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Heiko Wende

Publications and source records attributed to Heiko Wende.

At least 19 recordsLinked to original sources

Nanoscale Confinement Enhances Ultrafast Demagnetization

Nanoscale miniaturization has revolutionized the field of spintronics by enabling exponential growth in areal bit density. A similar leap is also expected in device speeds through successfully harnessing femtosecond magnetization dynamics. However, combining this with the miniaturization of realistic devices is challenging. To address this, we studied the effect of dimensional confinement on the femtosecond demagnetization of Fe. By gradually increasing the level of confinement while keeping excitation conditions constant, we found that Fe layers thinner than 10 nm exhibit enlarged demagnetization amplitudes, reaching a $\sim75\%$ increase at 2 nm. By combining ultrafast experiments sensitive to the spins, the charge carriers, and the phonons, we establish that this finite$\text{-}$size effect is magnetic in origin and is not phonon$\text{-}$driven. With the support of ab$\text{-}$initio calculations and atomistic spin dynamics simulations, we identify the enhancement effect as due to local weakening of spin order at the Fe$\text{'}$s interface, which becomes significant upon increased confinement.

cond-mat.mes-hall

A Combined Theoretical and Experimental Study of Oxygen Vacancies in Co$_3$O$_4$ for Liquid-Phase Oxidation Catalysis

In the present work, we investigate oxygen vacancies (V$_\mathrm{O}$) in Co$_3$O$_4$, both in the bulk phase and under liquid-phase ethylene glycol oxidation, by combining theoretical and experimental techniques. Density functional theory calculations for bulk Co$_3$O$_4$ show that introducing an oxygen vacancy reduces two adjacent Co$^{3+}$ ions to Co$^{2+}$ and narrows the band gap. The newly formed Co$^{2+}$ ions adopt high-spin configurations in distorted octahedral sites and remain stable in this state in ab initio molecular dynamics simulations at $300$ K. Computed O and Co K-edge X-ray absorption spectra for ideal and vacancy-containing Co$_3$O$_4$ show excellent agreement with the experimental data and serve as references to analyze the liquid-phase ethylene glycol oxidation. The comparison with experimental O K-edge spectra of fresh and post-reaction catalysts shows that fresh samples resemble the vacancy-containing reference, whereas post-reaction spectra shift toward the ideal reference. These results suggest that under liquid-phase ethylene glycol oxidation conditions, Co$_3$O$_4$ becomes more oxidized rather than reduced, by refilling preexisting oxygen vacancies. This is further supported by the observation that higher O$_2$ pressures increase the conversion and that the catalyst remains stable and active over several cycles.

cond-mat.mtrl-sci

Magnetomechanical Coupling in Ferronematic Phases: Influence of Spindle-Shaped Nanodopants on Liquid Crystalline Order

Ferronematic phases, composed of liquid crystals doped with magnetic nanoparticles, exhibit unique magnetomechanical coupling effects that are of interest for responsive materials. In this study, we investigate the influence of spindle-shaped {\alpha}-Fe_2O_3 nanoparticles functionalized with a mesogen-decorated polymer brush on the phase behavior and field-induced transitions of a nematic host (5CB). Differential scanning calorimetry (DSC), refractometry, and dielectric spectroscopy reveal a non-monotonic dependence of the nematic-isotropic transition temperature on particle concentration, indicating a competition between stabilizing and destabilizing effects. The order parameter increases with increasing nanoparticle content, in contrast to non-magnetic reference systems, suggesting an alignment effect induced by the magnetic rather than the geometric anisotropy axis of the dopants. Capacitance measurements of the Freedericksz transition show a pronounced shift in threshold fields, with a critical concentration marking a transition to enhanced magnetic responsiveness. Additional information on nanospindle diffusion correlated to the direction-dependent flow of the nematic host was inferred from comparison of Moessbauer spectroscopy and rheology data. Our findings provide insights into the interplay of magnetic and geometric anisotropy in ferronematic systems and highlight their potential for applications in tunable soft matter devices.

cond-mat.soft

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

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

Voltage-driven 90 switching of bulk perpendicular magnetic anisotropy in ferrimagnets

Unravelling the mechanism behind bulk perpendicular magnetic anisotropy (PMA) in amorphous rare earth-transition metal films has proven challenging. This is largely due to the inherent complexity of amorphous structure and the entangled potential origins arising from microstructure and atomic structure factors. Here, we present an approach wherein the magneto-electric effect is harnessed to induce 90{\deg} switching of bulk PMA in Tb-Co films to in-plane directions by applying voltages of only -1.2 V. This manipulation is achieved by voltage-driven insertion of hydrogen atoms into interstitial sites between Tb and Co atoms, which serves as a perturbation to local atomic structure. Using angle-dependent X-ray magnetic circular dichroism, we find that the anisotropy switching originates from the distortion of crystal field around Tb which reorients the alignment of Tb orbital moments. Initially aligned along Tb-Co bonding directions, the easy magnetization axis undergoes reorientation and switches by 90{\deg}, as substantiated by ab-initio calculations. Our study not only concludes the atomic origin of Tb-Co atom bonding configuration in shaping bulk PMA, but also establishes the groundwork for electrically programmable ferrimagnetic spintronics, such as controlling domain wall motion and programming artificial spin textures.

