arXiv subjects

Fabian Westermeier

Publications and source records attributed to Fabian Westermeier.

12 recordsLinked to original sources

arXiv2026

Liquid-liquid phase separation precedes crystallization in supercooled water-glycerol solutions

Understanding the structural evolution of supercooled water-glycerol solutions is important for cryopreservation, yet distinguishing liquid-state transformations from ice crystallization remains challenging. Here, we investigate a deeply supercooled water-glycerol solution by X-ray photon correlation spectroscopy (XPCS) in ultra-small-angle X-ray scattering (USAXS) geometry, combined with wide-angle X-ray scattering (WAXS). This combination simultaneously captures the structural and dynamical evolution of the supercooled liquid upon quenching to cryogenic temperatures (172 K). We observe discontinuous changes in the liquid structure on molecular length scales and formation of microscale domains. The dynamics slow down during this stage and exhibit hyper-diffusive, ballistic-like relaxation. This transformation precedes ice crystallization, which we identify from the emergence of ice Bragg peaks in WAXS, allowing the two processes to be temporally separated. Phase-field (Cahn-Hilliard) simulations qualitatively reproduce the experimental observations and show that a spinodal-decomposition scenario is consistent with the measured scattering evolution. These findings are consistent with a liquid-liquid phase separation scenario preceding ice crystallization and provide a route to disentangle the two processes in supercooled aqueous systems.

cond-mat.soft↗

arXiv2026

X-ray photo-induced atomic motion in Phase Change Materials and conventional covalent chalcogenide glasses

X-ray Photon Correlation Spectroscopy (XPCS) enables direct access to atomic-scale dynamics in disordered materials, revealing both spontaneous and X-ray-induced relaxation processes. Here, we study two compositionally similar alloy glasses near their glass transition temperatures: the phase change material (PCM) Ge15Sb85 and the non-PCM alloy Ge15Te85. Both exhibit X-ray induced atomic motion, yet with markedly different responses. Ge15Sb85 undergoes an immediate transition to a photo-induced yielding state, characterised by stationary dynamics governed solely by the absorbed dose. In contrast, Ge15Te85 shows a progressive slowing-down of the relaxation process, accompanied by a crossover from compressed to stretched exponential decay in the density autocorrelation functions. This behaviour is consistent with the emergence of liquid-like collective motion as supported by de Gennes narrowing in the wave-vector dependence of the dynamics at length scales comparable with the first sharp diffraction peak. Unlike Ge15Sb85, this alloy does not reach a stationary regime within experimental timescales, implying that the yielding transition occurs only after thousands of seconds with the available dose rate. Its response is also temperature dependent: at lower temperatures, the dynamics reflects intrinsic stress relaxation processes, whereas at higher temperatures becomes dose-controlled. These findings demonstrate that the dynamical response to X-ray excitation is not determined solely by chemical composition or bonding character, but results from the interplay between irradiation effects and structural relaxation pathways.

cond-mat.mtrl-sci↗

arXiv2025

X-ray photon correlation spectroscopy of hydrated lysozyme at elevated pressures

Pressure provides a powerful parameter to control the protein conformation state, which at sufficiently high values can lead to unfolding. Here, we investigate the effects of increasing pressure up to $0.4$ GPa on hydrated lysozyme proteins, by measuring the nanoscale stress relaxation induced and probed by X-rays. Structural and dynamical information at elevated pressures was obtained using X-ray photon correlation spectroscopy (XPCS) in combination with a diamond anvil cell (DAC). The dynamical analysis revealed a slowing down of the system up to $0.2$ GPa, followed by a re-acceleration at $0.4$ GPa. A similar non-monotonic behavior was observed both in the Porod and Kohlrausch-Williams-Watts (KWW) exponents, consistently indicating a crossover between $0.2$ and $0.4$ GPa. These findings suggest the presence of pressure-induced structural changes that impact protein collective stress-relaxation as the system transitions from a jammed state to an elastically driven regime. These results may be relevant for a deeper understanding of protein stability under compression as well as for practical high-pressure technologies, including food processing and pharmaceutical applications.

