SearcharxivSearch

arXiv subjects

Tobias Eklund

Publications and source records attributed to Tobias Eklund.

6 recordsLinked to original sources

Ultrafast light-induced formation of a metastable hidden state in bismuth vanadate

Bismuth vanadate (BiVO$_4$) is a key photocatalyst for solar fuel applications, yet fundamental questions remain regarding the nature of photogenerated polaronic states and the lattice dynamics that govern its light-to-chemical pathways. Here, we use femtosecond optical pump-X-ray probe measurements to track the photoinduced electronic and structural dynamics in BiVO$_4$ across multiple length and time scales. Transient X-ray absorption spectroscopy captures sub-picosecond electron localization within VO$_4$ tetrahedra, consistent with small polaron formation, whereas time-resolved X-ray diffraction reveals a slower, multi-picosecond lattice reorganization into a hidden photoexcited state that is structurally distinct from both the monoclinic ground state and the high-temperature tetragonal phase. Supported by density functional theory, we show that hole-lattice interactions dynamically reduce the ground state monoclinic distortion, stabilizing the hidden state. Our results demonstrate that electron- and hole-lattice coupling jointly shape the excited state landscape, with implications for carrier transport, interfacial energetics, and light-to-chemical energy conversion pathways.

cond-mat.mtrl-sci

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

Global $q$-dependent inverse transforms of intensity autocorrelation data

We present a new analysis approach for intensity autocorrelation data, as measured with dynamic light scattering and X-ray photon correlation spectroscopy. Our analysis generalizes the established CONTIN and MULTIQ methods by direct nonlinear modeling of the $g_2$ function, enabling decomposition of complex dynamics without a priori knowledge of experimental scaling factors. We describe the mathematical formulation, implementation details, and strategies for solution, as well as demonstrate decompositions of soft matter dynamics data into distributions of diffusion rates/velocities. The open-source MATLAB implementation, including example data, is publicly available for adoption and further development.

cond-mat.soft

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

Melting Domain Size and Recrystallization Dynamics of Ice Revealed by Time-Resolved X-ray Scattering

The phase transition between water and ice is ubiquitous and one of the most important phenomena in nature. Here, we performed time-resolved x-ray scattering experiments capturing the melting and recrystallization dynamics of ice. The ultrafast heating of ice I is induced by an IR laser pulse and probed with an intense x-ray pulse, which provided us with direct structural information on different length scales. From the wide-angle x-ray scattering (WAXS) patterns, the molten fraction, as well as the corresponding temperature at each delay, were determined. The small-angle x-ray scattering (SAXS) patterns, together with the information extracted from the WAXS analysis, provided the time-dependent change of the size and the number of the liquid domains. The results show partial melting (~13 %) and superheating of ice occurring at around 20 ns. After 100 ns, the average size of the liquid domains grows from about 2.5 nm to 4.5 nm by the coalescence of approximately six adjacent domains. Subsequently, we capture the recrystallization of the liquid domains, which occurs on microsecond timescales due to the cooling by heat dissipation and results to a decrease of the average liquid domain size.

physics.chem-ph

Energy in Newtonian gravity

In Newtonian gravity it is a moot question whether energy should be localized in the field or inside matter. An argument from relativity suggests a compromise in which the contribution from the field in vacuum is positive definite. We show that the same compromise is implied by Noether's theorem applied to a variational principle for perfect fluids, if we assume Dirichlet boundary conditions on the potential. We then analyse a thought experiment due to Bondi and McCrea that gives a clean example of inductive energy transfer by gravity. Some history of the problem is included

gr-qc