arXiv subjects

Andreas Scherz

Publications and source records attributed to Andreas Scherz.

At least 19 recordsLinked to original sources

arXiv2025

Picosecond localization dynamics following ultrafast nanoscale magnetic switching

Ultrashort laser pulses provide the fastest known way to switch magnetic order. Such excitation commonly creates nanometer-scale domains, even after homogeneous illumination when the position of nucleated domains is not externally defined. However, the physics of domain localization during such ultrafast phase transitions remains unresolved. Here, we use shot-resolved pump-probe resonant x-ray scattering together with a material featuring a periodically modulated magnetic anisotropy landscape to track, in real time, the laser-driven nucleation and localization of nanometer-scale spin textures. We find that nucleation and localization are two distinct processes. Nucleation occurs homogeneously via fluctuations at early times, whereas spatially periodic structures emerge only later and, under suitable conditions, localize in less than one nanosecond. Real-space simulations show that this localization is governed by strong lateral variations in spin-texture lifetimes. Our results demonstrate that ultrafast phase-transition dynamics fundamentally differ from conventional transitions, yet still can be controlled through moderate nanometer-scale tailoring of the energy landscape.

cond-mat.mes-hall↗

arXiv2025

Collective Magnetic Excitations in a Photo-excited Electron-doped Cuprate Superconductor

Elucidating the microscopic behavior of cuprates under ultrafast photoexcitation offers critical insights into their highly correlated out-of-equilibrium states. Although quasiparticle dynamics have been investigated extensively, the behavior of collective magnetic excitations remains comparatively unexplored. Here, we use time-resolved resonant inelastic X-ray scattering (trRIXS) at the Cu $L_3$-edge to track the collective magnetic excitations (paramagnons) in an optimally electron-doped cuprate driven out-of-equilibrium by a femtosecond pump laser pulse. Upon pumping, we observed an anti-Stokes signal associated with paramagnon generation, which modifies the paramagnon dispersion near the zone center, although the bandwidth remained unchanged. Moreover, the spectral weight exhibits a momentum-dependent variation across the Brillouin zone. The light-driven boost of the paramagnon population and the resulting spectral-weight transfer could provide new leverage to manipulate the properties of cuprates.

cond-mat.mtrl-sci↗

arXiv2025

High frame rate RIXS spectroscopy using a JUNGFRAU detector with an iLGAD sensor

Resonant inelastic X-ray scattering (RIXS) is a powerful photon-in, photon-out spectroscopy technique for probing electronic, magnetic, and lattice excitations in matter. Time-resolved RIXS extends this capability through a stroboscopic optical pump-probe scheme to characterize the time evolution of the photoexcitation and subsequent relaxation dynamics of a sample. This technique is, however, extremely photon-hungry, requiring high-repetition-rate and intense X-ray facilities. The Heisenberg RIXS (hRIXS) spectrometer at the Spectroscopy and Coherent Scattering (SCS) instrument of the European X-ray Free-Electron Laser (EuXFEL) is designed to exploit high-repetition-rates, while maintaining optimal time and energy resolution. In this work, we demonstrate the successful deployment of a JUNGFRAU detector equipped with an inverse Low Gain Avalanche Diode (iLGAD) sensor for time-resolved RIXS studies in the soft X-ray range, using the hRIXS spectrometer. A spatial resolution of $19.71 \pm 0.7~\mu\mathrm{m}$ and a resolving power exceeding 10,000 were achieved at an unprecedented frame rate of 47 kHz. Intra-train resolved data measured with a high FEL peak fluence of $1.8~\mathrm{mJ/cm^{2}}$ for a 928.5 eV ph photon energy and 1.1 MHz repetition rate from cupric oxide (CuO) revealed a decrease in the emitted signal by ~10% over a time interval of $340~\mu\mathrm{s}$, indicating FEL-induced effects that require monitoring when conducting high-repetition-rate experiments. These results establish the JUNGFRAU-iLGAD as a promising detector to harvest the full potential of the hRIXS spectrometer, and validate its suitability for soft X-ray applications.

