arXiv subjects

Matias Bargheer

Publications and source records attributed to Matias Bargheer.

At least 19 recordsLinked to original sources

arXiv2026

Spin waves excited by hard x-ray transient gratings

Recent progress in ultrafast x-ray sources helped establish x-rays as an important tool for probing lattice and magnetic dynamics initiated by femtosecond optical pulses. Here, we explore the potential of ultrashort hard x-ray pulses for driving magnetic dynamics. We use a transient grating technique in which a spatially periodic x-ray excitation pattern gives rise to material excitations at a well-defined wave vector, whose dynamics are monitored via diffraction of an optical probe pulse. The excitation of a ferrimagnetic gadolinium bismuth iron garnet film placed in an external tilted magnetic field by x-rays at the Gd L3 edge results in both magnetic and non-magnetic transient gratings whose contributions to the diffracted signal are separated by polarization analysis. We observe the magnetization precession at both longitudinal acoustic and spin wave frequencies. An analysis with the Landau-Lifshitz-Gilbert equation indicates that the magnetization precession is driven by strain resulting from thermal expansion induced by absorbed x-rays. The results establish x-ray transient gratings as a tool for driving coherent phonons and magnons, with the potential of accessing wave vectors across the entire Brillouin zone.

physics.optics↗

arXiv2025

Experimental evidence of dominant ultrafast diffusive energy transport by hot electrons in Cu

When the dimensions of structures shrink to the order of the inelastic mean free path of the energy-carrying quasi-particles, the character of energy transport changes from diffusive to ballistic. However, the point of transition remains a matter of debate. Here, we determine the dominant channel of energy transport through a nanoscale Cu layer as a function of its thickness. The energy rapidly transferred across Cu via hot electrons from a photo-excited Pt layer into a buried Ni detection layer translates into a rapid expansion of the Ni layer probed via ultrafast x-ray diffraction. The non-linear dependence of the Ni strain amplitude on the absorbed laser fluence indicates that the transport through Cu becomes more efficient with increasing fluence. This fluence-dependent transport efficiency is reproduced by a diffusive energy transport model and serves as a generally applicable experimental approach to distinguish diffusion from ballistic transport. Following this approach, we identify diffusive electronic energy transport to govern the spatial energy distribution for Cu layer thicknesses larger than twice the electronic inelastic mean free path.

cond-mat.mtrl-sci↗

arXiv2025

Intrinsic non-Markovian magnetisation dynamics

Memory effects arise in many complex systems, from protein folding, to the spreading of epidemics and financial decisions. While so-called non-Markovian dynamics is common in larger systems with interacting components, observations in fundamental physical systems have been confined to specifically engineered cases. Here, we report the experimental observation of non-Markovian dynamics in an elemental material, crystalline cobalt. By driving this material with an intense terahertz electromagnetic field, we bring its magnetisation into a non-equilibrium state and follow its evolution. We measure the sample's low temperature magnetic response in the time domain which leads to an unexpectedly rich multi-peaked spectrum in the Fourier domain, that cannot be explained by established models. We use open quantum system theory, which predicts a non-Markovian memory kernel in the dynamical equations to capture the fundamental interaction between the spin system and the phonon bath. Simulations based on this theory produce a multi-peaked spectrum, which matches the measured one. Our non-Markovian approach is also able to reproduce the modification of the spectrum at higher temperatures. Our findings demonstrate that non-Markovian effects are observable at a much more fundamental level than previously thought, opening the door to their exploration and control in a broad range of condensed matter systems.

quant-ph↗

arXiv2025

Rapid heat assisted polarization reversal in ferroelectric thin films

We demonstrate that switching of ferroelectric thin-films sandwiched between metallic electrodes can be controlled by laser-assisted heating, reminiscent of heat-assisted magnetic recording. We employ electrical switching cycles that quantify the electrically switchable remanent polarization $P_\mathrm{r}$ and show that 300\,ns voltage pulses alone change the polarization by less than $ΔP P_\mathrm{r}$ of the average polarization. The transient average temperature modeled by the heat equation can rationalize the polarization change observed for different relative timing $Δt$ of the laser pulse, if it arrives before the electrical pulse.

