arXiv subjects

Clemens von Korff Schmising

Publications and source records attributed to Clemens von Korff Schmising.

At least 19 recordsLinked to original sources

arXiv2026

Depth-resolved magnetization dynamics in Fe thin films after ultrafast laser excitation

We performed time-resolved x-ray resonant magnetic reflectivity measurements on a laser-excited ferromagnetic Fe thin film to simultaneously probe the transient magnetic and structural depth profiles with nanometer spatial and femtosecond temporal resolution. Our results show that during the first picoseconds after optical excitation, the magnetization of the Fe layer is strongly inhomogeneous, especially in the vicinity of the buried interface. By comparing our experimental results to predictions based on the microscopic three-temperature model and simulations of laser-induced spin-currents, we demonstrate that local and non-local angular momentum transfer phenomena take place simultaneously. After a few picoseconds, the magnetization relaxes back to equilibrium while the total thin film thickness starts oscillating periodically, with a maximum dilation of approximately 1.3% of the entire thin film thickness due to laser-induced stresses.

cond-mat.mtrl-sci↗

arXiv2026

Optically induced metallic state with persistent monoclinic symmetry in NdNiO$_3$

Understanding whether electronic and structural order remain coupled under nonequilibrium conditions is a central challenge in correlated materials. Here, we simultaneously track metallicity and symmetry across the photoinduced insulator-to-metal transition in NdNiO$_3$ using time-resolved optical reflectivity and symmetry-sensitive second-harmonic generation. We find that metallic reflectivity emerges at significantly lower excitation fluence than restoration of the orthorhombic high-temperature symmetry. As a result, optical excitation stabilizes a metastable state that combines the reflectivity of the metallic phase with the monoclinic symmetry of the insulating phase, revealing an optically induced monoclinic metal. Only at substantially higher fluences does the symmetry fully recover to that of the high-temperature phase. These results demonstrate a nonequilibrium decoupling of metallicity and structural symmetry and establish simultaneous multiprobe spectroscopy as a powerful approach for identifying emergent phases in correlated materials.

cond-mat.str-el↗

arXiv2026

Orientation-resolved ultrafast spin reorientation dynamics in ferrimagnetic DyCo$_5$

Under quasi-static conditions, ferrimagnetic DyCo$_5$ thin films exhibit a thermally induced spin-reorientation transition, in which the equilibrium magnetization changes from an out-of-plane to an in-plane orientation, mostly as a result of the competing magnetic anisotropy contributions of the Dy $4f$ rare-earth and Co $3d$ transition-metal sublattices. While this equilibrium transition has been studied, it remains an open question whether such a reorientation can be triggered on ultrafast timescales using femtosecond laser excitation. In this work, we investigate the ultrafast spin-reorientation dynamics in DyCo$_5$. The time-dependent orientation of the magnetization vector following femtosecond laser excitation is quantified by combining polar with transverse magneto-optical Kerr effect (MOKE) measurements in the extreme ultraviolet spectral range, which are sensitive to the out-of-plane and in-plane magnetization component, respectively. Both techniques are implemented at the Co M$_{3,2}$ resonance and are complemented by visible-light MOKE measurements. This combined approach allows us to resolve the canting of the magnetization from an out-of-plane toward an in-plane orientation and to determine the characteristic timescales of the transient spin-reorientation process.

cond-mat.mtrl-sci↗

arXiv2025

Spectroscopic probe of ultrafast magnetization dynamics in the extreme ultraviolet spectral range

The development of spectroscopic techniques in the extreme ultraviolet (XUV) spectral range has significantly advanced the understanding of ultrafast interactions in magnetic systems triggered by optical excitation. In this work, we introduce a previously missing geometry that facilitates the observation of the ultrafast magnetization dynamics of magnetic systems with an out-of-plane magnetization grown on XUV opaque substrates. This approach to probing ultrafast magnetization dynamics combines the magneto-optical Kerr effect with the strong dependence of a sample's reflectance near its Brewster angle. It therefore works with linearly polarized light and does not require any additional polarizing optics. We provide a comprehensive analysis of the technique by presenting both simulations and experimental data as a function of the energy and the polarization of the XUV probe radiation as well as of the delay time after optical excitation.

cond-mat.mtrl-sci↗

arXiv2025

Studying all-optical magnetization switching of GdFe by double-pulse laser excitation