physics.ins-det↗

arXiv2025

Anomalous spin dynamics after dual optical excitation

Ultrashort optical pulses are a cornerstone for manipulating electronic and magnetic states in materials on a femtosecond timescale. Conventional models assume that optical excitation primarily modifies the occupation of the electron energy levels without long-lasting altering of the coupling of individual electrons in certain processes. Here, we demonstrate that optical excitation with two femtosecond pulses that come from different directions fundamentally transforms the electron dynamics in copper, affecting the efficiency of angular momentum transfer between electrons and the lattice. Using time-resolved magneto-optical Kerr effect measurements, we reveal a ~2.5. increase in spin imbalance decay time following inverse Faraday effect excitation under dual-pump conditions compared to single-pulse excitation. This observation challenges the prevailing paradigm of ultrafast light-matter interactions, showing that dual optical excitation can transiently modify electron dynamics beyond simple changes in the energy levels occupancy. Our findings open new avenues for controlling quantum states through a dual pump approach, with implications for ultrafast spintronics and the design of novel light-driven states.

cond-mat.mtrl-sci↗

arXiv2025

Photo-generated charge-transfer excitons in NiO revealed by ultrafast time-resolved resonant inelastic x-ray scattering

Strong electronic correlation can lead to insulating behavior and to the opening of large optical gaps, even in materials with partly filled valence shells. Although the non-equilibrium optical response encodes both local (quasi atomic) and collective (long range) responses, optical spectroscopy is usually more sensitive to the latter. Resonant x-ray techniques are better suited to investigate the quasi-atomic properties of correlated solids. Using time-resolved resonant inelastic x-ray scattering (RIXS), here we study the ultrafast non-equilibrium processes in NiO following photo-excitation by ultraviolet photons with energy exceeding the optical gap. We observe the creation of charge-transfer excitons that decay with a time constant of about 2\,ps, while itinerant photo-doping persists for tens of picoseconds. Following our discovery, which establishes time-resolved high-resolution RIXS as a powerful tool for the study of transient phenomena in condensed matter, the possible presence of charge-transfer excitons will need to be considered when interpreting optical pump-probe experiments on correlated quantum materials.

cond-mat.str-el↗

arXiv2025

Ultrafast decoupling of polarization and strain in ferroelectric BaTiO$_3$

A fundamental understanding of the interplay between lattice structure, polarization and electrons is pivotal to the optical control of ferroelectrics. The interaction between light and matter enables the remote and wireless control of the ferroelectric polarization on the picosecond timescale, while inducing strain, i.e., lattice deformation. At equilibrium, the ferroelectric polarization is proportional to the strain, and is typically assumed to be so also out of equilibrium. Decoupling the polarization from the strain would remove the constraint of sample design and provide an effective knob to manipulate the polarization by light. Here, upon an above-bandgap laser excitation of the prototypical ferroelectric BaTiO$_3$, we induce and measure an ultrafast decoupling between polarization and strain that begins within 350 fs, by softening Ti-O bonds via charge transfer, and lasts for several tens of picoseconds. We show that the ferroelectric polarization out of equilibrium is mainly determined by photoexcited electrons, instead of the strain. This excited state could serve as a starting point to achieve stable and reversible polarization switching via THz light. Our results demonstrate a light-induced transient and reversible control of the ferroelectric polarization and offer a pathway to control by light both electric and magnetic degrees of freedom in multiferroics.

cond-mat.mtrl-sci↗

arXiv2024

Analysis of long-lived effects in high-repetition-rate stroboscopic transient X-ray absorption experiments on thin films

