arXiv subjects

B. Rethfeld

Publications and source records attributed to B. Rethfeld.

17 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

Capturing non-equilibrium electron dynamics in metals accurately and efficiently

The simulation of non-equilibrium electron distributions is essential for capturing light-metal interactions and therefore the study of photoabsorption, photocatalysis, laser ablation, and many other phenomena. Current methodologies, such as the Boltzmann equation using full collision integrals, describe non-equilibrium electron dynamics in great detail but at often prohibitive computational expense. In contrast, the simplification via a relaxation time approach can hinder the description of important features or, even worse, lead to nonphysical behavior due to the lack of particle and energy conservation. We propose a model that bridges the gap between the Boltzmann equation and two-temperature models to trace non-equilibrium distributions efficiently. This Athermal Electron Model (AthEM) separately captures the dynamics of thermal and athermal electrons and describes the energy and particle flow between two electronic systems and phonons. We show that the results align well with the results of Boltzmann equation and data from photoemission experiments. The AthEM enables the rapid generation of qualitatively accurate non-equilibrium electron distributions and provides a good starting point for further extensions.

cond-mat.mtrl-sci↗

arXiv2023

An adaptive model for the optical properties of excited gold

We study the temperature-dependent optical properties of gold over a broad energy spectrum covering photon energies below and above the interband threshold. We apply a semi-analytical Drude-Lorentz model with temperature-dependent oscillator parameters. Our approximations are based on the distribution of electrons over the active bands with a density of states provided by density functional theory. This model can be easily adapted to other materials with similar band structures and can also be applied to the case of occupational nonequilibrium. Our calculations show a strong enhancement of the intraband response with increasing electron temperature while the interband component decreases. Moreover, our model compares well with density functional theory-based calculations for the reflectivity of highly excited gold and reproduces many of its key features. Applying our methods to thin films shows a sensitive nonlinear dependence of the reflection and absorption on the electron temperature. These features are more prominent at small photon energies and can be highlighted with polarized light. Our findings offer valuable insights for modeling ultrafast processes, in particular, the pathways of energy deposition in laser-excited samples.

cond-mat.mtrl-sci↗

arXiv2023

Effect of iron thicknesses on spin transport in a Fe/Au bilayer system

This paper is concerned with a theoretical analysis of the behavior of optically excited spin currents in bilayer and multilayer systems of ferromagnetic and normal metals. As the propagation, control and manipulation of the spin currents created in ferromagnets by femtosecond optical pulses is of particular interest, we examine the influence of different thicknesses of the constituent layers for the case of electrons excited several electronvolts above the Fermi level. Using a Monte-Carlo simulation framework for such highly excited electrons, we first examine the spatio-temporal characteristics of the spin current density driven in a Fe layer, where the absorption profile of the light pulses plays an important role. Further, we examine how the combination of light absorption profiles, spin-dependent transmission probabilities, and iron layer thicknesses affect spin current density in a Fe/Au bilayer system. For high-energy electrons studied here, the interface and secondary electron generation have a small influence on spin transport in the bilayer system. However, we find that spin injection from one layer to another is most effective within a certain range of iron layer thicknesses.

cond-mat.mes-hall↗

arXiv2022

Fundamentals of Scanning Surface Structuring by Ultrashort Laser Pulses: From Electron Diffusion to Final Morphology

Industrial use of ultrashort-pulse surface structuring would significantly increase by an effective utilization of the average laser powers available currently. However, the unexplained degradation of surfaces processed with numerous pulses at high average laser power makes this difficult. Based on a systematic experimental study, the structure formation underlying such surface degradation was investigated. We presented a hierarchical structural formation model that bridges the gap between laser-induced periodic surface structures and surface degradation. Contrary to expectations based on previous research, we observed less structure formation on titanium for high laser fluences. As a possible reason, enhanced electron diffusion with increasing intensity was investigated within the framework of the two-temperature model. Our findings provide a deeper understanding of the microscopic mechanisms involved in surface structuring with ultrashort pulses.

physics.app-ph↗

arXiv2021

Monte Carlo simulation of ultrafast nonequilibrium spin and charge transport in iron

Spin transport and spin dynamics after femtosecond laser pulse irradiation of iron (Fe) are studied using a kinetic Monte Carlo model. This model simulates spin dependent dynamics by taking into account two interaction processes during nonequilibrium: Elastic electron - lattice scattering, where only the direction of the excited electrons changes neglecting the energy loss, and inelastic electron - electron interaction, where secondary electrons are generated. An analysis of the particle kinetics inside the material shows that a smaller elastic scattering time affects the spin dynamics by leading to a larger spatial spread of electrons in the material, whereas generation of secondary electrons affects the spin transport with a larger time of propagation of homogeneous spin polarization.

cond-mat.mtrl-sci↗

arXiv2021

Influence of an external electric field on the energy dissipation at the initial stage of laser ablation

