime, which is attributed to rapid changes in hydration water and protein structural dynamics. Here, we investigate the nanoscale stress relaxation in hydrated lysozyme proteins stimulated and probed by X-ray Photon Correlation Spectroscopy (XPCS). This approach allows us to access the nanoscale dynamic response in the deeply supercooled regime (T = 180 K) which is typically not accessible through equilibrium methods. The relaxation time constants exhibit Arrhenius temperature dependence upon cooling with a minimum in the Kohlrausch-Williams-Watts exponent at T = 227 K. The observed minimum is attributed to an increase in dynamical heterogeneity, which coincides with enhanced fluctuations observed in the two-time correlation functions and a maximum in the dynamic susceptibility quantified by the normalised variance $\chi_T$. Our study provides new insights into X-ray stimulated stress relaxation and the underlying mechanisms behind spatio-temporal fluctuations in biological granular materials.

The journal of physical chemistry letters 12(30), 7085 - 7090 (2021). doi:10.1021/acs.jpclett.1c01940, Microscopic dynamics of complex fluids in the early stage of spinodal decomposition (SD) is strongly intertwined with the kinetics of structural evolution, which makes a quantitative characterization challenging. In this work, we use X-ray photon correlation spectroscopy to study the dynamics and kinetics of a protein solution undergoing liquid���liquid phase separation (LLPS). We demonstrate that in the early stage of SD, the kinetics relaxation is up to 40 times slower than the dynamics and thus can be decoupled. The microscopic dynamics can be well described by hyper-diffusive ballistic motions with a relaxation time exponentially growing with time in the early stage followed by a power-law increase with fluctuations. These experimental results are further supported by simulations based on the Cahn���Hilliard equation. The established framework is applicable to other condensed matter and biological systems undergoing phase transitions and may also inspire further theoretical work., Published by ACS, Washington, DC

We utilize coherent femtosecond extreme ultraviolet (EUV) pulses derived from a free electron laser (FEL) to generate transient periodic magnetization patterns with periods as short as 44 nm. Combining spatially periodic excitation with resonant probing at the dichroic M-edge of cobalt allows us to create and probe transient gratings of electronic and magnetic excitations in a CoGd alloy. In a demagnetized sample, we observe an electronic excitation with 50 fs rise time close to the FEL pulse duration and ~0.5 ps decay time within the range for the electron-phonon relaxation in metals. When the experiment is performed on a sample magnetized to saturation in an external field, we observe a magnetization grating, which appears on a sub-picosecond time scale as the sample is demagnetized at the maxima of the EUV intensity and then decays on the time scale of tens of picoseconds via thermal diffusion. The described approach opens prospects for studying dynamics of ultrafast magnetic phenomena on nanometer length scales.

Journal of applied crystallography 55(4), 751 - 757 (2022). doi:10.1107/S1600576722004435, Machine learning methods are used for an automated classification of experimental two-time X-ray photon correlation maps from an arrested liquid–liquid phase separation of a protein solution. The correlation maps are matched with correlation maps generated with Cahn–Hilliard-type simulations of liquid–liquid phase separations according to two simulation parameters and in the last step interpreted in the framework of the simulation. The matching routine employs an auto-encoder network and a differential evolution based algorithm. The method presented here is a first step towards handling large amounts of dynamic data measured at high-brilliance synchrotron and X-ray free-electron laser sources, facilitating fast comparison with phase field models of phase separation., Published by Wiley-Blackwell, [S.l.]

New journal of physics 23(9), 093041 (2021). doi:10.1088/1367-2630/ac2594, We demonstrate the successful application of x-ray speckle visibility spectroscopy (XSVS) experiments to study the dynamics of radiation sensitive, biological samples with unprecedented small x-ray doses of 45 Gy and below. Using XSVS, we track the dynamics of casein micelles in native, concentrated, and acidified solution conditions, while substantially reducing the deposited dose as compared to alternative techniques like sequential x-ray photon correlation spectroscopy. The Brownian motion in a skim milk sample yields the hydrodynamic radius of the casein micelles while deviations from Brownian motion with a characteristic q-dependent diffusion coefficient D(q) can be observed in more concentrated solution conditions. The low dose applied in our experiments allows the observation of static, frozen speckle patterns from gelled acidic milk. We show that the XSVS technique is especially suitable for tracking dynamics of radiation sensitive samples in combination with the improved coherent properties of new generation x-ray sources, emphasizing the great potential for further investigations of protein dynamics using fourth generation synchrotrons and free electron lasers., Published by IOP, [London]