cond-mat.mtrl-sci↗

arXiv2025

Atomistic spin dynamics with quantum colored noise

The accurate prediction of temperature-dependent magnetization dynamics is a fundamental challenge in computational magnetism. While Atomistic Spin Dynamics (ASD) simulations have emerged as a powerful tool for studying magnetic phenomena, their classical nature leads to significant deviations from experimental observations, particularly at low temperatures. Here we present a comprehensive implementation of quantum-corrected ASD into the Vampire software package, based on the open-system Landau-Lifshitz-Gilbert equation with a quantum thermostat. Our implementation incorporates memory effects along with colored noise derived from quantum-mechanical considerations that improve the description of the equilibrium magnetization. We demonstrate excellent quantitative agreement with experimental magnetization curves for nickel and gadolinium across the full temperature range. Our results establish that incorporating quantum environmental effects and colored noise substantially enhances the predictive capabilities of ASD simulations, providing a robust framework for modeling temperature-dependent magnetic phenomena in localized moment magnetic systems.

cond-mat.mtrl-sci↗

arXiv2025

Non-thermal electrons open the non-equilibrium pathway of the phase transition in FeRh

We use ultrafast x-ray diffraction to study non-equilibrium pathways of the phase transition in FeRh parametrized by the structural response. By increasing the pump-pulse duration beyond the electron-phonon coupling time, we suppress the electron-phonon non-equilibrium present upon femtosecond laser excitation but still photoexcite electrons to non-thermal states. Irrespective of the pump pulse duration, we find an optically induced nucleation of ferromagnetic domains on an $8\,\text{ps}$ timescale that starts as soon as the successively deposited energy surpasses the site-specific threshold energy. If in contrast, FeRh is only indirectly excited by diffusion of thermalized electrons from an opaque Pt cap layer, the ferromagnetic phase rises on a $50\,\text{ps}$ timescale. These findings unambiguously identify the photo-excitation of non-thermal electrons and not electron-phonon non-equilibria to enable the non-equilibrium pathway of the phase transition in FeRh.

cond-mat.mtrl-sci↗

arXiv2025

Inverted Temperature Gradients in Gold-Palladium Antenna-Reactor Nanoparticles

In addition to enhanced fields and possible charge transfer, the concentration of photothermal energy at the nanoscale is a foundation of plasmon-driven photochemistry. We demonstrate a further enhancement of heat localization during the dissipation of energy in a bimetallic antenna--reactor system with palladium satellites attached to a gold nanoparticle. After pulsed excitation of the gold core, the satellites collect nearly all photothermal energy and heat up by 180\,K while the light-absorbing gold core remains much colder. By comparing transient absorption dynamics of a series of bimetallic nanoparticles with a three-temperature model, we can precisely assess the temperatures of the electronic and vibrational subsystems. We find a strong inverted temperature gradient that opposes the direction of energy input and concentrates the light energy at the active catalytic nanosite.

cond-mat.soft↗

arXiv2024

Unveiling the nanomorphology of HfN thin films by ultrafast reciprocal space mapping

Hafnium Nitride (HfN) is a promising and very robust alternative to gold for applications of nanoscale metals. Details of the nanomorphology related to variations in strain states and optical properties can be crucial for applications in nanophotonics and plasmon-assisted chemistry. We use ultrafast reciprocal space mapping (URSM) with hard x-rays to unveil the nanomorphology of thin HfN films. Static high-resolution x-ray diffraction reveals a twofold composition of the thin films being separated into regions with identical lattice constant and similar out-of-plane but hugely different in-plane coherence lengths. URSM upon femtosecond laser excitation reveals different transient strain dynamics for the two respective Bragg peak components. This unambiguously locates the longer in-plane coherence length in the first 15\,nm of the thin film adjacent to the substrate. The transient shift of the broad diffraction peak displays the strain dynamics of the entire film, implying that the near-substrate region hosts nanocrystallites with small and large coherence length, whereas the upper part of the film grows in small columnar grains. Our results illustrate that URSM is a suitable technique for non-destructive investigations of the depth-resolved nanomorphology of nanostructures.

cond-mat.mtrl-sci↗

arXiv2024

Accelerating the laser-induced phase transition in nanostructured FeRh via plasmonic absorption

By ultrafast x-ray diffraction we show that the laser-induced magnetostructural phase transition in FeRh nanoislands proceeds faster and more complete than in continuous films. We observe an intrinsic 8 ps timescale for nucleation of ferromagnetic (FM) domains in both types of samples. For the continuous film, the substrate-near regions, which are not directly exposed to light, are only slowly transformed to the FM state by domain wall motion following heat transport. In contrast, numerical modeling of the plasmonic absorption in the investigated nanostructure reveals a strong contribution near the FeRh/MgO interface. On average, the absorption is larger and more homogeneous in the nanoislands, enabling the phase transition throughout the entire volume at the intrinsic nucleation timescale.

