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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.

Ultrashort and intense extreme ultraviolet (XUV) and X-ray pulses readily available at free-electron lasers (FELs) enable studying non-linear light−matter interactions on femtosecond timescales. Here, we report on the non-linear fluence dependence of magnetic scattering of Co/Pt multilayers, using FERMI FEL’s 70-fs-long single and double XUV pulses, the latter with a temporal separation of 200 fs, with a photon energy slightly detuned to the Co M2,3 absorption edge. We observe a quenching in magnetic scattering that sets-in already in the non-destructive fluence regime of a few mJ/cm² typically used for FEL-probe experiments on magnetic materials. Calculations of the transient electronic structure in tandem with a phenomenological modeling of the experimental data by means of ultrafast demagnetization unambiguously show that XUV-radiation-induced demagnetization is the dominant mechanism for the quenching in the investigated fluence regime of

One of the intriguing problems of modern magnetism is unravelling the non-equilibrium spin dynamics following laser excitation on the nanometer length scale. In this work the ultrafast magnetic behavior of thin Co/Pt multilayers is studied by resonant magnetic SAXS in transmission geometry. We have for the first time observed a very bright transient scattering from nanometer scale magnetic fluctuations.

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.

The generation of two X-ray pulses with tunable nanosecond scale time separations has recently been demonstrated at the Linac Coherent Light Source using an accelerator based technique. This approach offers the opportunity to extend X-ray Photon Correlation Spectroscopy techniques to the yet unexplored regime of nanosecond timescales by means of X-ray Speckle Visibility Spectroscopy. As the two pulses originate from two independent Spontaneous Amplified Stimulated Emission processes, the beam properties fluctuate from pulse pair to pulse pair, but as well between the individual pulses within a pair. However, two-pulse XSVS experiments require the intensity of the individual pulses to be either identical in the ideal case, or with a accurately known intensity ratio. We present the design and performances of a non-destructive intensity diagnostic based on measurement of scattering from a transparent target using a high-speed photo-detector. Individual pulses within a pulse pair with time delays as short as 0.7 ns can be resolved. Moreover, using small angle coherent scattering, we characterize the averaged spatial overlap of the focused pulse pairs. The multi-shot average-speckle contrasts from individual pulses and pulse pairs are compared.

We present a method to determine the two-dimensional spatial coherence of synchrotron radiation in the soft X-ray regime by analyzing the Fourier transform of the magnetic speckle pattern from a ferromagnetic film in a multidomain state. To corroborate the results, a Young's double-pinhole experiment has been performed. The transverse coherence lengths in vertical and horizontal direction of both approaches are in a good agreement. The method presented here is simple and gives a direct access to the coherence properties of synchrotron radiation without nanostructured test objects.

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 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.

We have explored the feasibility of X-ray fluorescence correlation spectroscopy for studying the dynamics of colloidal particles in solution. We measured suspensions of Au nanoparticles from 5 to 150 nm diameter in water/glycerol mixtures of various compositions. Time-averaged sample properties were traced via small-angle X-ray scattering. The contrast of the measured time-correlation functions scales as expected with the particle concentration in the sample. The time constants for translational diffusion and sedimentation in water/glycerol mixtures follow only qualitatively the expected behaviour.

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.

A hard X-ray delay line device capable of splitting single FEL X-ray pulses into two adjustable fractions and recombining them with the goal of performing X-ray Photon Correlation Spectroscopy and pump - probe type studies was designed. The performance of the device has been verified at the XPP and XCS instruments of LCLS. The measured throughput of the device at 7.9 keV is 3.6%. The coherence properties of the LCLS beam passing through the delay line were investigated by analyzing speckle patterns produced by single LCLS pulses. A high speckle contrast of 0.69 was found, indicating the feasibility of performing coherence based experiments with the delay line.

We report a comprehensive joint experimental-theoretical study of the equilibrium pair-structure and short-time diffusion in aqueous suspensions of highly charged poly-acrylate (PA) spheres in the colloidal fluid phase. Low-polydispersity PA sphere systems with two different hard-core radii, R(0) = 542 and 1117 Å, are explored over a wide range of concentrations and salinities using static and dynamic light scattering (DLS), small angle x-ray scattering, and x-ray photon correlation spectroscopy (XPCS). The measured static and dynamic scattering functions are analyzed using state-of-the-art theoretical methods. For all samples, the measured static structure factor, S(Q), is in good agreement with results by an analytical integral equation method for particles interacting by a repulsive screened Coulomb plus hard-core pair potential. In our DLS and XPCS measurements, we have determined the short-time diffusion function D(Q) = D(0) H(Q)∕S(Q), comprising the free diffusion coefficient D(0) and the hydrodynamic function H(Q). The latter is calculated analytically using a self-part corrected version of the δγ-scheme by Beenakker and Mazur which accounts approximately for many-body hydrodynamic interactions (HIs). Except for low-salinity systems at the highest investigated volume fraction φ ≈ 0.32, the theoretical predictions for H(Q) are in excellent agreement with the experimental data. In particular, the increase in the collective diffusion coefficient D(c) = D(Q → 0), and the decrease of the self-diffusion coefficient, D(s) = D(Q → ∞), with increasing φ is well described. In accord with the theoretical prediction, the peak value, H(Q(m)), of H(Q) relates to the nearest neighbor cage size ∼2π∕Q(m), for which concentration scaling relations are discussed. The peak values H(Q(m)) are globally bound from below by the corresponding neutral hard-spheres peak values, and from above by the limiting peak values for low-salinity charge-stabilized systems. HIs usually slow short-time diffusion on colloidal length scales, except for the cage diffusion coefficient, D(cge) = D(Q(m)), in dilute low-salinity systems where a speed up of the system dynamics and corresponding peak values of H(Q(m))1 are observed experimentally and theoretically.

We report on the feasibility of high wavevector temporal speckle correlation measurements at the world’s first hard x-ray free electron laser, the Linac Coherent Light Source (LCLS). Due to the chaotic nature of LCLS, the spectral profile of the x-ray radiation fluctuates on a pulse-to-pulse basis. Its impact on the determination of the single shot speckle contrast in a wide angle x-ray scattering geometry is investigated by analyzing FEL power spectra that are simulated based on the nominal operational parameters of LCLS. Ultimately, a potential scheme to deliver a single-mode hard x-ray pulse is proposed by using a narrow bandpass crystal monochromator.

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., A hard X-ray delay line capable of splitting and delaying single X-ray pulses has been developed with the aim of performing X-ray photon correlation spectroscopy (XPCS) and X-ray pump–probe experiments at hard X-ray free-electron laser sources. The performance of the device was tested with 8.39 keV synchrotron radiation. Time delays up to 2.95 ns have been demonstrated. The feasibility of the device for performing XPCS studies was tested by recording static speckle patterns. The achieved speckle contrast of 56% indicates the possibility of performing ultra-fast XPCS studies with the delay line.

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.