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C. Schüßler-Langeheine

Publications and source records attributed to C. Schüßler-Langeheine.

14 recordsLinked to original sources

Simultaneous mapping of the ultrafast time and fluence dependence of the laser-induced insulator-to-metal transition in magnetite

Pump-probe methods are a ubiquitous tool in the field of ultrafast dynamic measurements. In recent years, x-ray free-electron laser experiments have gained importance due to their ability to probe with high chemical selectivity and at atomic length scales. Measurements are typically repeated many thousands of times to collect sufficient statistics and vary parameters like delay or fluence, necessitating that initial conditions are restored each time. An alternative is presented by experiments which measure the relevant parameters in a single shot. Here, we present a time-to-space mapping imaging scheme that enables us to record a range of delays and laser fluences in any single shot of the x-ray probe. We demonstrate the use of this scheme by mapping the ultrafast dynamics of the optically induced insulator-to-metal Verwey transition in a magnetite thin film, probed by soft x-ray resonant diffraction. By extrapolating our results toward the conditions found at x-ray free-electron lasers with higher photon energy, we demonstrate that the presented data could be recorded in a single shot.

cond-mat.mtrl-sci↗

First experiments with ultrashort, circularly polarized soft X-ray pulses at FLASH2

Time-resolved absorption spectroscopy as well as magnetic circular dichroism with circularly polarized soft X-rays (XAS and XMCD) are powerful tools to probe electronic and magnetic dynamics in magnetic materials element- and site-selectively. Employing these methods, groundbreaking results have been obtained for instance for magnetic alloys, which helped to fundamentally advance the field of ultrafast magnetization dynamics. At the free electron laser facility FLASH key capabilities for ultrafast XAS and XMCD experiments have recently improved: In an upgrade, an APPLE-III helical afterburner undulator was installed at FLASH2 in September 2023. This installation allows for the generation of circularly polarized soft X-ray pulses with a duration of a few tens of femtoseconds covering the L3,2-edges of the important 3d transition metal elements with pulse energies of several uJ. Here, we present first experimental results with such ultrashort X-ray pulses from the FL23 beamline employing XMCD at the L-edges of the 3d metals, Co, Fe and Ni. We obtain significant dichroic difference signals indicating a degree of circular polarization close to 100%. With the pulse-length preserving monochromator at beamline FL23 and an improved pump laser setup, FLASH can offer important and efficient experimental instrumentation for studies on ultrafast spin dynamics in 3d transition metals, multilayers, and alloys.

cond-mat.mtrl-sci↗

Optical control of 4f orbital state in rare-earth metals

A change of orbital state alters the coupling between ions and their surroundings drastically. Orbital excitations are hence key to understand and control interaction of ions. Rare-earth (RE) elements with strong magneto-crystalline anisotropy (MCA) are important ingredients for magnetic devices. Thus, control of their localized 4f magnetic moments and anisotropy is one major challenge in ultrafast spin physics. With time-resolved X-ray absorption and resonant inelastic scattering experiments, we show for Tb metal that 4f-electronic excitations out of the ground state multiplet occur after optical pumping. These excitations are driven by inelastic 5d-4f-electron scattering, alter the 4f-orbital state and consequently the MCA with important implications for magnetization dynamics in 4f-metals, and more general for the excitation of localized electronic states in correlated materials.

cond-mat.mtrl-sci↗

Ultrafast modification of the electronic structure of a correlated insulator

A non-trivial balance between Coulomb repulsion and kinematic effects determines the electronic structure of correlated electron materials. The use electromagnetic fields strong enough to rival these native microscopic interactions allows us to study the electronic response as well as the timescales and energies involved in using quantum effects for possible applications. We use element-specific transient x-ray absorption spectroscopy and high-harmonic generation to measure the response to ultrashort off-resonant optical fields in the prototypical correlated electron insulator NiO. Surprisingly, fields of up to 0.22 V/Å leads to no detectable changes on the correlated Ni 3d-orbitals contrary to previous predictions. A transient directional charge transfer is uncovered, a behavior that is captured by first-principles theory. Our results highlight the importance of retardation effects in electronic screening, and pinpoints a key challenge in functionalizing correlated materials for ultrafast device operation.

