arXiv subjects

James Wrigley

Publications and source records attributed to James Wrigley.

10 recordsLinked to original sources

arXiv2026

Generation of high-fluence and high-intensity hard x-ray attosecond pulses at European XFEL

By combining hard x-ray attosecond pulses from the European XFEL with total-reflection focusing x-ray optics, we generated nanofocused hard x-ray attosecond pulses with intensities and fluences comparable to the highest values attained in the hard x-ray regime. A peak intensity on the order of 10$^{20}$ W/cm$^2$ is confirmed through the observation of saturation in amplified spontaneous emission from copper atoms. These x-ray pulses enable new scientific opportunities, including the exploration of higher-order nonlinear light--matter interactions, damage-free structure determination, and coherent control of atoms and molecules.

physics.optics↗

arXiv2025

Spatio-temporal migration of antiferromagnetic domain walls in Sr2IrO4

By laser pump-probe time-resolved coherent magnetic X-ray diffraction imaging, we have measured the migration velocity of antiferromagnetic domain walls in the Mott insulator Sr2IrO4 at 100 K. During the laser-induced demagnetization, we observe domain walls moving at 3x10^6 m/s, significantly faster than acoustic velocities. This is understood to arise from a purely electronic spin contribution to the magnetic structure without any role for coupling to the crystal lattice.

cond-mat.str-el↗

arXiv2025

Depletion-Induced Interactions Modulate Nanoscale Protein Diffusion in Polymeric Crowder Solutions

Macromolecular crowding plays a crucial role in modulating protein dynamics in cellular and in vitro environments. Polymeric crowders such as dextran and Ficoll are known to induce entropic forces, including depletion interactions, that promote structural organization, but the nanoscale consequences for protein dynamics remain less well understood. Here, we employ megahertz X-ray photon correlation spectroscopy (MHz-XPCS) at the European XFEL to probe the dynamics of the protein ferritin in solutions containing sucrose, dextran, and Ficoll. We find that depletion-driven short-range attractions combined with long-range repulsions give rise to intermediate-range order (IRO) once the polysaccharide overlap concentration $c^*$ is exceeded. These IRO features fluctuate on microsecond to millisecond timescales, strongly modulating the collective dynamics of ferritin. The magnitude of these effects depends sensitively on crowder type, concentration, and molecular weight. Normalizing the crowder concentration by $c^*$ reveals scaling behavior in ferritin self-diffusion with a crossover near 2$c^*$, marking a transition from depletion-enhanced mobility to viscosity-dominated slowing. Our results demonstrate that bulk properties alone cannot account for protein dynamics in crowded solutions, underscoring the need to include polymer-specific interactions and depletion theory in models of crowded environments.

cond-mat.soft↗

arXiv2025

Ultrafast heat transfer in single palladium nanocrystals seen with an X-ray free-electron laser

We report transient highly strained structural states in individual palladium (Pd) nanocrystals, electronically heated using an optical laser, which precede their uniform thermal expansion. Using an X-ray free-electron laser probe, the evolution of individual 111 Bragg peaks is measured as a function of delay time at various laser fluences. Above a laser fluence threshold at a sufficient pump-probe delay, the Bragg peak splits into multiple peaks, indicating heterogeneous strain, before returning to a single peak, corresponding to even heat distribution throughout the lattice expanded crystal. Our findings are supported by a lattice displacement and strain model of a single nanocrystal at different delay times, which agrees with the experimental data. Our observations have implications for understanding femtosecond laser interactions with metals and the potential photo-catalytic performance of Pd.

cond-mat.mtrl-sci↗

arXiv2025

Ultrafast X-ray sonography reveals the spatial heterogeneity of the laser-induced magneto-structural phase transition in FeRh

Phase transitions are governed by both intrinsic and extrinsic heterogeneities, yet capturing their spatio-temporal dynamics remains a challenge. While ultrafast techniques track phase changes on femtosecond timescales, the spatial complexity and stochastic nature of the processes often remain hidden. Here, we present an experimental approach that combines well-established ultrafast hard-X-ray diffraction with a propagating strain pulse as a universal and non-invasive probe. This ultrafast X-ray sonography can capture the spatio-temporal phase heterogeneity in great detail by resolving the phase-specific strain response. We apply this approach to the antiferromagnetic-to-ferromagnetic magneto-structural phase transition in FeRh and identify the ferromagnetic phase to nucleate at the surface as narrow columnar domains of approximately $30\,\text{nm}$ diameter. Besides reconciling the diverse experimental results in the literature on FeRh, X-ray sonography offers a versatile platform for investigating a wide range of phase transitions accompanied by structural changes.

cond-mat.mtrl-sci↗

arXiv2025

A pipeline for Megahertz X-ray Photon Correlation Spectroscopy on soft matter samples at the MID instrument of European XFEL

In this paper we present the experimental protocol and data processing framework for Megahertz X-ray Photon Correlation Spectroscopy (MHz-XPCS) experiments on soft matter samples, implemented at the Materials Imaging and Dynamics (MID) instrument of the European X-ray Free-Electron Laser (EuXFEL). Due to the introduction of a standard configuration and the implementation of a highly automated data processing pipeline, MHz-XPCS measurements can now be conducted and analyzed with minimal user intervention. A key challenge lies in managing the extremely large data volumes generated by the Adaptive Gain Integrating Pixel Detector (AGIPD) - often reaching several petabytes within a single experiment. We describe the technical implementation, discuss the hardware requirements related to effective parallel data processing, and propose strategies to enhance data quality, in particular related to data reduction strategies and an improvement of the signal-to-noise ratio. Finally, we address strategies for making the processed data FAIR (Findable, Accessible, Interoperable, Reusable), in alignment with the goals of the DAPHNE4NFDI project.