Time-resolved X-ray absorption spectroscopy (tr-XAS) has been shown to be a versatile measurement technique for investigating non-equilibrium dynamics. Novel X-ray free electron laser (XFEL) facilities like the European XFEL offer increased repetition rates for stroboscopic XAS experiments through a burst operation mode, which enables measurements with up to 4.5 MHz. These higher repetition rates lead to higher data acquisition rates but can also introduce long-lived excitations that persist and thus build up during each burst. Here, we report on such long-lived effects in Ni and NiO thin film samples that were measured at the European XFEL. We disentangle the long-lived excitations from the initial pump-induced change and perform a detailed modelling-based analysis of how they modify transient X-ray spectra. As a result, we link the long-lived effects in Ni to a local temperature increase, as well as the effects in NiO to excited charge carrier trapping through polaron formation. In addition, we present possible correction methods, as well as discuss ways in which the effects of these long-lived excitations could be minimized for future time-resolved X-ray absorption spectroscopy measurements.

cond-mat.mtrl-sci↗

arXiv2024

Demagnetization dynamics after noncollinear dual optical excitation

We explore the impact of optical excitation using two interfering ultrashort optical pulses on ultrafast magnetization dynamics. Our investigation focuses on Pt/Co/Pt multilayers and TbCo alloy samples, employing a dual pump approach. We observe significant variations in the dynamics of magnetization suppression and subsequent recovery when triggered with two optical pulses of the same polarization-essentially meeting conditions for interference. Conversely, dynamics triggered with cross-polarized pump beams exhibit expected similarity to that triggered with a single pulse. Delving into the underlying physical processes contributing to laser-induced demagnetization and recovery dynamics, we find that our current understanding cannot elucidate the observed trends. Consequently, we propose that optical excitation with interfering light possesses not previously acknowledged capacity to induce long-lasting alterations in the dynamics of angular momentum.

physics.optics↗

arXiv2024

The Heisenberg-RIXS instrument at the European XFEL

Resonant Inelastic X-ray Scattering (RIXS) is an ideal X-ray spectroscopy method to push the combination of energy and time resolutions to the Fourier transform ultimate limit, because it is unaffected by the core-hole lifetime energy broadening. And in pump-probe experiments the interaction time is made very short by the same core-hole lifetime. RIXS is very photon hungry so it takes great advantage from high repetition rate pulsed X-ray sources like the European XFEL. The hRIXS instrument is designed for RIXS experiments in the soft X-ray range with energy resolution approaching the Fourier and the Heisenberg limits. It is based on a spherical grating with variable line spacing (VLS) and a position-sensitive 2D detector. Initially, two gratings are installed to adequately cover the whole photon energy range. With optimized spot size on the sample and small pixel detector the energy resolution can be better than 40 meV at any photon energy below 1000 eV. At the SCS instrument of the European XFEL the spectrometer can be easily positioned thanks to air-pads on a high-quality floor, allowing the scattering angle to be continuously adjusted over the 65-145 deg range. It can be coupled to two different sample interaction chamber, one for liquid jets and one for solids, each equipped at the state-of-the-art and compatible for optical laser pumping in collinear geometry. The measured performances, in terms of energy resolution and count rate on the detector, closely match design expectations. hRIXS is open to public users since the summer of 2022.

cond-mat.str-el↗

arXiv2023

Magnetization precession after non-collinear dual optical excitation

We investigate the impact of non-collinear dual optical excitation on the magnetization precession in a permalloy thin film using two ultrashort laser pulses. By analyzing the magnetization dynamics using time-resolved magneto-optical methods, we find that the excitation with two ultrashort optical pulses introduces a long-lasting modification of the electron system seen as a sizable decrease of the precession frequency and significant increase (about 25%) of the decay time. Our results reveal that the observed effect strongly depends on the respective polarization of the two excitation pulses and the time delay between two optical pulses. Our findings indicate the occurrence of a new nonlinear opto-spin effect during photoexcitation with two interfering optical pulses which can potentially be observed in various materials and at different photon wavelengths.

cond-mat.mtrl-sci↗

arXiv2023

Femtosecond spin-state switching dynamics of spin-crossover molecules condensed in thin films