cond-mat.mtrl-sci↗

Exchange scaling of ultrafast angular momentum transfer in 4$\it{f}$ antiferromagnets

Ultrafast manipulation of the magnetic state of matter bears great potential for future information technologies. While demagnetisation in ferromagnets is governed by dissipation of angular momentum, materials with multiple spin sublattices, e.g. antiferromagnets, can allow direct angular momentum transfer between opposing spins, promising faster functionality. In lanthanides, 4$\it{f}$ magnetic exchange is mediated indirectly through the conduction electrons (the Ruderman-Kittel-Kasuya-Yosida interaction, RKKY), and the effect of such conditions on direct spin transfer processes is largely unexplored. Here, we investigate ultrafast magnetization dynamics in 4f antiferromagnets, and systematically vary the 4$\it{f}$ occupation, thereby altering the magnitude of RKKY. By combining time-resolved soft x-ray diffraction with ab-initio calculations, we find that the rate of direct transfer between opposing moments is directly determined by the magnitude of RKKY. Given the high sensitivity of RKKY to the conduction electrons, our results offer a novel approach for fine-tuning the speed of magnetic devices.

cond-mat.mtrl-sci↗

Ultrafast optically induced ferromagnetic state in an elemental antiferromagnet

We present evidence for an ultrafast optically induced ferromagnetic alignment of antiferromagnetic Mn in Co/Mn multilayers. We observe the transient ferromagnetic signal at the arrival of the pump pulse at the Mn L$_3$ resonance using x-ray magnetic circular dichroism in reflectivity. The timescale of the effect is comparable to the duration of the excitation and occurs before the magnetization in Co is quenched. Theoretical calculations point to the imbalanced population of Mn unoccupied states caused by the Co interface for the emergence of this transient ferromagnetic state.

cond-mat.mes-hall↗

Large response of charge stripes to uniaxial stress in $\textrm{La}_{1.475}\textrm{Nd}_{0.4}\textrm{Sr}_{0.125}\textrm{Cu}\textrm{O}_{4}$

The La-based '214' cuprates host several symmetry breaking phases including superconductivity, charge and spin order in the form of stripes, and a structural othorhombic-to-tetragonal phase transition. Therefore, these materials are an ideal system to study the effects of uniaxial stress onto the various correlations that pervade the cuprate phase diagram. We report resonant x-ray scattering experiments on $\textrm{La}_{1.475}\textrm{Nd}_{0.4}\textrm{Sr}_{0.125}\textrm{Cu}\textrm{O}_{4}$ (LNSCO-125) that reveal a significant response of charge stripes to uniaxial tensile-stress of $\sim$ 0.1 GPa. These effects include a reduction of the onset temperature of stripes by $\sim$ 50 K, a 29 K reduction of the low-temperature orthorhombic-to-tetragonal transition, competition between charge order and superconductivity, and a preference for stripes to form along the direction of applied stress. Altogether, we observe a dramatic response of the electronic properties of LNSCO-125 to a modest amount of uniaxial stress.

cond-mat.str-el↗

Charge disproportionation and nano phase separation in $R$SrNiO$_4$

We have successfully grown centimeter-sized layered $R$SrNiO$_4$ single crystals under high oxygen pressures of 120 bar by the floating zone technique. This enabled us to perform neutron scattering experiments where we observe close to quarter-integer magnetic peaks below $\sim$77 K that are accompanied by steep upwards dispersing spin excitations. Within the high-frequency Ni-O bond stretching phonon dispersion, a softening at the propagation vector for a checkerboard modulation can be observed. Together with our spin wave simulations these observations reveal that this Ni$^{3+}$ system exhibits charge disproportionation with charges segregating into a checkerboard pattern within a nano phase separation scenario rather than showing a Jahn-Teller effect.

cond-mat.str-el↗

Epitaxy, stoichiometry, and magnetic properties of Gd-doped EuO films on YSZ (001)