physics.ins-det↗

arXiv2025

Softness and Hydrodynamic Interactions Regulate Lipoprotein Transport in Crowded Yolk Environments

Low-density lipoproteins (LDLs) serve as nutrient reservoirs in egg yolk for embryonic development and as promising drug carriers. Both roles critically depend on their mobility in densely crowded biological environments. Under these crowded conditions, diffusion is hindered by transient confinement within dynamic cages formed by neighboring particles, driven by solvent-mediated hydrodynamic interactions and memory effects -- phenomena that have remained challenging to characterize computationally and experimentally. Here, we employ megahertz X-ray photon correlation spectroscopy to directly probe the cage dynamics of LDLs in yolk-plasma across various concentrations. We find that LDLs undergo anomalous diffusion, experiencing $\approx$ 100-fold reduction in self-diffusion at high concentrations compared to dilute solutions. This drastic slowing-down is attributed to a combination of hydrodynamic interactions, direct particle-particle interactions, and the inherent softness of LDL particles. Despite reduced dynamics, yolk-plasma remains as a liquid, yet sluggish, balancing dense packing, structural stability, and fluidity essential for controlled lipid release during embryogenesis.

cond-mat.soft↗

arXiv2025

Orthogonal lattice distortions inside crystalline Si upon sub-threshold femtosecond laser-induced excitation

Material processing with femtosecond lasers has attracted enormous attention because of its potential for technology and industrial applications. In parallel, time-resolved x-ray diffraction has been successfully used to study ultrafast structural distortion dynamics in semiconductor thin films or surface layers. However, real-world processing applications mostly are concerned with bulk materials, which prevents the use of x-ray surface based techniques. For processing applications, a fast and depth-sensitive probe is needed. To address this, we present a novel technique based on ultrafast x-ray dynamical diffraction (UDD) capable of imaging transient strain distributions inside bulk crystals upon laser excitation. This pump-probe technique provides a complete picture of thetemporal evolution of ultrafast distorted lattice depth profiles. We demonstrate the potential of UDD by studying a thin Si single crystal upon single pulse femtosecond optical excitation. Our study reveals that below the melting threshold strong lattice distortions not only longitudinal, but also transversal to the propagation of the strain wave appear on picosecond time scales along the single crystal. The observation of this transversal deformation after laser excitation contradicts previous work that were not able to observed it, what could be related to the high sensitivity of dynamical diffraction with respect to the lattice distortions. The speed of propagation of this ultrafast transversal strain deformation is observed to be slower to the longitudinal sound speed for Si as described in the bibliography.

cond-mat.mtrl-sci↗

arXiv2024

Coherent X-rays reveal anomalous molecular diffusion and cage effects in crowded protein solutions

Understanding protein motion within the cell is crucial for predicting reaction rates and macromolecular transport in the cytoplasm. A key question is how crowded environments affect protein dynamics through hydrodynamic and direct interactions at molecular length scales. Using megahertz X-ray Photon Correlation Spectroscopy (MHz-XPCS) at the European X-ray Free Electron Laser (EuXFEL), we investigate ferritin diffusion at microsecond time scales. Our results reveal anomalous diffusion, indicated by the non-exponential decay of the intensity autocorrelation function $g_2(q,t)$ at high concentrations. This behavior is consistent with the presence of cage-trapping in between the short- and long-time protein diffusion regimes. Modeling with the $\delta\gamma$-theory of hydrodynamically interacting colloidal spheres successfully reproduces the experimental data by including a scaling factor linked to the protein direct interactions. These findings offer new insights into the complex molecular motion in crowded protein solutions, with potential applications for optimizing ferritin-based drug delivery, where protein diffusion is the rate-limiting step.

cond-mat.soft↗

arXiv2024

Origins of suppressed self-diffusion of nanoscale constituents of a complex liquid

Understanding and ultimately controlling the transformations and properties of nanoscale systems, from proteins to synthetic nanomaterial assemblies, is limited by the inability to uncover their dynamics on their characteristic length and time scales. Here, we nevertheless demonstrate this ability using MHz X-ray photon correlation spectroscopy (XPCS) -- directly elucidating the characteristic microsecond-dynamics of density fluctuations of semiconductor nanocrystals (NCs), not only in a colloidal dispersion but also in a liquid phase consisting of densely packed, yet mobile, NCs with no long-range order. We find the wavevector-dependent fluctuation rates in the liquid phase are suppressed relative to those in the colloidal phase and relative to observations of densely packed repulsive particles. We show that the suppressed rates are due to a substantial decrease in the self-diffusion of NCs, which we attribute to explicit attractive interactions. Using coarse-grained simulations, we find that the extracted shape and strength of the interparticle potential explains the stability of the liquid phase, in contrast to the gelation observed via XPCS in many other charged colloidal systems. This work opens the door to elucidating fast, condensed phase dynamics in complex fluids and other nanoscale soft matter, such as densely packed proteins and non-equilibrium self-assembly processes, in addition to designing microscopic strategies to avert gelation.

cond-mat.soft↗