The tremendous interest in the technology and underlying physics of all-optical switching of magnetization brings up the question of how fast the switching can occur and how high the frequency of writing the data with ultrafast laser pulses can be. To answer this question, we excited a GdFe ferrimagnetic alloy, the magnetization of which can be reversed by single laser pulses, a phenomenon known as toggle switching, by two pulses with a certain time delay in between. Using photoemission electron microscopy and Kerr microscopy for magnetic domain imaging, we explore the effects of varying fluences of the first and second pulse as well as the time delay between the two pulses. Our results show that when the fluence of the first pulse is adjusted just above the threshold of single-pulse switching, a second pulse with about 60% of the fluence of the first pulse, arriving only 3 ps later, switches the magnetization back. This reswitching persists up to about 40 ps pulse separation. We interpret the latter as the time required for the sample to cool down and remagnetize after the first pulse. For shorter time delays below about 2 ps, no re-switching occurs. However, the effect of the two pulses adds up, enabling switching for fluences of both pulses below the threshold for single-pulse switching. Atomistic spin dynamics simulations are used to model the experimental data, successfully confirming our results.

cond-mat.mtrl-sci↗

arXiv2025

Tunable magnons in a dual-gated 2D antiferromagnet

The layered antiferromagnet CrSBr features magnons coupled to other quasiparticles, including excitons and polaritons, enabling their easy optical accessibility. In this work, we investigate the tunability of magnons in few-layered devices in response to changes in carrier density and the application of a perpendicular electric field. We demonstrate an on-chip tunability of the in- and out-of-phase magnon frequencies by up to 2 GHz. While the frequencies of both modes increase with the electron density, we observe an asymmetric response with respect to the electric field in a dual-gated trilayer device. To understand the mechanism of this disparity, we develop a layer-resolved macrospin model describing the magnetic dynamics in thin, non-uniformly doped devices. Through this model we establish the doping- and electric-field-dependence of the exchange interaction, magnetic anisotropy, and magnetic moment of individual layers. Our results advance the applications of gate-tunable magnonic devices based on 2D materials.

cond-mat.mes-hall↗

arXiv2025

X-ray View of Light-Induced Spin Reorientation in TmFeO$_{3}$: Direct Observation of a 90$^\circ$ Néel Vector Rotation

Using time-resolved X-ray magnetic linear dichroism in reflection, we provide a direct probe of the Néel vector dynamics in TmFeO$_3$ on a ultrafast timescale. Our measurements reveal that, following optical excitation, the Néel vector undergoes a spin reorientation transition primarily within the a-c plane, completing a full 90° rotation within approximately 20 ps. This study highlights the ability to probe dynamics of antiferromagnets at its intrinsic timescale in reflection geometry, paving the way for investigations of a wide range of antiferromagnets grown on application relevant substrates.

cond-mat.mtrl-sci↗

arXiv2025

Fluence dependent delay of Ni in an FeNi alloy supports an exchange based origin

The delayed demagnetization in Ni relative to Fe in the ultrafast demagnetization studies in FeNi alloy has led to two competing theoretical explanations: The Inhomogeneous Magnon Generation (IMG) and the Optically Induced Spin Transfer (OISTR) model. The IMG attributes the delay to the preferential magnon generation at the Fe sites and its subsequent propagation to Ni, while OISTR proposes direct spin transfer from Ni to Fe. In this study, we employ element-resolved extreme ultraviolet spectroscopy to investigate the effect of excitation strength on this delay, aiming to resolve the controversy. The data indicate a significant reduction in the delay with increasing fluence, which is inconsistent with the theoretical predictions of OISTR. These findings, in conjunction with the observation of a saturation of Fe demagnetization at the onset of Ni demagnetization, indicate that a spin-wave instability within the IMG framework may provide a potential explanation for the experimental results.

cond-mat.mtrl-sci↗

arXiv2025

Wavelength-Dependent Photodissociation of Iodomethylbutane

Ultrashort XUV pulses of the Free-Electron-LASer in Hamburg (FLASH) were used to investigate laser-induced fragmentation patterns of the prototypical chiral molecule 1-iodo-2-methyl-butane (C$_5$H$_{11}$I) in a pump-probe scheme. Ion velocity-map images and mass spectra of optical-laser-induced fragmentation were obtained for subsequent FEL exposure with photon energies of 63 eV and 75 eV. These energies specifically address the iodine 4d edge of neutral and singly charged iodine, respectively. The presented ion spectra for two optical pump-laser wavelengths, i.e., 800 nm and 267 nm, reveal substantially different cationic fragment yields in dependence on the wavelength and intensity. For the case of 800-nm-initiated fragmentation, the molecule dissociates notably slower than for the 267-nm pump. The results underscore the importance of considering optical-laser wavelength and intensity in the dissociation dynamics of this prototypical chiral molecule that is a promising candidate for future studies of its asymmetric nature.