cond-mat.soft↗

arXiv2025

Defect migration in supercrystalline nanocomposites

Supercrystalline nanocomposites (SCNCs) are nanostructured hybrid materials with unique emergent functional properties. Given their periodically arranged building blocks, they also offer interesting parallelisms with crystalline materials. They can be processed in multiple forms and at different scales, and crosslinking their organic ligands via heat treatment leads to a remarkable boost of their mechanical properties. This study shows, via X-ray and in-situ scanning transmission (STEM) electron microscopy analyses, how each of these processing steps plays a distinct role in the generation, migration, interaction and healing of supercrystalline defects. Pressing of SCNCs into bulk pellets leads to a distortion of the otherwise fcc superlattice, while emulsion-templated self-assembly yields supraparticles (SPs) with stacking faults and size-dependent symmetries. Interestingly, heat treatment at the same temperatures as those applied for the organic crosslinking has significant effects on planar defects. Stacking faults migrate and get healed, as also confirmed via molecular dynamics simulations, and inter-supercrystalline 'grain' boundaries undergo structural changes. These rearrangements of defects at the supercrystalline scale (tens of nm) in nanocomposites with such remarkable mechanical properties (compressive strength of 100-500 MPa) provide new insights into the formation and evolution of ordered assemblies of functionalized nanoparticles.

cond-mat.mtrl-sci↗

arXiv2025

Three-phase contact line dynamics on moving fibers measured by X-ray holography

Wetting of solid surfaces by a liquid is important for many natural and industrial processes such as printing, painting and coating. However, a quantitative description of the dynamic receding and advancing contact angle is still debated, in particular for aqueous solutions. One reason for our lack of quantitative understanding is the limited spatial resolution of currently used optical methods. We therefore present a new approach to access the sub-microscopic region. We use X-ray phase contrast imaging to measure the dynamic receding contact angle on a moving glass fiber of 17 um diameter. The fiber was pulled out of a liquid bath which was filled with a mixture of glycerol and Milli-Q water. The dynamic receding contact angle decreased with increasing contact line velocity for all mixtures. In the holograms we achieved a resolution of 50 nm/pixel with a spatial error of 450 nm. This spatial error is due to an extended surface region of the fiber and the liquid surface in the holograms. Our results demonstrate the feasibility of X-ray holography as a method to investigate dynamic contact angle phenomena and thereby opening pathways to higher spatial and temporal resolution.

physics.chem-ph↗

arXiv2025

Linking the pressure dependence of the structure and thermal stability to {\alpha}- and \b{eta}-relaxations in metallic glasses

Glasses derive their functional properties from complex relaxation dynamics that remain enigmatic under extreme conditions. While the temperature dependence of these relaxation processes is well-established, their behavior under high-pressure conditions remains poorly understood due to significant experimental difficulties. In this study, we employ cutting-edge experimental techniques to probe the pressure evolution of the relaxation spectrum in a Zr46.8Ti8.2Cu7.5Ni10Be27.5 metallic glass across gigapascal pressure ranges. Our findings reveal two distinct relaxation mechanisms under high pressure: In the \b{eta}-relaxation regime, compression drives the system with reduced atomic mobility and enhanced structural disorder, without significant density changes. Conversely, {\alpha}-relaxation under pressure promotes density-driven structural ordering that improves thermal stability. Notably, the transition between these regimes occurs at a constant T/Tg,P ratio, independent of applied pressure. These results provide crucial insights for decoupling the competing structural and relaxation contributions to glass stability, establishing a systematic framework for tailoring glass properties through controlled thermo-mechanical processing.

cond-mat.mtrl-sci↗

arXiv2024

On the interplay of liquid-like and stress-driven dynamics in a metallic glass former observed by temperature scanning XPCS