Physical review letters 126(13), 138004 (2021). doi:10.1103/PhysRevLett.126.138004, While the interplay between liquid-liquid phase separation (LLPS) and glass formation in biological systems is highly relevant for their structure formation and thus function, the exact underlying mechanisms are not well known. The kinetic arrest originates from the slowdown at the molecular level, but how this propagates to the dynamics of microscopic phase domains is not clear. Since with diffusion, viscoelasticity, and hydrodynamics, distinctly different mechanisms are at play, the dynamics needs to be monitored on the relevant time and length scales and compared to theories of phase separation. Using x-ray photon correlation spectroscopy, we determine the LLPS dynamics of a model protein solution upon low temperature quenches and find distinctly different dynamical regimes. We observe that the early stage LLPS is driven by the curvature of the free energy and speeds up upon increasing quench depth. In contrast, the late stage dynamics slows down with increasing quench depth, fingerprinting a nearby glass transition. The dynamics observed shows a ballistic type of motion, implying that viscoelasticity plays an important role during LLPS. We explore possible explanations based on the Cahn-Hilliard theory with nontrivial mobility parameters and find that these can only partially explain our findings., Published by APS, College Park, Md.

Physical review / B 101(2), 020508 (2020). doi:10.1103/PhysRevB.101.020508, The coexistence of phases, characterized by different electronic degrees of freedom, commonly occurs in layered superconductors. Among them, alkaline intercalated chalcogenides are model systems showing the microscale coexistence of paramagnetic (PAR) and antiferromagnetic (AFM) phases, however, the temporal behavior of different phases is still unknown. Here, we report a visualization of the atomic motion in the granular phase of KxFe2−ySe2 using x-ray photon correlation spectroscopy. Unlike the PAR phase, the AFM texture reveals an intermittent dynamics with avalanches as in martensites. When cooled down across the superconducting transition temperature Tc, the AFM phase goes through an anomalous slowing behavior, suggesting a direct relationship between the atomic motions in the AFM phase and the superconductivity. In addition to providing compelling evidence of avalanchelike dynamics in a layered superconductor, the results provide a basis for different theoretical models to describe the quantum states in inhomogeneous solids., Published by Inst., Woodbury, NY

Physical review letters 125(5), 055701 (2020). doi:10.1103/PhysRevLett.125.055701, We present a detailed investigation of the wave-vector dependence of collective atomic motion in Au$_{49}$Cu$_{26.9}$Si$_{16.3}$Ag$_{5.5}$Pd$_{2.3}$ and Pd$_{42.5}$Cu$_{27}$Ni$_{9.5}$P$_{21}$ supercooled liquids close to the glass transition temperature. Using x-ray photon correlation spectroscopy in a previously uncovered spatial range of only a few interatomic distances, we show that the microscopic structural relaxation process mimics the structure and presents a marked slowing down at the main average interparticle distance. This behavior is accompanied by dramatic changes in the shape of the intermediate scattering functions, which suggest the presence of large dynamical heterogeneities at length scales corresponding to a few particle diameters. A ballisticlike mechanism of particle motion seems to govern the structural relaxation of the two systems in the highly viscous phase, likely associated with hopping of caged particles in agreement with theoretical studies., Published by APS, College Park, Md.