physics.chem-ph↗

arXiv2024

Sub-wavelength localized all-optical helicity-independent magnetic switching using plasmonic gold nanostructures

All-optical helicity-independent switching (AO-HIS) is of interest for ultrafast and energy efficient magnetic switching in future magnetic data storage approaches. Yet, to achieve high bit density magnetic recording it is necessary to reduce the size of the magnetic bits addressed by laser pulses at well-controlled positions. Metallic nanostructures that support localized surface plasmons enable spatial electromagnetic confinement well below the diffraction limit and rare-earth transition metal alloys such as GdTbCo have demonstrated nanometre-sized stable domains. Here, we deposit plasmonic gold nanostructures on a GdTbCo film and probe the magnetic state using magnetic force microscopy. We observe localized AO-HIS down to a critical dimension of 240 nm after excitation of the gold nanostructures by a single 370 fs long laser pulse with a centre wavelength of 1030 nm. We demonstrate that the strong localization of optical fields through plasmonic nanostructures enables reproducible localized nanoscale AO-HIS at sub-wavelength length scales. We study the influence of the localized electromagnetic field enhancement by the plasmonic nanostructures on the required fluence to switch the magnetization.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast Opto-magnetic Effects in the Extreme Ultraviolet Spectral Range

Coherent light-matter interactions mediated by opto-magnetic phenomena like the inverse Faraday effect (IFE) are expected to provide a non-thermal pathway for ultrafast manipulation of magnetism on timescales as short as the excitation pulse itself. As the IFE scales with the spin-orbit coupling strength of the involved electronic states, photo-exciting the strongly spin-orbit coupled core-level electrons in magnetic materials appears as an appealing method to transiently generate large opto-magnetic moments. Here, we investigate this scenario in a ferrimagnetic GdFeCo alloy by using intense and circularly polarized pulses of extreme ultraviolet radiation. Our results reveal ultrafast and strong helicity-dependent magnetic effects which are in line with the characteristic fingerprints of an IFE, corroborated by ab initio opto-magnetic IFE theory and atomistic spin dynamics simulations.

cond-mat.mtrl-sci↗

arXiv2023

Nanoscale transient polarization gratings

We present the generation of transient polarization gratings at the nanoscale, achieved using a tailored accelerator configuration of the FERMI free electron laser. We demonstrate the capabilities of such a transient polarization grating by comparing its induced dynamics with the ones triggered by a more conventional intensity grating on a thin film ferrimagnetic alloy. While the signal of the intensity grating is dominated by the thermoelastic response of the system, such a contribution is suppressed in the case of the polarization grating. This exposes helicity-dependent magnetization dynamics that have so-far remained hidden under the large thermally driven response. We anticipate nanoscale transient polarization gratings to become useful for the study of any physical, chemical and biological systems possessing chiral symmetry.

cond-mat.mtrl-sci↗

arXiv2023

Ultrafast behavior of induced and intrinsic magnetic moments in CoFeB/Pt bilayers probed by element-specific measurements in the extreme ultraviolet spectral range

The ultrafast and element-specific response of magnetic systems containing ferromagnetic 3d transition metals and 4d/5d heavy metals is of interest both from a fundamental as well as an applied research perspective. However, to date no consensus about the main microscopic processes describing the interplay between intrinsic 3d and induced 4d/5d magnetic moments upon femtosecond laser excitation exist. In this work, we study the ultrafast response of CoFeB/Pt bilayers by probing element-specific, core-to-valence band transitions in the extreme ultraviolet spectral range using high harmonic radiation. We show that the combination of magnetic scattering simulations and analysis of the energy- and time-dependent magnetic asymmetries allows to accurately disentangle the element-specific response in spite of overlapping Co and Fe M$_{2,3}$ as well as Pt O$_{2,3}$ and N$_7$ resonances. We find a considerably smaller demagnetization time constant as well as much larger demagnetization amplitudes of the induced moment of Pt compared to the intrinsic moment of CoFeB. Our results are in agreement with enhanced spin-flip probabilities due to the high spin-orbit coupling localized at the heavy metal Pt, as well as with the recently formulated hypothesis that a laser generated, incoherent magnon population within the ferromagnetic film leads to an overproportional reduction of the induced magnetic moment of Pt.

cond-mat.mtrl-sci↗

arXiv2022

Picosecond x-ray magnetic circular dichroism spectroscopy at the Fe L-edges with a laser-driven plasma source