A density-dependent two-temperature model is applied to describe laser excitation and the following relaxation processes of silicon in an external electric field. Two approaches on how to describe the effects of the external electric field are presented. The first approach avoids the buildup of internal electric fields due to charge separation by assuming ambipolar diffusion and adds an additional carrier-pair current. In the second approach, electrons and holes are treated separately to account for charge separation and the resulting shielding of the external electric field inside the material. The two approaches are compared to experimental results. Both the first approach and the experimental results show similar tendencies for optimization of laser ablation in the external electric field.

physics.optics↗

arXiv2021

Magnetic-field assisted laser ablation of silicon

Understanding and manipulation of the laser processing quality during the ablation of solids have crucial importance from fundamental and industrial perspectives. Here we have studied the effect of external magnetic field on the micro-material processing of silicon by ultrashort laser pulses. It was found experimentally that such a field directed along the laser beam improves the quality and efficiency of the material removal. Additionally, we observe that the formation of laser-induced periodic surface structures (LIPSS) in a multi-pulse regime is affected by the external magnetic field. Our results open a route towards efficient and controllable ultrafast laser micromachining.

physics.optics↗

arXiv2021

Plasmonic nature of periodic surface structures following single laser pulse irradiation

Understanding the mechanisms and controlling the possibilities of surface nanostructuring is of crucial interest from fundamental and practical perspectives. Here we report a direct experimental observation of laser-induced periodic surface structures (LIPSS) formed near a predesigned gold step edge following single-pulse femtosecond laser irradiation. A hybrid atomistic-continuum model fully supports experimental observations. We identify two key components of single-pulse LIPSS formation: excitation of surface plasmon polaritons and material reorganization. Our results lay the foundation towards simple and efficient single laser pulse micromachining.

physics.optics↗

arXiv2019

Influence of surface plasmon polaritons on laser energy absorption and structuring of surfaces

The accurate calculation of laser energy absorption during femto- or picosecond laser pulse experiments is very important for the description of the formation of periodic surface structures. On a rough material surface, a crack or a step edge, ultrashort laser pulses can excite surface plasmon polaritons (SPP), i.e. surface plasmons coupled to a laser-electromagnetic wave. The interference of such plasmon wave and the incoming pulse leads to a periodic modulation of the deposited laser energy on the surface of the sample. In the present work, within the frames of a Two Temperature Model we propose the analytical form of the source term, which takes into account SPP excited at a step edge of a dielectric-metal interface upon irradiation of an ultrashort laser pulse at normal incidence. The influence of the laser pulse parameters on energy absorption is quantified for the example of gold. This result can be used for nanophotonic applications and for the theoretical investigation of the evolution of electronic and lattice temperatures and, therefore, of the formation of surfaces with predestined properties under controlled conditions.

physics.app-ph↗

arXiv2018

Wavelength-dependent reflectivity changes on gold at elevated electronic temperatures

Upon the excitation by an ultrashort laser pulse the conditions in a material can drastically change, altering its optical properties and therefore the relative amount of absorbed energy, a quan- tity relevant for determining the damage threshold and for developing a detailed simulation of a structuring process. The subject of interest in this work is the d-band metal gold which has an absorption edge marking the transition of free valence electrons and an absorbing deep d-band with bound electrons. Reflectivity changes are observed in experiment over a broad spectral range at ablation conditions. To understand the involved processes the laser excitation is modeled by a com- bination of first principle calculations with a two-temperature model. The description is kept most general and applied to realistically simulate the transfer of the absorbed energy of a Gaussian laser pulse into the electronic system at every point in space at every instance of time. An electronic temperature-dependent reflectivity map is calculated, describing the out of equilibrium reflectivity during laser excitation for photon energies from 0.9 - 6.4 eV, including inter- and intra-band transi- tions and a temperature-dependent damping factor. The main mechanisms are identified explaining the electronic temperature-dependent change in reflectivity: broadening of the edge of the occu- pied/unoccupied states around the chemical potential $\mu$, also leading to a shift of the $\mu$ and an increase of the collision rate of free s/p-band electrons with bound d-band holes.

cond-mat.mtrl-sci↗

arXiv2017

Femtosecond formation dynamics of the spin Seebeck effect revealed by terahertz spectroscopy

Understanding the transfer of spin angular momentum is essential in modern magnetism research. A model case is the generation of magnons in magnetic insulators by heating an adjacent metal film. Here, we reveal the initial steps of this spin Seebeck effect with <27fs time resolution using terahertz spectroscopy on bilayers of ferrimagnetic yttrium-iron garnet and platinum. Upon exciting the metal with an infrared laser pulse, a spin Seebeck current $j_\textrm{s}$ arises on the same ~100fs time scale on which the metal electrons thermalize. This observation highlights that efficient spin transfer critically relies on carrier multiplication and is driven by conduction electrons scattering off the metal-insulator interface. Analytical modeling shows that the electrons' dynamics are almost instantaneously imprinted onto $j_\textrm{s}$ because their spins have a correlation time of only ~4fs and deflect the ferrimagnetic moments without inertia. Applications in material characterization, interface probing, spin-noise spectroscopy and terahertz spin pumping emerge.