Modern detector technology and highly brilliant fourth-generation synchrotrons allow to improve the temporal resolution in time-resolved diffraction studies. Profiting from this, we applied temperature scanning X-ray photon correlation spectroscopy (XPCS) to probe the dynamics of a Pt-based metallic glass former in the glass, glass transition region, and supercooled liquid, covering up to six orders of magnitude in time scales. Our data demonstrates that the structural alpha-relaxation process is still observable in the glass, although it is partially masked by a faster source of decorrelation observed at atomic scale. We present an approach that interprets these findings as the superposition of heterogeneous liquid-like and stress-driven ballistic-like atomic motions. This work not only extends the dynamical range probed by standard isothermal XPCS, but also clarifies the fate of the alpha-relaxation across the glass transition and provides a new perception on the anomalous, compressed temporal decay of the density-density correlation functions observed in metallic glasses and many out-of-equilibrium soft materials.

cond-mat.mtrl-sci↗

arXiv2023

Coherent X-ray Scattering Reveals Nanoscale Fluctuations in Hydrated Proteins

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.

cond-mat.soft↗

arXiv2022

Disentangling structural and kinetic components of the {\alpha}-relaxation in supercooled metallic liquids

The particle motion associated to the {\alpha}-relaxation in supercooled liquids is still challenging scientists due to its difficulty to be probed experimentally. By combining synchrotron techniques, we found the existence of microscopic structure-dynamics relationships in Pt42.5Cu27Ni9.5P21 and Pd42.5Cu27Ni9.5P21 liquids which allows us to disentangle structural and kinetic contributions to the {\alpha}-process. While the two alloys show similar kinetic fragilities, their structural fragilities differ and correlate with the temperature dependence of the stretching parameter describing the decay of the density fluctuations. This implies that the evolution of dynamical heterogeneities in supercooled alloys is determined by the rigidity of the melt structure. We find also that the atomic motion not only reflects the topological order but also the chemical short-range order, which can lead to a surprising slowdown of the {\alpha}-process at the mesoscopic length scale. These results will contribute to the comprehension of the glass transition, which is still missing.

cond-mat.mtrl-sci↗

arXiv2022

In-situ Characterization of Crystallization and Melting of Soft, Thermoresponsive Microgels by Small-Angle X-ray Scattering

Depending on the volume fraction and interparticle interactions, colloidal suspensions can form different phases, ranging from fluids, crystals, and glasses to gels. For soft microgels that are made from thermoresponsive polymers, the volume fraction can be tuned by temperature, making them excellent systems to experimentally study phase transitions in dense colloidal suspensions. However, investigations of phase transitions at high particle concentration and across the volume phase transition temperature in particular, are challenging due to the deformability and possibility for interpenetration between microgels. Here, we investigate the dense phases of composite core-shell microgels that have a small gold core and a thermoresponsive microgel shell. Employing Ultra Small Angle X-ray Scattering, we make use of the strong scattering signal from the gold cores with respect to the almost negligible signal from the shells. By changing the temperature we study the freezing and melting transitions of the system in-situ. Using Bragg peak analysis and the Williamson-Hall method, we characterize the phase transitions in detail. We show that the system crystallizes into an rhcp structure with different degrees of in-plane and out-of-plane stacking disorder that increase upon particle swelling. We further find that the melting process is distinctly different, where the system separates into two different crystal phases with different melting temperatures and interparticle interactions.

cond-mat.soft↗

arXiv2021

Using low dose X-ray Speckle Visibility Spectroscopy to study dynamics of soft matter samples

We demonstrate the successful application of X-ray Speckle Visibility Spectroscopy (XSVS) experiments to study the dynamics of radiation sensitive, biological samples with unprecedentedly 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 (XPCS). 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.

cond-mat.soft↗

arXiv2021

Interplay between Kinetics and Dynamics of Liquid-Liquid Phase Separation in a Protein Solution Revealed by Coherent X-ray Spectroscopy

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 structural relaxation kinetics is up to 40 times slower than the dynamics and thus can be decoupled. The kinetic decay rate is inversely proportional to time in the early stage, followed by a nearly constant behavior during the coarsening stage. 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.

cond-mat.soft↗