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Journal of synchrotron radiation 1(1), 242 - 250 (2023). doi:10.1107/S1600577522010347, The PERCIVAL detector is a CMOS imager designed for the soft X-ray regime at photon sources. Although still in its final development phase, it has recently seen its first user experiments: ptychography at a free-electron laser, holographic imaging at a storage ring and preliminary tests on X-ray photon correlation spectroscopy. The detector performed remarkably well in terms of spatial resolution achievable in the sample plane, owing to its small pixel size, large active area and very large dynamic range; but also in terms of its frame rate, which is significantly faster than traditional CCDs. In particular, it is the combination of these features which makes PERCIVAL an attractive option for soft X-ray science., Published by Wiley-Blackwell, [Erscheinungsort nicht ermittelbar]

The journal of physical chemistry letters 14(20), 4719 - 4725 (2023). doi:10.1021/acs.jpclett.3c00631, The dynamics and time scales of higher-order correlations are studied in supercooled colloidal systems. A combination of X-ray photon correlation spectroscopy (XPCS) and X-ray cross-correlation analysis (XCCA) shows the typical slowing of the dynamics of a hard sphere system when approaching the glass transition. The time scales of higher-order correlations are probed using a novel time correlation function g$_C$, tracking the time evolution of cross-correlation function C. With an increasing volume fraction, the ratio of relaxation times of g$_C$ to the standard individual particle relaxation time obtained by XPCS increases from ∼0.4 to ∼0.9. While a value of ∼0.5 is expected for free diffusion, the increasing values suggest that the local orders within the sample are becoming more long-lived for larger volume fractions. Furthermore, the dynamics of local order is more heterogeneous than the individual particle dynamics. These results indicate that not only the presence but also the lifetime of locally favored structures increases close to the glass transition., Published by ACS, Washington, DC

Hamburg : Deutsches Elektronen-Synchrotron DESY 127 pp. (2021)., This White Paper describes the scope of the Centre for Molecular Water Science (CMWS), a collaborative, cross-disciplinary research initiative that shall use a highly dedicated laboratory infrastructure, the most advanced experimental techniques, leading theory/simulation tools and forefront photon facilities to answer the most important questions in molecular water science. The key scientific challenges, preliminary work, objectives, methodologies and infrastructural needs for five major scientific research areas (pillars) have been identified during the past three years by a group of more than 140 scientists from more than 15 countries. The results are compiled and summarised in this document. This task would not have been possible without the continued support from the host laboratory DESY in Hamburg (Germany). Special thanks to the Chairman of the DESY Board of Directors, Prof Helmut Dosch, and the Director in charge of Photon Science, Prof. Edgar Weckert., Published by Deutsches Elektronen-Synchrotron DESY, Hamburg

IUCrJ 8(5), 775 - 783 (2021). doi:10.1107/S2052252521006333, Many soft-matter systems are composed of macromolecules or nanoparticles suspended in water. The characteristic times at intrinsic length scales of a few nanometres fall therefore in the microsecond and sub-microsecond time regimes. With the development of free-electron lasers (FELs) and fourth-generation synchrotron light-sources, time-resolved experiments in such time and length ranges will become routinely accessible in the near future. In the present work we report our findings on prototypical soft-matter systems, composed of charge-stabilized silica nanoparticles dispersed in water, with radii between 12 and 15 nm and volume fractions between 0.005 and 0.2. The sample dynamics were probed by means of X-ray photon correlation spectroscopy, employing the megahertz pulse repetition rate of the European XFEL and the Adaptive Gain Integrating Pixel Detector. We show that it is possible to correctly identify the dynamical properties that determine the diffusion constant, both for stationary samples and for systems driven by XFEL pulses. Remarkably, despite the high photon density the only observable induced effect is the heating of the scattering volume, meaning that all other X-ray induced effects do not influence the structure and the dynamics on the probed timescales. This work also illustrates the potential to control such induced heating and it can be predicted with thermodynamic models., Published by Chester

Applied Sciences 11, 6179 (1-33) (2021). doi:10.3390/app11136179, X-ray photon correlation spectroscopy (XPCS) enables the study of sample dynamics between micrometer and atomic length scales. As a coherent scattering technique, it benefits from the increased brilliance of the next-generation synchrotron radiation and Free-Electron Laser (FEL) sources. In this article, we will introduce the XPCS concepts and review the latest developments of XPCS with special attention on the extension of accessible time scales to sub-μs and the application of XPCS at FELs. Furthermore, we will discuss future opportunities of XPCS and the related technique X-ray speckle visibility spectroscopy (XSVS) at new X-ray sources. Due to its particular signal-to-noise ratio, the time scales accessible by XPCS scale with the square of the coherent flux, allowing to dramatically extend its applications. This will soon enable studies over more than 18 orders of magnitude in time by XPCS and XSVS., Published by MDPI, Basel

IUCrJ 5(3), 354 - 360 (2018). doi:10.1107/S2052252518005407, We report on the self-assembly of gold nanoparticles coated with a soft poly(ethylene glycol) shell studied by X-ray cross-correlation analysis. Depending on the initial concentration of gold nanoparticles used, structurally heterogeneous films were formed. The films feature hot spots of dominating four- and sixfold local order with patch sizes of a few micrometres, containing 10$^4$–10$^5$ particles. The amplitude of the order parameters suggested that a minimum sample amount was necessary to form well ordered local structures. Furthermore, the increasing variation in order parameters with sample thickness demonstrated a high degree of structural heterogeneity. This wealth of information cannot be obtained by the conventional microscopy techniques that are commonly used to study nanocrystal superstructures, as illustrated by complementary scanning electron microscopy measurements., Published by IUCr, Chester

An X-ray cross-correlation study with emphasis on colloidal crystals is presented and demonstrates how to access higher-order structure beyond pair correlations. In this way symmetries of the crystal can be determined that are inaccessible in conventional crystallography., The results of an X-ray cross-correlation analysis (XCCA) study on hard-sphere colloidal crystals and glasses are presented. The article shows that cross-correlation functions can be used to extract structural information beyond the static structure factor in such systems. In particular, the powder average can be overcome by accessing the crystals’ unit-cell structure. In this case, the results suggest that the crystal is of face-centered cubic type. It is demonstrated that XCCA is a valuable tool for X-ray crystallography, in particular for studies on colloidal systems. These are typically characterized by a rather poor crystalline quality due to size polydispersity and limitations in experimental resolution because of the small q values probed. Furthermore, nontrivial correlations are observed that allow a more detailed insight into crystal structures beyond conventional crystallography, especially to extend knowledge in structure formation processes and phase transitions.

IUCrJ 5(6), 801 - 807 (2018). doi:10.1107/S2052252518013696, The application of X-ray photon correlation spectroscopy (XPCS) at free-electron laser (FEL) facilities enables, for the first time, the study of dynamics on a (sub-)nanometre scale in an unreached time range between femtoseconds and seconds. For soft-matter materials, radiation damage is a major limitation when going beyond single-shot applications. Here, an XPCS study is presented at a hard X-ray FEL on radiation-sensitive polymeric poly(N-isopropylacrylamide) (PNIPAM) nanoparticles. The dynamics of aqueous suspensions of densely packed silica-PNIPAM core-shell particles and a PNIPAM nanogel below the radiation-damage threshold are determined. The XPCS data indicate non-diffusive behaviour, suggesting ballistic and stress-dominated heterogeneous particle motions. These results demonstrate the feasibility of XPCS experiments on radiation-sensitive soft-matter materials at FEL sources and pave the way for future applications at MHz repetition rates as well as ultrafast modes using split-pulse devices., Published by Wiley, Chester