How to optimize experimental setups to make BioXPCS measurements feasible at new generation synchrotron sources., This study explores the possibility of measuring the dynamics of proteins in solution using X-ray photon correlation spectroscopy (XPCS) at nearly diffraction-limited storage rings (DLSRs). We calculate the signal-to-noise ratio (SNR) of XPCS experiments from a concentrated lysozyme solution at the length scale of the hydrodynamic radius of the protein molecule. We take into account limitations given by the critical X-ray dose and find expressions for the SNR as a function of beam size, sample-to-detector distance and photon energy. Specifically, we show that the combined increase in coherent flux and coherence lengths at the DLSR PETRA IV yields an increase in SNR of more than one order of magnitude. The resulting SNR values indicate that XPCS experiments of biological macromolecules on nanometre length scales will become feasible with the advent of a new generation of synchrotron sources. Our findings provide valuable input for the design and construction of future XPCS beamlines at DLSRs.

This paper reports on coherent scattering experiments in the low-count regime with less than one photon per pixel per acquisition on average, conducted with two detectors based on the Eiger single-photon-counting chip. The obtained photon-count distributions show systematic deviations from the expected Poisson–gamma distribution, which result in a strong overestimation of the measured speckle contrast. It is shown that these deviations originate from an artificial increase of double-photon events, which is proportional to the detected intensity and inversely proportional to the exposure time. The observed miscounting effect may have important implications for new coherent scattering experiments emerging with the advent of high-brilliance X-ray sources. Different correction schemes are discussed in order to obtain the correct photon distributions from the data. A successful correction is demonstrated with the measurement of Brownian motion from colloidal particles using X-ray speckle visibility spectroscopy.

A Correction to this paper has been published: https://doi.org/10.1038/s41467-021-21915-9

Proceedings of the National Academy of Sciences of the United States of America 115(29), E6680 - E6689 (2018). doi:10.1073/pnas.1720991115, echnologically important properties of ferroic materials are determined by their intricate response to external stimuli. This response is driven by distortions of the crystal structure and/or by domain wall motion. Experimental separation of these two mechanisms is a challenging problem which has not been solved so far. Here, we apply X-ray photon correlation spectroscopy (XPCS) to extract the contribution of domain wall dynamics to the overall response. Furthermore, we show how to distinguish the dynamics related to the passing of domain walls through the periodic (Peierls) potential of the crystal lattice and through the random potential caused by lattice defects (pinning centers). The approach involves the statistical analysis of correlations between X-ray speckle patterns produced by the interference of coherent synchrotron X-rays scattered from different nanosize volumes of the crystal and identification of Poisson-type contribution to the statistics. We find such a contribution in the thermally driven response of the monoclinic phase of a ferroelectric PbZr$_{0.55}$Ti$_{0.45}$O$_3$ crystal and calculate the number of domain wall jumps in the studied microvolume., Published by National Acad. of Sciences, Washington, DC

Physical review letters 120(16), 168001 (2018). doi:10.1103/PhysRevLett.120.168001, X-ray radiation damage provides a serious bottleneck for investigating microsecond to second dynamics on nanometer length scales employing x-ray photon correlation spectroscopy. This limitation hinders the investigation of real time dynamics in most soft matter and biological materials which can tolerate only x-ray doses of kGy and below. Here, we show that this bottleneck can be overcome by low dose x-ray speckle visibility spectroscopy. Employing x-ray doses of 22–438 kGy and analyzing the sparse speckle pattern of count rates as low as $6.7×10^{−3}$ per pixel, we follow the slow nanoscale dynamics of an ionic liquid (IL) at the glass transition. At the prepeak of nanoscale order in the IL, we observe complex dynamics upon approaching the glass transition temperature TG with a freezing in of the alpha relaxation and a multitude of millisecond local relaxations existing well below $T_G$. We identify this fast relaxation as being responsible for the increasing development of nanoscale order observed in ILs at temperatures below $T_G$., Published by APS, College Park, Md.

We study the feasibility of using small angle X-ray scattering (SAXS) as a new experimental diagnostic for intense laser-solid interactions. By using X-ray pulses from a hard X-ray free electron laser, we can simultaneously achieve nanometer and femtosecond resolution of laser-driven samples. This is an important new capability for the Helmholtz international beamline for extreme fields at the high energy density endstation currently built at the European X-ray free electron laser. We review the relevant SAXS theory and its application to transient processes in solid density plasmas and report on first experimental results that confirm the feasibility of the method. We present results of two test experiments where the first experiment employs ultra-short laser pulses for studying relativistic laser plasma interactions, and the second one focuses on shock compression studies with a nanosecond laser system.