Time-resolved x-ray magnetic circular dichroism (XMCD) enables a unique spectroscopic view on complex spin and charge dynamics in multi-elemental magnetic materials. So far, its application in the soft-x-ray range has been limited to synchrotron-radiation sources and free-electron lasers. By combining a laser-driven plasma source with a magnetic thin-film polarizer, we generate circularly polarized photons in the soft x-ray regime, enabling the first XMCD spectroscopy at the Fe L edges in a laser laboratory. Our approach can be readily adapted to other transition metal L and rare earth M absorption edges and with a temporal resolution of < 10 ps, a wide range of ultrafast magnetization studies can be realized.

cond-mat.mtrl-sci↗

arXiv2022

Ultrafast element- and depth-resolved magnetization dynamics probed by transverse magneto-optical Kerr effect spectroscopy in the soft x-ray range

We report on time- and angle-resolved transverse magneto-optical Kerr effect spectroscopy in the soft x-ray range that, by analysis via polarization-dependent magnetic scattering simulations, allows us to determine the spatio-temporal and element-specific evolution of femtosecond laser-induced spin dynamics in nanostructured magnetic materials. In a ferrimagnetic GdFe thin film system, we correlate a reshaping spectrum of the magneto-optical Kerr signal to depth-dependent magnetization dynamics and disentangle contributions due to non-equilibrium electron transport and nanoscale heat diffusion on their intrinsic time scales. Our work provides a quantitative insight into light-driven spin dynamics occurring at buried interfaces of complex magnetic heterostructures, which can be tailored and functionalized for future opto-spintronic devices.

cond-mat.mtrl-sci↗

arXiv2022

All-optical switching on the nanometer scale excited and probed with femtosecond extreme ultraviolet pulses

Ultrafast control of magnetization on the nanometer length scale, in particular all-optical switching, is key to putting ultrafast magnetism on the path towards future technological application in data storage technology. However, magnetization manipulation with light on this length scale is challenging due to the wavelength limitations of optical radiation. Here, we excite transient magnetic gratings in a GdFe alloy with a periodicity of 87 nm by interference of two coherent femtosecond light pulses in the extreme ultraviolet spectral range at the free electron laser facility FERMI. The subsequent ultrafast evolution of the magnetization pattern is probed by diffraction of a third, time-delayed pulse tuned to the Gd N-edge at a wavelength of 8.3 nm. By examining the simultaneously recorded first and second diffraction orders and by performing reference real-space measurements with a wide-field magneto-optical microscope with femtosecond time resolution, we can conclusively demonstrate the ultrafast emergence of all-optical switching on the nanometer length scale.

cond-mat.mtrl-sci↗

arXiv2022

Megahertz-rate Ultrafast X-ray Scattering and Holographic Imaging at the European XFEL

The advent of X-ray free-electron lasers (XFELs) has revolutionized fundamental science, from atomic to condensed matter physics, from chemistry to biology, giving researchers access to X-rays with unprecedented brightness, coherence, and pulse duration. All XFEL facilities built until recently provided X-ray pulses at a relatively low repetition rate, with limited data statistics. Here, we present the results from the first megahertz repetition rate X-ray scattering experiments at the Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL. We illustrate the experimental capabilities that the SCS instrument offers, resulting from the operation at MHz repetition rates and the availability of the novel DSSC 2D imaging detector. Time-resolved magnetic X-ray scattering and holographic imaging experiments in solid state samples were chosen as representative, providing an ideal test-bed for operation at megahertz rates. Our results are relevant and applicable to any other non-destructive XFEL experiments in the soft X-ray range.

cond-mat.mes-hall↗

arXiv2021

Probing electron and hole co-localization by resonant four-wave mixing in the extreme-ultraviolet

The extension of nonlinear spectroscopic techniques into the x-ray domain is in its infancy but holds the promise to provide unique insight into the dynamics of charges in photoexcited processes, which are of fundamental as well as applied interest. We report on the observation of a third order nonlinear process in lithium fluoride at a free-electron laser. Exploring the yield of four wave mixing (FWM) in resonance with transitions to strongly localized core exciton states vs. delocalized Bloch states, we find resonant FWM to be a sensitive probe for the degree of charge localization: substantial sum- and difference-frequency generation is observed exclusively when in a one- or three-photon resonance with a LiF core exciton, with a dipole forbidden transition affecting details of the nonlinear response. Our reflection-geometry-based approach to detect FWM signals enables the study of a wide variety of condensed matter sample systems, provides atomic selectivity via resonant transitions and can be easily scaled to shorter wavelengths at free electron x-ray lasers.

physics.app-ph↗