The photoinduced switching of Fe(II)-based spin-crossover complexes from singlet to quintet takes place at ultrafast time scales. This a priori spin-forbidden transition triggered numerous time-resolved experiments of solvated samples to elucidate the mechanism at play. The involved intermediate states remain uncertain. We apply ultrafast x-ray spectroscopy in molecular films as a method sensitive to spin, electronic, and nuclear degrees of freedom. Combining the progress in molecule synthesis and film growth with the opportunities at x-ray free-electron lasers, we analyze the transient evolution of the Fe L3 fine structure at room temperature. Our measurements and calculations indicate the involvement of an Fe triplet intermediate state. The high-spin state saturates at half of the available molecules, limited by molecule-molecule interaction within the film.

cond-mat.mes-hall↗

arXiv2023

Optically Induced Ferromagnetic Order in a Ferrimagnet

The parallel or antiparallel arrangement of electron spins plays a pivotal role in determining the properties of a physical system. To meet the demands for innovative technological solutions, extensive efforts have been dedicated to exploring effective methods for controlling and manipulating this arrangement [1]. Among various techniques, ultrashort laser pulses have emerged as an exceptionally efficient tool to influence magnetic order. Ultrafast suppression of the magnetic order [2,3], all-optical magnetization switching [4, 5, 6, 7], and light-induced magnetic phase transitions [8] are just a few notable examples. However, the transient nature of light-induced changes in the magnetic state has been a significant limitation, hindering their practical implementation. In this study, we demonstrate that infrared ultrashort laser pulses can induce a ferromagnetic arrangement of magnetic moments in an amorphous TbCo alloy, a material that exhibits ferrimagnetism under equilibrium conditions. Strikingly, the observed changes in the magnetic properties persist for significantly longer durations than any previously reported findings. Our results reveal that ultrashort optical pulses can generate materials with identical chemical composition and structural state but entirely distinct magnetic arrangements, leading to unique magnetic properties. This breakthrough discovery marks a new era in light-driven control of matter, offering the exciting potential to create materials with properties that were once considered unattainable.

cond-mat.mtrl-sci↗

arXiv2023

Probing the Surface Polarization of Ferroelectric Thin Films by X-ray Standing Waves

Understanding the mechanisms underlying a stable polarization at the surface of ferroelectric thin films is of particular importance both from a fundamental point of view and to achieve control of the surface polarization itself. In this study, it is demonstrated that the X-ray standing wave technique allows the polarization near the surface of a ferroelectric thin film to be probed directly. The X-ray standing wave technique is employed to determine, with picometer accuracy, Ti and Ba atomic positions near the surface of three differently strained $\mathrm{BaTiO_3}$ thin films grown on scandate substrates, with a $\mathrm{SrRuO_3}$ film as bottom electrode. This technique gives direct access to atomic positions, and thus to the local ferroelectric polarization, within the first 3 unit cells below the surface. By employing X-ray photoelectron spectroscopy, a detailed overview of the oxygen-containing species adsorbed on the surface, upon exposure to ambient conditions, is obtained. The combination of structural and spectroscopic information allows us to conclude on the most plausible mechanisms that stabilize the surface polarization in the three samples under study. The different amplitude and orientation of the local ferroelectric polarizations are associated with surface charges attributed to the type, amount and spatial distribution of the oxygen-containing adsorbates.

cond-mat.mtrl-sci↗

arXiv2023

Photo-induced charge-transfer renormalization in NiO

Photo-doped states in strongly correlated charge transfer insulators are characterized by $d$-$d$ and $d$-$p$ interactions and the resulting intertwined dynamics of charge excitations and local multiplets. Here we use femtosecond x-ray absorption spectroscopy in combination with dynamical mean-field theory to disentangle these contributions in NiO. Upon resonant optical excitation across the charge transfer gap, the Ni $L_3$ and O $K$ absorption edges red-shift for $>10$ ps, associated with photo-induced changes in the screening environment. An additional signature below the Ni $L_3$ edge is identified for $<1$ ps, reflecting a transient nonthermal population of local many-body multiplets. We employ a nonthermal generalization of the multiplet ligand field theory to show that the feature originates from $d$-$d$ transitions. Overall, the photo-doped state differs significantly from a chemically doped state. Our results demonstrate the ability to reveal excitation pathways in correlated materials by x-ray spectroscopies, which is relevant for ultrafast materials design.