Mixtures of different particle species are often investigated using the angular averages of the scattered X-ray intensity. The number of species is deduced by singular value decomposition methods. The full disentanglement of the data into per-species contributions requires additional knowledge about the system under investigation. We propose to exploit higher-order angular X-ray intensity correlations with a new computational protocol, which we apply to synchrotron data from two-species mixtures of two-dimensional static test nanoparticles. Without any other information besides the correlations, we demonstrate the assessment of particle species concentrations in the measured data sets, as well as the full ab initio reconstruction of both particle structures. The concept extends straightforwardly to more species and to the three-dimensional case, whereby the practical application will require the measurements to be performed at an X-ray free electron laser.

The complex physics of the interaction between short-pulse ultrahigh-intensity lasers and solids is so far difficult to access experimentally, and the development of compact laser-based next-generation secondary radiation sources, e.g., for tumor therapy, laboratory astrophysics, and fusion, is hindered by the lack of diagnostic capabilities to probe the complex electron dynamics and competing instabilities. At present, the fundamental plasma dynamics that occur at the nanometer and femtosecond scales during the laser-solid interaction can only be elucidated by simulations. Here we show experimentally that small-angle x-ray scattering of femtosecond x-ray free-electron laser pulses facilitates new capabilities for direct in situ characterization of intense short-pulse laser-plasma interactions at solid density that allows simultaneous nanometer spatial and femtosecond temporal resolution, directly verifying numerical simulations of the electron density dynamics during the short-pulse high-intensity laser irradiation of a solid density target. For laser-driven grating targets, we measure the solid density plasma expansion and observe the generation of a transient grating structure in front of the preinscribed grating, due to plasma expansion. The density maxima are interleaved, forming a double frequency grating in x-ray free-electron laser projection for a short time, which is a hitherto unknown effect. We expect that our results will pave the way for novel time-resolved studies, guiding the development of future laser-driven particle and photon sources from solid targets.

Synchrotron radiation news 26(6), 27 - 32 (2013). doi:10.1080/08940886.2013.850384, The free-electron laser (FEL) sources FLASH in Hamburg, LCLS at Stanford, and FERMI in Trieste provide XUV to soft X-ray radiation (FLASH and FERMI) or soft to hard X-ray radiation (LCLS) with unprecedented parameters in terms of ultrashort pulse length, high photon flux, and coherence. These properties make FELs ideal tools for studying ultrafast dynamics in matter on a previously unaccessible level. This paper first reviews results obtained at FEL sources during the last few years in the field of magnetism research. We start with pioneering experiments at FLASH demonstrating the feasibility of magnetic scattering at FELs [1, 2], then present pump–probe scattering experiments [3, 4] as well as the first FEL magnetic imaging experiments [5], and finally discuss a limitation of the scattering methods due to a quenching of the magnetic scattering signal by high-fluence FEL pulses [6]. All of the presented experiments exploit the X-ray magnetic circular dichroism effect [7, 8] to obtain element-specific magnetic scattering contrast, as known from synchrotron experiments [9–12]., Published by Taylor & Francis, Philadelphia, Pa.

Scientific Reports 6: Article number: 18970; published online: 06 January 2016; updated: 04 March 2016 The original version of this Article contained a typographical error in the spelling of the author Bharati Tudu, which was incorrectly given as Bahrati Tudu. This has now been corrected in the PDF and HTML versions of the Article.

We report on high pressure small angle x-ray scattering on suspensions of colloidal crystallites in water. The crystallites made out of charge-stabilized poly-acrylate particles exhibit a complex pressure dependence which is based on the specific pressure properties of the suspending medium water. The dominant effect is a compression of the crystallites caused by the compression of the water. In addition, we find indications that also the electrostatic properties of the system, i.e. the particle charge and the dissociation of ions, might play a role for the pressure dependence of the samples. The data further suggest that crystallites in a metastable state induced by shear-induced melting can relax to a similar structural state upon the application of pressure and dilution with water. X-ray cross correlation analysis of the two-dimensional scattering patterns indicates a pressure-dependent increase of the orientational order of the crystallites correlated with growth of these in the suspension. This study underlines the potential of pressure as a very relevant parameter to understand colloidal crystallite systems in aqueous suspension.

