arXiv subjects

K. Sokolowski-Tinten

Publications and source records attributed to K. Sokolowski-Tinten.

10 recordsLinked to original sources

arXiv2025

Probing the atomic dynamics of ultrafast melting with femtosecond electron diffraction

Melting is an everyday phase transition that is determined by thermodynamic parameters like temperature and pressure. In contrast, ultrafast melting is governed by the microscopic response to a rapid energy input and, thus, can reveal the strength and dynamics of atomic bonds as well as the energy flow rate to the lattice. Accurately describing these processes remains challenging and requires detailed insights into transient states encountered. Here, we present data from femtosecond electron diffraction measurements that capture the structural evolution of copper during the ultrafast solid to liquid phase transformations. At absorbed energy densities 2 to 4 times the melting threshold, melting begins at the surface slightly below the nominal melting point followed by rapid homogeneous melting throughout the volume. Molecular dynamics simulations reproduce these observations and reveal a weak electron lattice energy transfer rate for the given experimental conditions. Both simulations and experiments show no indications of rapid lattice collapse when its temperature surpasses proposed limits of superheating, providing evidence that inherent dynamics limits the speed of disordering in ultrafast melting of metals.

cond-mat.mtrl-sci↗

arXiv2025

Laser-induced ultrafast structural transformations in thin Fe layer revealed by time-resolved X-ray diffraction

The ultrafast structural response of a thin iron film to sub-ps pulsed laser-induced heating has been investigated using time-resolved X-ray diffraction in the partial melting regime. A tetragonal distortion of the bcc-phase emerges at ~6 ps. Its formation is delayed relative to the initial heating (1-2 ps) and partial melting (2-5 ps) of the material, and controlled by the stress release in the quasi-instantaneously pressurized film. The distortion persists for at least 60 ps indicating the formation of a metastable bct phase between the equilibrium bcc and fcc phases.

cond-mat.mtrl-sci↗

arXiv2023

On the path to ion-based pump-probe experiments: Generation of 18 picosecond keV Ne$^+$ ion pulses from a cooled supersonic gas beam

The dynamics triggered by the impact of an ion onto a solid surface has been explored mainly by theoretical modeling or computer simulation to date. Results indicate that the microscopic non-equilibrium relaxation processes triggered by the interaction of the ion with the solid occur on (sub-)picosecond time scales. A suitable experimental approach to these dynamics therefore requires a pump-probe method with an appropriate time resolution. Recent experiments have successfully used laser photoionization of noble gas atoms in combination with a Wiley-MacLaren ion buncher to obtain arrival time distributions as narrow as $t_{ion} = 180$ ps. Here we show that this setup can be significantly improved by replacing the gas at a temperature of $T_{atoms}$ = 300 K with a supersonic beam of cooled noble gas atoms at $T_{atoms}$ = 4 K. The detailed analysis of measured arrival times of individual Ne$^+$ ions with a kinetic energy of 4 keV reveals that the arrival time jitter can be reduced by this technique down to (18$\pm$4) ps. This opens the door to pump-probe experiments with keV ions with a time-resolution in the picosecond range.

physics.atom-ph↗

arXiv2022

In-situ observation of the formation of laser-induced periodic surface structures with extreme spatial and temporal resolution

Irradiation of solid surfaces with intense ultrashort laser pulses represents a unique way of depositing energy into materials. It allows to realize states of extreme electronic excitation and/or very high temperature and pressure, and to drive materials close to and beyond fundamental stability limits. As a consequence, structural changes and phase transitions often occur along unusual pathways and under strongly non-equilibrium conditions. Due to the inherent multiscale nature - both temporally and spatially - of these irreversible processes their direct experimental observation requires techniques that combine high temporal resolution with the appropriate spatial resolution and the capability to obtain good quality data on a single pulse/event basis. In this respect fourth generation light sources, namely short wavelength, short pulse free electron lasers (FELs) are offering new and fascinating possibilities. As an example, this chapter will discuss the results of scattering experiments carried at the FLASH free electron laser at DESY (Hamburg, Germany), which allowed us to resolve laser-induced structure formation at surfaces on the nanometer to sub-micron length scale and in temporal regimes ranging from picoseconds to several nanoseconds with sub-picosecond resolution.

cond-mat.mtrl-sci↗

arXiv2021

Effect of lattice excitations on transient near edge X-ray absorption spectroscopy

Time-dependent and constituent-specific spectral changes in soft near edge X-ray spectroscopy (XAS) of an [Fe/MgO]$_8$ metal/insulator heterostructure upon laser excitation are analyzed at the O K-edge with picosecond time resolution. The oxygen absorption edge of the insulator features a uniform intensity decrease of the fine structure at elevated phononic temperatures, which can be quantified by a simple simulation and fitting procedure presented here. Combining X-ray absorption spectroscopy with ultrafast electron diffraction measurements and ab initio calculations demonstrate that the transient intensity changes in XAS can be assigned to a transient lattice temperature. Thus, the sensitivity of transient near edge XAS to phonons is demonstrated.