cond-mat.mtrl-sci

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

Element-Specific Study of Magnetic Anisotropy and Hardening in SmCo$_{5-x}$Cu$_{x}$ Thin Films

This work investigates the effect of copper substitution on the magnetic properties of SmCo$_{5}$ thin films synthesized by molecular beam epitaxy. A series of thin films with varying concentrations of Cu were grown under otherwise identical conditions to disentangle structural and compositional effects on the magnetic behavior. The combined experimental and theoretical studies show that Cu substitution at the Co$_{3g}$ sites not only stabilizes the formation of the SmCo$_{5}$ structure but enhances magnetic anisotropy and coercivity. Density functional theory calculations indicate that Sm(Co$_4$Cu$_{3g}$)$_5$ possesses a higher single-ion anisotropy as compared to pure SmCo$_{5}$. In addition, X-ray magnetic circular dichroism reveals that Cu substitution causes an increasing decoupling of the Sm 4\textit{f} and Co 3\textit{d} moments. Scanning transmission electron microscopy confirms predominantly SmCo$_{5}$ phase formation and reveals nanoscale inhomogeneities in the Cu and Co distribution. Our study based on thin film model systems and advanced characterization as well as modeling reveals novel aspects of the complex interplay of intrinsic and extrinsic contributions to magnetic hysteresis in rare earth-based magnets, \textit{i.e.} the combination of increased intrinsic anisotropy due to Cu substitution and the extrinsic effect of inhomogeneous elemental distribution of Cu and Co.

cond-mat.mtrl-sci

Formation of Core-Shell Precipitates in off-stochiometric Ni-Mn-Sn Heusler alloys probed through the induced Sn-moment

The Shell-ferromagnetic effect originates from the segregation process in off-stochiometric Ni-Mn-based Heusler. In this work, we investigate the precipitation process of L2$_1$-ordered Ni$_2$MnSn and L1$_0$-ordered NiMn in off-stochiometric Ni$_{50}$Mn$_{45}$Sn$_{5}$ during temper annealing, by X-ray diffraction (XRD) and $^{119}$Sn Mössbauer spectroscopy. While XRD probes long-range ordering of the lattice structure, Mössbauer spectroscopy probes nearest-neighbour interactions, reflected in the induced Sn magnetic moment. As shown in this work, the induced magnetic Sn moment can be used as a detector for microscopic structural changes and is, therefore, a powerful tool for investigating the formation of nano-precipitates. Similar research can be performed in the future, for example, on different pinning type magnets like Sm-Co or Nd-Fe-B.

cond-mat.mtrl-sci

Local magnetic and geometric structure in Mn-doped La(Fe,Si)13

Magnetic cooling has the potential to replace conventional gas compression refrigeration. Materials such as La(Fe,Si)$_{13}$ exhibit a sizeable first-order magnetocaloric effect, and it is possible to tailor the phase transition towards room temperature by Mn-H-doping, resulting in a large temperature range for operation. Within this work, we discuss variations of the electronic and lattice structure in La(Fe,Si)$_{13}$ with increasing Mn content utilizing X-ray magnetic circular dichroism (XMCD) and extended X-ray absorption fine structure spectroscopy (EXAFS). While XMCD shows a decrease of the magnetic polarization at the Fe K edge, low-temperature EXAFS measurements indicate increased positional disorder in the La environment that is otherwise absent for Fe and Mn. First-principles calculations link the positional disorder to an enlarged Mn-Si distance -- explaining the increased positional disorder in the La surrounding.

cond-mat.mtrl-sci

Autonomous atomic Hamiltonian construction and active sampling of x-ray absorption spectroscopy by adversarial Bayesian optimization

X-ray absorption spectroscopy (XAS) is a well-established method for in-depth characterization of the electronic structure due to its sensitivity to the local coordination and electronic states of the active ions. In practice hundreds of energy points should be sampled during the XAS measurement, most of which are redundant and do not contain important information. In addition, it is also a tedious procedure to estimate reasonable parameters in the atomic Hamiltonian for mechanistic understanding. We implemented an Adversarial Bayesian optimization (ABO) algorithm comprising two coupled BOs to automatically fit the multiplet model Hamiltonian and meanwhile to sample effectively based on active learning. Taking NiO as an example, for simulated spectra which can be well fitted by the atomic model, we found that less than 30 sampling points are enough to obtain the complete XAS with the corresponding crystal field or charge transfer model, which can be selected based on intuitive hypothesis learning. Further application on the experimental spectra, it revealed that less than 80 sampling points can already give reasonable XAS and reliable atomic model parameters. Our ABO algorithm has a great potential for future application in automated physics-driven XAS analysis and active learning sampling.