International audience; Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/ palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions. Ultrafast demagnetization is a very intriguing phenomenon. The existence and origin of this rapid loss of a thin film's magnetization on the femtosecond timescale has been controversially debated ever since its discovery in 1996 1. Recently, it has been proposed that the origin of this magnetization loss could be due to spin-dependent motion of the optically excited hot valence electrons causing a spatial redistribution of the magnetization, either to an adjacent metallic layer 2,3 or within the magnetic layer itself 4. Strong experimental evidence for this so-called superdiffusive spin transport has been found lately 5-8. However, the experiment of Eschenlohr and co-workers 8 , similar to our study reported here, has been challenged recently. Khorsand and co-workers 9 showed that the Au cap layer employed in that experiment does not yield the postulated, and for the interpretation of the data crucial, attenuation of the incident IR pump pulse. Implementing a truly IR-opaque capping layer, we evade the limitation affecting the interpretation of the results of Eschenlohr and co-workers 8. Proper characterization of the number of photons reaching the magnetic layer demonstrates that the transmitted intensity is by orders of magnitude too small to excite the ultrafast demagnet-ization process.

Hard X-ray free electron lasers allow for the first time to access dynamics of condensed matter samples ranging from femtoseconds to several hundred seconds. In particular, the exceptional large transverse coherence of the X-ray pulses and the high time-averaged flux promises to reach time and length scales that have not been accessible up to now with storage ring based sources. However, due to the fluctuations originating from the stochastic nature of the self-amplified spontaneous emission (SASE) process the application of well established techniques such as X-ray photon correlation spectroscopy (XPCS) is challenging. Here we demonstrate a single-shot based sequential XPCS study on a colloidal suspension with a relaxation time comparable to the SACLA free-electron laser pulse repetition rate. High quality correlation functions could be extracted without any indications for sample damage. This opens the way for systematic sequential XPCS experiments at FEL sources.

We present an x-ray reflectivity study of the water–propane interface. The vertical structure of the interface is analyzed and the adsorption of thin layers of propane on the water surface is observed. An increase of layer thickness with rising pressure is found. The electron density of the thin films is identical with the corresponding value of bulk liquid propane. From the adsorption isotherm we determine the Hamaker constant of the system, which shows a considerably higher value compared to calculations based on the Lifshitz theory. The surface tension of the molecularly thin layer is reduced in comparison to the bulk value. The measured surface roughness is in good agreement with a modified model based on capillary wave fluctuations of the water-propane–gas interfaces. Copyright © 2008 John Wiley & Sons, Ltd.

We report on a nano-beam small angle X-ray scattering study on densely-packed, dried binary films made out of spherical silica particles with radii of 11.2 and 19.3 nm. For these three-dimensional thin films prepared by drop casting, only a finite number of colloidal particles contributes to the scattering signal due to the small beam size of 400 × 400 nm2. By scanning the samples, the structure and composition of the silica particle films are determined spatially resolved revealing spatial heterogeneities in the films. Three different types of domains were identified: regions containing mainly large particles, regions containing mainly small particles, and regions where both particle species are mixed. Using the new angular X-ray cross-correlations analysis (XCCA) approach, spatial maps of the local type and degree of orientational order within the silica particle films are obtained. Whereas the mixed regions have dominant two-fold order, weaker four-fold and marginal six-fold order, regions made out of large particles are characterized by an overall reduced orientational order. Regions of small particles are highly ordered showing actually crystalline order. Distinct differences in the local particle order are observed by analyzing sections through the intensity and XCCA maps. The different degree of order can be understood by the different particle size polydispersities. Moreover, we show that preferential orientations of the particle domains can be studied by cross-correlation analysis yielding information on particle film formation. We find patches of preferential order with an average size of 8–10 μm. Thus, by this combined X-ray cross-correlation microscopy (XCCM) approach the structure and orientational order of films made out of nanometer sized colloids can be determined. This method will allow to reveal the local structure and order of self-assembled structures with different degree of order in general.