cond-mat.str-el↗

arXiv2023

Transient non-collinear magnetic state for all-optical magnetization switching

Resonant absorption of a photon by bound electrons in a solid can promote an electron to another orbital state or transfer it to a neighboring atomic site. Such a transition in a magnetically ordered material could affect the magnetic order. While this process is an obvious road map for optical control of magnetization, experimental demonstration of such a process remains challenging. Exciting a significant fraction of magnetic ions requires a very intense incoming light beam, as orbital resonances are often weak compared to above-band-gap excitations. In the latter case, a sizeable reduction of the magnetization occurs as the absorbed energy increases the spin temperature, masking the non-thermal optical effects. Here, using ultrafast x-ray spectroscopy, we were able to resolve changes in the magnetization state induced by resonant absorption of infrared photons in Co-doped yttrium iron garnet, with negligible thermal effects. We found that the optical excitation of the Co ions affects the two distinct magnetic Fe sublattices differently, resulting in a transient non-collinear magnetic state. The present results indicate that the all-optical magnetization switching most likely occurs due to the creation of a transient, non-collinear magnetic state followed by coherent spin rotations of the Fe moments.

cond-mat.mtrl-sci↗

arXiv2023

Photon shot-noise limited transient absorption soft X-ray spectroscopy at the European XFEL

Femtosecond transient soft X-ray Absorption Spectroscopy (XAS) is a very promising technique that can be employed at X-ray Free Electron Lasers (FELs) to investigate out-of-equilibrium dynamics for material and energy research. Here we present a dedicated setup for soft X-rays available at the Spectroscopy & Coherent Scattering (SCS) instrument at the European X-ray Free Electron Laser (EuXFEL). It consists of a beam-splitting off-axis zone plate (BOZ) used in transmission to create three copies of the incoming beam, which are used to measure the transmitted intensity through the excited and unexcited sample, as well as to monitor the incoming intensity. Since these three intensity signals are detected shot-by-shot and simultaneously, this setup allows normalized shot-by-shot analysis of the transmission. For photon detection, the DSSC imaging detector, which is capable of recording up to 800 images at 4.5 MHz frame rate during the FEL burst, is employed and allows approaching the photon shot-noise limit. We review the setup and its capabilities, as well as the online and offline analysis tools provided to users.

physics.ins-det↗

arXiv2022

Electron Dynamics at High-Energy Densities in Nickel from Non-linear Resonant X-ray Absorption Spectra

The pulse intensity from X-ray free-electron lasers (FELs) can create extreme excitation densities in solids, entering the regime of non-linear X-ray-matter interactions. We show L3-edge absorption spectra of metallic nickel thin films with fluences entering a regime where several X-ray photons are incident per absorption cross-section. Main features of the observed non-linear spectral changes are described with a predictive rate model for electron population dynamics during the pulse, utilizing a fixed density of states and tabulated ground-state properties.

cond-mat.mtrl-sci↗

arXiv2022

The interplay of local electron correlations and ultrafast spin dynamics in fcc Ni

The complex electronic structure of metallic ferromagnets is determined by a balance between exchange interaction, electron hopping leading to band formation, and local Coulomb repulsion. The interplay between the respective terms of the Hamiltonian is of fundamental interest, since it produces most, if not all, of the exotic phenomena observed in the solid state. By combining high energy and temporal resolution in femtosecond time-resolved X-ray absorption spectroscopy with ab initio time-dependent density functional theory we analyze the electronic structure in fcc Ni on the time scale of these interactions in a pump-probe experiment. We distinguish transient broadening and energy shifts in the absorption spectra, which we demonstrate to be caused by electron repopulation and correlation-induced modifications of the electronic structure, respectively. Importantly, the theoretical description of this experimental result hence requires to take the local Coulomb interaction into account, revealing a temporal interplay between band formation, exchange interaction, and Coulomb repulsion.

cond-mat.mtrl-sci↗