cond-mat.mtrl-sci

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

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

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

Element-specific visualization of dynamic magnetic coupling in a Co/Py bilayer microstructure

We present the element-specific and time resolved visualization of uniform ferromagnetic resonance excitations of a Permalloy (Py) disk - Cobalt (Co) stripe bilayer microstructure. The transverse high frequency component of the resonantly excited magnetization is sampled in the ps regime by a combination of ferromagnetic resonance (FMR) and scanning transmission X-ray microscopy (STXM- FMR) recording snapshots of the local magnetization precession of Py and Co with nanometer spatial resolution. The approach allows us to individually image the resonant dynamic response of each element, and we find that angular momentum is transferred from the Py disk to the Co stripe and vice versa at their respective resonances. The integral (cavity) FMR spectrum of our sample shows an unexpected additional third resonance. This resonance is observed in the STXM-FMR experiments as well and our microscopic findings suggest that it is governed by magnetic exchange between Py and Co, showing for the Co stripe a difference in relative phase of the magnetization due to stray field influence.

cond-mat.mes-hall

Complete crystallographic, spin-electronic and magnetic structure of (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)3O4: Unraveling the suppression of entropy in high entropy oxides

High entropy oxides (HEOs) are a rapidly emerging class of functional materials consisting of multiple principal cations. The original paradigm of HEOs assumes cationic occupations with the highest possible configurational entropy allowed by the composition and crystallographic structure. However, the fundamental question remains on the actual degree of configurational disorder in HEOs, especially, in systems with a low enthalpy barriers for cation anti-site mixing. Considering the experimental limitations due to the presence of multiple principal cations in HEOs, here we utilize a robust and cross-referenced characterization approach using soft X-ray magnetic circular dichroism, hard X-ray absorption spectroscopy, Mössbauer spectroscopy, neutron powder diffraction and SQUID magnetometry to study the competition between crystal field stabilization energy and configurational entropy governing the cation occupation in a spinel HEO (S-HEO), (Co$_{0.2}$Cr$_{0.2}$Fe$_{0.2}$Mn$_{0.2}$Ni$_{0.2}$)$_3$O$_4$. In contrast to the previous studies, the derived complete structural and spin-electronic model, (Co$_{0.6}$Fe$_{0.4}$)(Cr$_{0.3}$Fe$_{0.1}$Mn$_{0.3}$Ni$_{0.3}$)$_2$O$_4$, highlights a significant deviation from the hitherto assumed paradigm of entropy-driven non-preferential distribution of cations in HEOs. An immediate correlation of this result can be drawn with bulk as well as the local element specific magnetic properties, which are intrinsically dictated by cationic occupations in spinels. The real local lattice picture presented here provides an alternate viewpoint on ionic arrangement in HEOs, which is of fundamental interest for predicting and designing their structure-dependent functionalities.

cond-mat.mtrl-sci

Single-crystal graphene on Ir(110)

A single-crystal sheet of graphene is synthesized on the low-symmetry substrate Ir(110) by thermal decomposition of C$_2$H$_4$ at 1500 K. Using scanning tunneling microscopy, low-energy electron diffraction, angle-resolved photoemission spectroscopy, and ab initio density functional theory the structure and electronic properties of the adsorbed graphene sheet and its moiré with the substrate are uncovered. The adsorbed graphene layer forms a wave pattern of nm wave length with a corresponding modulation of its electronic properties. This wave pattern is demonstrated to enable the templated adsorption of aromatic molecules and the uniaxial growth of organometallic wires. Not limited to this, graphene on Ir(110) is also a versatile substrate for 2D-layer growth and makes it possible to grow epitaxial layers on ureconstructed Ir(110).

cond-mat.mtrl-sci

A full gap above the Fermi level: the charge density wave of monolayer VS2

In the standard model of charge density wave (CDW) transitions, the displacement along a single phonon mode lowers the total electronic energy by creating a gap at the Fermi level, making the CDW a metal--insulator transition. Here, using scanning tunneling microscopy and spectroscopy and ab initio calculations, we show that VS$_2$ realizes a CDW which stands out of this standard model. There is a full CDW gap residing in the unoccupied states of monolayer VS$_2$. At the Fermi level, the CDW induces a topological metal-metal (Lifshitz) transition. Non-linear coupling of transverse and longitudinal phonons is essential for the formation of the CDW and the full gap above the Fermi level. Additionally, x-ray magnetic circular dichroism reveals the absence of net magnetization in this phase, pointing to coexisting charge and spin density waves in the ground state.

cond-mat.mtrl-sci