cond-mat.mes-hall↗

arXiv2015

Semi-implicit finite-difference method with predictor-corrector algorithm for solution of diffusion equation with nonlinear terms

We present a finite-difference integration algorithm for solution of a system of differential equations containing a diffusion equation with nonlinear terms. The approach is based on Crank-Nicolson method with predictor-corrector algorithm and provides high stability and precision. Using a specific example of short-pulse laser interaction with semiconductors, we give a detailed description of the method and apply it for the solution of the corresponding system of differential equations, one of which is a nonlinear diffusion equation. The calculated dynamics of the energy density and the number density of photoexcited free carriers upon the absorption of laser energy are presented for the irradiated thin silicon film. The energy conservation within 0.2% has been achieved for the time step $10^4$ times larger than that in case of the explicit scheme, for the chosen numerical setup. We also present a few examples of successful application of the method demonstrating its benefits for the theoretical studies of laser-matter interaction problems.

physics.comp-ph↗

arXiv2014

Atomistic-continuum modeling of short laser pulse melting of Si targets

We present an atomistic-continuum model to simulate ultrashort laser-induced melting processes in semiconductor solids on the example of silicon. The kinetics of transient non-equilibrium phase transition mechanisms is addressed with a Molecular Dynamics method at atomic level, whereas the laser light absorption, strong generated electron-phonon non-equilibrium, fast diffusion and heat conduction due to photo-excited free carriers are accounted for in the continuum. We give a detailed description of the model, which is then applied to study the mechanism of short laser pulse melting of free standing Si films. The effect of laser-induced pressure and temperature of the lattice on the melting kinetics is investigated. Two competing melting mechanisms, heterogeneous and homogeneous, were identified. Apart of classical heterogeneous melting mechanism, the nucleation of the liquid phase homogeneously inside the material significantly contributes to the melting process. The simulations showed, that due to the open diamond structure of the crystal, the laser-generated internal compressive stresses reduce the crystal stability against the homogeneous melting. Consequently, the latter can take a massive character within several picoseconds upon the laser heating. Due to negative volume of melting of modeled Si material, -7.5%, the material contracts upon the phase transition, relaxes the compressive stresses and the subsequent melting proceeds heterogeneously until the excess of thermal energy is consumed. The threshold fluence value, at which homogeneous nucleation of liquid starts contributing to the classical heterogeneous propagation of the solid-liquid interface, is found from the series of simulations at different laser input fluences. On the example of Si, the laser melting kinetics of semiconductors was found to be noticeably different from that of metals with fcc crystal structure.

cond-mat.mtrl-sci↗

arXiv2014

Laser damage in silicon: energy absorption, relaxation and transport

Silicon irradiated with an ultrashort 800 nm-laser pulse is studied theoretically using a two temperature description that considers the transient free carrier density during and after irradiation. A Drude model is implemented to account for the highly transient optical parameters. We analyze the importance of considering these density-dependent parameters as well as the choice of the Drude collision frequency. In addition, degeneracy and transport effects are investigated. The importance of each of these processes for resulting calculated damage thresholds is studied.We report damage thresholds calculations that are in very good agreement with experimental results over a wide range of pulse durations.

cond-mat.mes-hall↗

arXiv2014

Driving ferromagnets into a critical region of a magnetic phase diagram

Exciting a ferromagnetic sample with an ultrashort laser pulse leads to a quenching of the magne- tization on a subpicosecond timescale. On the basis of the equilibration of intensive thermodynamic variables we establish a powerful model to describe the demagnetization dynamics. We demonstrate that the magnetization dynamics is mainly driven by the equilibration of chemical potentials. The minimum of magnetization is revealed as a transient electronic equilibrium state. Our method iden- tifies the slowing down of ultrafast magnetization dynamics by a critical region within a magnetic phase diagram.

cond-mat.mtrl-sci↗

arXiv2011

Driving Force of Ultrafast Magnetization Dynamics

Irradiating a ferromagnetic material with an ultrashort laser pulse leads to demagnetization on a femtosecond timescale. We implement Elliott-Yafet type spin-flip scattering, mediated by electron-electron and electron-phonon collisions, into the framework of a spin-resolved Boltzmann equation. Considering three mutually coupled reservoirs, (i) spin-up electrons, (ii) spin-down electrons and (iii) phonons, we trace non-equilibrium electron distributions during and after laser excitation. We identify the driving force for ultrafast magnetization dynamics as the equilibration of temperatures and chemical potentials between the electronic subsystems. This principle can be used to easily predict the maximum quenching of magnetization upon ultrashort laser irradiation in any material, as we show for the example of 3d-ferromagnetic nickel.

cond-mat.mtrl-sci↗