cond-mat.mtrl-sci↗

arXiv2024

Controlling effective field contributions to laser-induced magnetization precession by heterostructure design

Nanoscale heterostructure design can control laser-induced heat dissipation and strain propagation as well as their efficiency for driving magnetization precession. We use insulating MgO layers incorporated into metallic Pt-Cu-Ni heterostructures to block the propagation of hot electrons. Ultrafast x-ray diffraction (UXRD) experiments quantify how this enables controlling the spatio-temporal shape of the transient heat and strain, which drive the magnetization dynamics in the Ni layer. The frequency of the magnetization precession observed by the time-resolved magneto-optical Kerr effect (MOKE) in polar geometry is systematically tuned by the magnetic field orientation. The combined experimental analysis (UXRD and MOKE) and modeling of transient strain, heat and magnetization uniquely highlights the importance of quasi-static strain as a driver of precession, when the magnetic material is rapidly heated via electrons. The concomitant effective field change originating from demagnetization partially compensates the change induced by quasi-static strain. Tailored strain pulses shaped via the nanoscale heterostructure design provide an equally efficient, phase-matched driver of precession, paving the way for opto-magneto-acoustic devices with low heat energy deposited in the magnetic layer.

cond-mat.mtrl-sci↗

arXiv2024

Speed limits of the laser-induced phase transition in FeRh

We use ultrafast x-ray diffraction (UXRD) and the polar time-resolved magneto-optical Kerr effect (tr-MOKE) to study the laser-induced metamagnetic phase transition in two FeRh films with thicknesses below and above the optical penetration depth. In the thin film, we identify an intrinsic timescale for the light-induced nucleation of ferromagnetic (FM) domains in the antiferromagnetic material of $8\,\text{ps}$ that is substantially slower than the speed of sound. For the inhomogeneously excited thicker film, only the optically excited near-surface part transforms within $8\,\text{ps}$. For strong excitations we observe an additional slow rise of the FM phase, which we experimentally relate to a growth of the FM phase into the depth of the layer by comparing the transient magnetization in front- and backside excitation geometry. In the lower lying parts of the film, which are only excited via near-equilibrium heat transport, the FM phase emerges significantly slower than $8\,\text{ps}$ after heating above the transition temperature.

cond-mat.mtrl-sci↗

arXiv2023

Optical Non-linearities in Plasmon-Exciton Core-Shell Particles: the Role of Heat

Strong coupling between plasmons and excitons gives rise to new hybrid polariton states with various fields of potential applications. Despite a plethora of research on plasmon--exciton systems, their transient behaviour is not yet fully understood. Besides Rabi oscillations in the first femtoseconds after an optical excitation, coupled systems show interesting non-linear features on the picosecond time scale. Here, we conclusively show that the source of these features is heat that is generated inside the particles. Until now, this hypothesis was only based on phenomenological arguments. We investigate the role of heat by recording transient spectra of plasmon--exciton core--shell nanoparticles with excitation off the polariton resonance. We present analytical simulations that precisely recreate the measurements solely by assuming an initial temperature rise of the electron gas inside the particles. The simulations combine established strategies for describing uncoupled plasmonic particles with a recently published model for static spectra. The simulations are consistent for various excitation powers confirming that indeed heating of the particles is the root of the changes in the transient signals.

physics.optics↗

arXiv2023

Concepts and use cases for picosecond ultrasonics with x-rays

This review discusses picosecond ultrasonics experiments using ultrashort hard x-ray probe pulses to extract the transient strain response of laser-excited nanoscopic structures from Bragg-peak shifts. This method provides direct, layer-specific, and quantitative information on the picosecond strain response for structures down to few-nm thickness. We model the transient strain using the elastic wave equation and express the driving stress using Grüneisen parameters stating that the laser-induced stress is proportional to energy density changes in the microscopic subsystems of the solid, i.e., electrons, phonons and spins. The laser-driven strain response can thus serve as an ultrafast proxy for local energy-density and temperature changes, but we emphasize the importance of the nanoscale morphology for an accurate interpretation due to the Poisson effect. The presented experimental use cases encompass ultrathin and opaque metal heterostructures, continuous and granular nanolayers as well as negative thermal expansion materials, that each pose a challenge to established all-optical techniques.