cond-mat.mtrl-sci↗

arXiv2019

Acoustic response of a laser-excited polycrystalline Au-film studied by ultrafast Debye-Scherrer diffraction at a table-top short-pulse X-ray source

The transient acoustic response of a free-standing, polycrystalline thin Au film upon femtosecond optical excitation has been studied by time-resolved Debye-Scherrer X-ray diffraction using ultrashort Cu K$_α$ X-ray pulses from a laser-driven plasma X-ray source. The temporal strain evolution has been determined from the transient shifts of multiple Bragg diffraction peaks. The experimental data are in good agreement with the results of calculations based on the two-temperature model and an acoustic model assuming uni-axial strain propagation in the laser-excited thin film.

cond-mat.mes-hall↗

arXiv2019

Microscopic non-equilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure

The element specificity of soft X-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. Using [Fe/MgO]$_n$ as a model system, we perform ultraviolet pump/soft X-ray probe experiments, which are sensitive to all constituents of these heterostructures, to probe both electronic and lattice excitations. Complementary ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and together with ab initio calculations yield comprehensive insight into the microscopic processes leading to local relaxation within a single constituent or non-local relaxation between two constituents. Besides electronic excitations in Fe, which are monitored at the Fe L$_3$ absorption edge and relax within 1 ps by electron-phonon coupling, soft X-ray analysis identifies a change at the oxygen K absorption edge of the MgO layers which occurs within 0.5 ps. This ultrafast energy transfer across the Fe-MgO interface is mediated by high-frequency, interface vibrational modes, which are excited by hot electrons in Fe and couple to vibrations in MgO in a mode-selective, non-thermal manner. A second, slower timescale is identified at the oxygen K pre-edge and the Fe L$_3$ edge. The slower process represents energy transfer by acoustic phonons and contributes to thermalization of the entire heterostructure. We thus find that the interfacial energy transfer is associated with non-equilibrium behavior in the phonon system. Because our experiments lack signatures of charge transfer across the interface, we conclude that phonon-mediated processes dominate the competition of electronic and lattice excitations in these non-local, non-equilibrium dynamics.

cond-mat.mtrl-sci↗

arXiv2019

Tracking the Ultrafast Non-Equilibrium Energy Flow between Electronic and Lattice Degrees of Freedom in Crystalline Nickel

Femtosecond laser excitation of solid-state systems creates non-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering we gain a detailed understanding of the complex non-equilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wavevector resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable agreement with our theoretical results. We find that zone-boundary phonon modes become occupied first. As soon as the energy in these modes becomes larger than the average electron energy a backflow of energy from lattice to electronic degrees of freedom occurs. Subsequent excitation of lower-energy phonon modes drives the thermalization of the whole system on the picosecond timescale. We determine the evolving non-equilibrium phonon occupations which we find to deviate markedly from thermal occupations.

cond-mat.mtrl-sci↗

arXiv2016

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO$_3$

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply sub-picosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO$_3$ ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond timescales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables direct comparison with first-principles-based molecular dynamics simulations, with good agreement obtained.

cond-mat.mtrl-sci↗

arXiv2013

Direct measurement of time-dependent density-density correlations in a solid through the acoustic analog of the dynamical Casimir effect

The macroscopic characteristics of a solid, such as its thermal, optical or transport properties are determined by the available microscopic states above its lowest energy level. These slightly higher quantum states are described by elementary excitations and dictate the response of the system under external stimuli. The spectrum of these excitations, obtained typically from inelastic neutron and x-ray scattering, is the spatial and temporal Fourier transform of the density-density correlation function of the system, which dictates how a perturbation propagates in space and time. As frequency-domain measurements do not generally contain phase information, time-domain measurements of these fluctuations could yield a more direct method for investigating the excitations of solids and their interactions both in equilibrium and far-from equilibrium. Here we show that the diffuse scattering of femtosecond x-ray pulses produced by a free electron laser (FEL) can directly measure these density-density correlations due to lattice vibrations in the time domain. We obtain spectroscopic information of the lattice excitations with unprecedented momentum- and frequency- resolution, without resolving the energy of the outgoing photon. Correlations are created via an acoustic analog of the dynamical Casimir effect, where a femtosecond laser pulse slightly quenches the phonon frequencies, producing pairs of squeezed phonons at momenta +q and -q. These pairs of phonons manifest as macroscopic, time-dependent coherences in the displacement correlations that are then probed directly by x-ray scattering. Since the time-dependent correlations are preferentially created in regions of strong electron-phonon coupling, the time-resolved approach is natural as a spectroscopic tool of low energy collective excitations in solids, and their microscopic interactions, both in linear response and beyond.

cond-mat.mtrl-sci↗