We report x-ray photon correlation spectroscopy experiments on the dynamics of the glass-former polypropylene glycol covering a temperature range from room temperature to the glass transition at Tg = 205 K using silica tracer particles. Three temperature regimes are identified: At high temperatures, Brownian motion of the tracer particles is observed. Near Tg, the dynamics is hyperdiffusive and ballistic. Around 1.12Tg, we observe an intermediate regime. Here the stretching exponent of the Kohlrausch-Williams-Watts function becomes q dependent. By analyzing higher-order correlations in the scattering data, we find that dynamical heterogeneities dramatically increase in this intermediate-temperature regime. This leads to two effects: increasing heterogeneous dynamics and correlated motion at temperatures close to and below 1.12Tg.

Here we propose to exploit the low energy bandwidth, small wavelength and penetration power of ultrashort pulses from XFELs for resonant Small Angle Scattering (SAXS) on plasma structures in laser excited plasmas. Small angle scattering allows to detect nanoscale density fluctuations in forward scattering direction. Typically, the SAXS signal from laser excited plasmas is expected to be dominated by the free electron distribution. We propose that the ionic scattering signal becomes visible when the X-ray energy is in resonance with an electron transition between two bound states (Resonant coherent X-ray diffraction, RCXD). In this case the scattering cross-section dramatically increases so that the signal of X-ray scattering from ions silhouettes against the free electron scattering background which allows to measure the opacity and derived quantities with high spatial and temporal resolution, being fundamentally limited only by the X-ray wavelength and timing. Deriving quantities such as ion spatial distribution, charge state distribution and plasma temperature with such high spatial and temporal resolution will make a vast number of processes in shortpulse laser-solid interaction accessible for direct experimental observation e.g. hole-boring and shock propagation, filamentation and instability dynamics, electron transport, heating and ultrafast ionization dynamics.

A new internet-based synchrotron experiment for students is presented. A polarimeter and computer software have been developed for measuring via the internet the X-ray magnetic circular dichroism of PtFe around its Pt L(II) and L(III) absorption edges. From the experiment, students can examine the X-ray magnetic circular dichroism of a thin PtFe foil utilizing circular-polarized synchrotron radiation emitted by the superconducting asymmetric wiggler at the synchrotron radiation source DELTA of the University of Dortmund.

We report the results of resonant magnetic XUV reflectivity experiments performed at the XUV free-electron laser FERMI. Circularly polarized XUV light with the photon energy tuned to the Fe M2,3 edge is used to measure resonant magnetic reflectivities and the corresponding Q-resolved asymmetry of a Permalloy/Ta/Permalloy trilayer film. The asymmetry exhibits ultrafast changes on 240 fs time scales upon pumping with ultrashort IR laser pulses. Depending on the value of the wavevector transfer Qz, we observe both decreasing and increasing values of the asymmetry parameter, which is attributed to ultrafast changes in the vertical spin and charge density profiles of the trilayer film.

Recently the analysis of scattering patterns by angular cross-correlation analysis (CCA) was introduced to reveal the orientational order in disordered samples with special focus to future applications on x-ray free-electron laser facilities. We apply this CCA approach to ultra-small-angle light-scattering data obtained from two-dimensional monolayers of microspheres. The films were studied in addition by optical microscopy. This combined approach allows to calculate the cross-correlations of the scattering patterns, characterized by the orientational correlation function Ψ(l)(q), as well as to obtain the real-space structure of the monolayers. We show that CCA is sensitive to the orientational order of monolayers formed by the microspheres which are not directly visible from the scattering patterns. By mixing microspheres of different radii the sizes of ordered monolayer domains is reduced. For these samples it is shown that Ψ(l)(q) quantitatively describes the degree of hexagonal order of the two-dimensional films. The experimental CCA results are compared with calculations based on the microscopy images. Both techniques show qualitatively similar features. Differences can be attributed to the wave-front distortion of the laser beam in the experiment. This effect is discussed by investigating the effect of different wave fronts on the cross-correlation analysis results. The so-determined characteristics of the cross-correlation analysis will be also relevant for future x-ray-based studies.