cond-mat.mtrl-sci↗

arXiv2022

Standing spin wave excitation in Bi:YIG films via temperature induced anisotropy changes and magnetoacoustic coupling

Based on micromagnetic simulations and experimental observations of the magnetization and lattice dynamics following the direct optical excitation of the magnetic insulator Bi:YIG or indirect excitation via an optically opaque Pt/Cu double layer, we disentangle the dynamical effects of magnetic anisotropy and magnetoelastic coupling. The strain and temperature of the lattice are quantified via modeling ultrafast x-ray diffraction data. Measurements of the time-resolved magneto-optical Kerr effect agree well with the magnetization dynamics simulated according to the excitation via two mechanisms: The magneto-acoustic coupling to the experimentally verified strain dynamics and the ultrafast temperature-induced transient change in the magnetic anisotropy. The numerical modeling proves that for direct excitation both mechanisms drive the fundamental mode with opposite phase. The relative ratio of standing spin-wave amplitudes of higher order modes indicates that both mechanisms are substantially active.

cond-mat.other↗

arXiv2020

Vacuum-Induced Saturation in Plasmonic Nanoparticles

Vacuum fluctuations are a fundamental feature of quantized fields. It is usually assumed that observations connected to vacuum fluctuations require a system well isolated from other influences. In this work, we demonstrate that effects of the quantum vacuum can already occur in simple colloidal nano-assemblies prepared by wet chemistry. We claim that the electromagnetic field fluctuations at the zero-point level saturate the absorption of dye molecules self-assembled at the surface of plasmonic nano-resonators. For this effect to occur, reaching the strong coupling regime between the plasmons and excitons is not required. This intriguing effect of vacuum-induced saturation (VISA) is discussed within a simple quantum optics picture and demonstrated by comparing the optical spectra of hybrid gold-core dye-shell nanorods to electromagnetic simulations.

physics.optics↗

arXiv2018

Critical behavior of the damping rate of GHz acoustic phonons in SrTiO3 at the antiferrodistortive phase transition measured by time- and frequency-resolved Brillouin scattering

We determine the temperature dependent damping rate of longitudinal acoustic phonons in SrTiO3 using frequency domain Brillouin scattering and time domain Brillouin scattering. We investigate samples with (La,Sr)MnO3 and SrRuO3 capping layers, which result in compressive or tensile strain at the layer - substrate interface, respectively. The different strain states lead to dif- ferent domain structures in SrTiO3 that extend into the bulk of the SrTiO3 substrates and strongly affect the phonon propagation. Our experiments show that the damping rate of acoustic phonons in the interfacial STO layer depends strongly on the sample temperature and strain induced do- main structure. We also show that the damping rate as function of temperature exhibits a critical behavior close to the cubic-to-tetragonal phase transition of SrTiO3.

cond-mat.mtrl-sci↗

arXiv2017

Quantitative disentanglement of coherent and incoherent laser-induced surface deformations by time-resolved x-ray reflectivity

We present time-resolved x-ray reflectivity measurements on laser excited coherent and incoherent surface deformations of thin metallic films. Based on a kinematical diffraction model, we derive the surface amplitude from the diffracted x-ray intensity and resolve transient surface excursions with sub-Angstrom spatial precision and 70 ps temporal resolution. The novel analysis allows for decomposition of the surface amplitude into multiple coherent acoustic modes and a substantial contribution from incoherent phonons which constitute the sample heating.

cond-mat.mtrl-sci↗

arXiv2017

Spatio-temporal coherent control of thermal excitations in solids

X-ray reflectivity (XRR) measurements of femtosecond laser-induced transient gratings are applied to demonstrate the spatio-temporal coherent control of thermally induced surface deformations on ultrafast timescales. Using gracing incidence X-ray diffraction we unambiguously measure the amplitude of transient surface deformations with sub-Å resolution. Understanding the dynamics of femtosecond TG excitations in terms of superposition of acoustic and thermal gratings makes it possible to develop new ways of coherent control in X-ray diffraction experiments. Being the dominant source of TG signal, the long-living thermal grating with spatial period $Λ$ can be canceled by a second, time-delayed TG excitation shifted by $Λ/2$. The ultimate speed limits of such an ultrafast X-ray shutter are inferred from the detailed analysis of thermal and acoustic dynamics in TG experiments.

cond-mat.mtrl-sci↗