We have succeeded in preparing high-quality Gd-doped single-crystalline EuO films. Using Eu-distillation-assisted molecular beam epitaxy and a systematic variation in the Gd and oxygen deposition rates, we have been able to observe sustained layer-by-layer epitaxial growth on yttria-stabilized cubic zirconia (001). The presence of Gd helps to stabilize the layer-by-layer growth mode. We used soft x-ray absorption spectroscopy at the Eu and Gd M4,5 edges to confirm the absence of Eu3+ contaminants and to determine the actual Gd concentration. The distillation process ensures the absence of oxygen vacancies in the films. From magnetization measurements we found the Curie temperature to increase smoothly as a function of doping from 70 K up to a maximum of 125 K. A threshold behavior was not observed for concentrations as low as 0.2%.

cond-mat.str-el↗

Epitaxial and layer-by-layer growth of EuO thin films on yttria-stabilized cubic zirconia (001) using MBE distillation

We have succeeded in growing epitaxial and highly stoichiometric films of EuO on yttria-stabilized cubic zirconia (YSZ) (001). The use of the Eu-distillation process during the molecular beam epitaxy assisted growth enables the consistent achievement of stoichiometry. We have also succeeded in growing the films in a layer-by-layer fashion by fine tuning the Eu vs. oxygen deposition rates. The initial stages of growth involve the limited supply of oxygen from the YSZ substrate, but the EuO stoichiometry can still be well maintained. The films grown were sufficiently smooth so that the capping with a thin layer of aluminum was leak tight and enabled ex situ experiments free from trivalent Eu species. The findings were used to obtain recipes for better epitaxial growth of EuO on MgO (001).

cond-mat.str-el↗

Magnetic structure of RuSr$_2$GdCu$_2$O$_8$ determined by resonant x-ray diffraction

X-ray diffraction with photon energies near the Ru L$_2$-absorption edge was used to detect resonant reflections characteristic of a G-type superstructure in RuSr$_2$GdCu$_2$O$_8$ single crystals. A polarization analysis confirms that these reflections are due to magnetic order of Ru moments, and the azimuthal-angle dependence of the scattering amplitude reveals that the moments lie along a low-symmetry axis with substantial components parallel and perpendicular to the RuO$_2$ layers. Complemented by susceptibility data and a symmetry analysis of the magnetic structure, these results reconcile many of the apparently contradictory findings reported in the literature.

cond-mat.str-el↗

Atomic multiplet calculation of 3d_{5/2} -> 4f resonant x-ray diffraction from Ho metal

We compare for Ho metal the x-ray absorption spectrum and the resonant soft x-ray diffraction spectra obtained at the $3d_{5/2} \to 4f$ ($M_5$) resonance for the magnetic 1st and 2nd order diffraction peaks $(0,0,τ)$ and $(0,0,2τ)$ with the result of an atomic multiplet calculation. We find a good agreement between experiment and simulation giving evidence that this kind of simulation is well suited to quantitatively analyze resonant soft x-ray diffraction data from correlated electron systems.

cond-mat.str-el↗

Resonant soft x-ray scattering from stepped surfaces of SrTiO3

We studied the resonant diffraction signal from stepped surfaces of SrTiO3 at the Ti 2p -> 3d (L2,3) resonance in comparison with x-ray absorption (XAS) and specular reflectivity data. The steps on the surface form an artificial superstructure suited as a model system for resonant soft x-ray diffraction. A small step density on the surface is sufficient to produce a well defined diffraction peak, showing the high sensitivity of the method. At larger incidence angles, the resonant diffraction spectrum from the steps on the surface resembles the spectrum for specular reflectivity. Both deviate from the XAS data in the relative peak intensities and positions of the peak maxima. We determined the optical parameters of the sample across the resonance and found that the differences between the XAS and scattering spectra reflect the different quantities probed in the different signals. When recorded at low incidence or detection angles, XAS and specular reflectivity spectra are distorted by the changes of the angle of total reflection with energy. Also the step peak spectra, though less affected, show an energy shift of the peak maxima in grazing incidence geometry.

cond-mat.str-el↗

Electronic structure of NiS$_{1-x}$Se$_x$ across the phase transition

We report very highly resolved photoemission spectra of NiS(1-x)Se(x) across the so-called metal-insulator transition as a function of temperature as well as composition. The present results convincingly demonstrate that the low temperature, antiferromagnetic phase is metallic, with a reduced density of states at E$_F$. This decrease is possibly due to the opening of gaps along specific directions in the Brillouin zone caused by the antiferromagnetic ordering.

cond-mat.str-el↗