We measured the coherence properties of the free-electron laser SACLA on a single shot basis at an X-ray energy of 8 keV. By analysing small-angle X-ray scattering speckle patterns from colloidal dispersions we found a degree of transverse coherence of βt = 0.79 ± 0.09. Taking detector properties into account, we developed a simulation model in oder to determine the degree of coherence from intensity histograms. Finally we calculated a coherence time of τc = 0.1 fs and a pulse duration of 5.2 fs which corresponds with previous predictions.

The recent advent of hard x-ray free electron lasers (XFELs) opens new areas of science due to their exceptional brightness, coherence, and time structure. In principle, such sources enable studies of dynamics of condensed matter systems over times ranging from femtoseconds to seconds. However, the studies of "slow'' dynamics in polymeric materials still remain in question due to the characteristics of the XFEL beam and concerns about sample damage. Here we demonstrate the feasibility of measuring the relaxation dynamics of gold nanoparticles suspended in polymer melts using X-ray photon correlation spectroscopy (XPCS), while also monitoring eventual X-ray induced damage. In spite of inherently large pulse-to-pulse intensity and position variations of the XFEL beam, measurements can be realized at slow time scales. The X-ray induced damage and heating are less than initially expected for soft matter materials.

We measured the coherence properties of the free-electron laser SACLA on a single shot basis at an X-ray energy of 8 keV. By analysing small-angle X-ray scattering speckle patterns from colloidal dispersions we found a degree of transverse coherence of βt = 0.79 ± 0.09. Taking detector properties into account, we developed a simulation model in oder to determine the degree of coherence from intensity histograms. Finally we calculated a coherence time of τc = 0.1 fs and a pulse duration of 5.2 fs which corresponds with previous predictions.

The results of a computational X-ray cross-correlation analysis (XCCA) study on two-dimensional polygonal model structures are presented. This article shows how to detect and identify the orientational order of such systems, demonstrates how to eliminate the influence of the `computational box' on the XCCA results and develops new correlation functions that reflect the sample's orientational order only. For this purpose, the dependence of the correlation functions on the number of polygonal clusters and scattering vector magnitude q is studied for various types of polygons, including mixtures of polygons and randomly placed particles. An order parameter that describes the orientational order within the sample is defined. Finally, the influence of detector noise and nonplanar wavefronts on the XCCA data is determined, both of which appear to affect the results significantly and have thus to be considered in real experiments.

Am Meeresgrund und vereinzelt in Dauerfrostböden liegt eine schier unerschöpfliche Energiequelle verborgen: Methanhydrat — eine Einschlussverbindung aus Wasser und Methan, in der das Methangas in Eiskäfigen eingeschlossen wird. Makroskopisch nimmt Methanhydrat eine eisähnliche Gestalt an. In reiner Form ist es schneeweiß und zersetzt sich bei Raumtemperatur und Atmosphärendruck. Dabei wird Methangas frei, dessen Menge ausreicht, um eine dauerhafte Flamme bis zur vollständigen Zersetzung eines Gashydratbrockens zu erzeugen — daher rührt auch der Name „Brennendes Eis”. Die mikroskopische Struktur und Dynamik von Methanhydrat waren bislang noch weitgehend unerforscht. Neutronenstreuexperimente ergaben jetzt erste Einsichten.

International audience; The first X-ray photon correlation spectroscopy experiments using the fast single-photon-counting detector PILATUS (Paul Scherrer Institut, Switzerland) have been performed. The short readout time of this detector permits access to intensity autocorrelation functions describing dynamics in the millisecond range that are difficult to access with charge-coupled device detectors with typical readout times of several seconds. Showing no readout noise the PILATUS detector enables measurements of samples that either display fast dynamics or possess only low scattering power with an unprecedented signal-to-noise ratio.