arXiv subjects

H. A. Dürr

Publications and source records attributed to H. A. Dürr.

At least 19 recordsLinked to original sources

arXiv2025

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↗

arXiv2021

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↗

arXiv2021

Non-equilibrium self-assembly of spin-wave solitons in FePt nanoparticles

Magnetic nanoparticles such as FePt in the L10-phase are the bedrock of our current data storage technology. As the grains become smaller to keep up with technological demands, the superparamagnetic limit calls for materials with higher magneto-crystalline anisotropy. This in turn reduces the magnetic exchange length to just a few nanometers enabling magnetic structures to be induced within the nanoparticles. Here we describe the existence of spin-wave solitons, dynamic localized bound states of spin-wave excitations, in FePt nanoparticles. We show with time-resolved X-ray diffraction and micromagnetic modeling that spin-wave solitons of sub-10 nm sizes form out of the demagnetized state following femtosecond laser excitation. The measured soliton spin-precession frequency of 0.1 THz positions this system as a platform to develop miniature devices capable of filling the THz gap.

cond-mat.mtrl-sci↗

arXiv2019

Tracking the Ultrafast Non-Equilibrium Energy Flow between Electronic and Lattice Degrees of Freedom in Crystalline Nickel

Femtosecond laser excitation of solid-state systems creates non-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering we gain a detailed understanding of the complex non-equilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wavevector resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable agreement with our theoretical results. We find that zone-boundary phonon modes become occupied first. As soon as the energy in these modes becomes larger than the average electron energy a backflow of energy from lattice to electronic degrees of freedom occurs. Subsequent excitation of lower-energy phonon modes drives the thermalization of the whole system on the picosecond timescale. We determine the evolving non-equilibrium phonon occupations which we find to deviate markedly from thermal occupations.

cond-mat.mtrl-sci↗

arXiv2018

Spin-current-mediated rapid magnon localisation and coalescence after ultrafast optical pumping of ferrimagnetic alloys

Sub-picosecond magnetisation manipulation via femtosecond optical pumping has attracted wide attention ever since its original discovery in 1996. However, the spatial evolution of the magnetisation is not yet well understood, in part due to the difficulty in experimentally probing such rapid dynamics. Here, we find evidence of rapid magnetic order recovery in materials with perpendicular magnetic anisotropy via nonlinear magnon processes. We identify both localisation and coalescence regimes, whereby localised magnetic textures nucleate and subsequently evolve in accordance with a power law formalism. Coalescence is observed for optical excitations both above and below the switching threshold. Simulations indicate that the ultrafast generation of noncollinear magnetisation via optical pumping establishes exchange-mediated spin currents with an equivalent 100% spin polarised charge current density of $10^8$ A/cm$^2$. Such large spin currents precipitate rapid recovery of magnetic order after optical pumping. These processes suggest an ultrafast optical route for the stabilization of desired meta-stable states, e.g., isolated skyrmions.

cond-mat.mes-hall↗

arXiv2017

Beyond a phenomenological description of magnetostriction

We use ultrafast x-ray and electron diffraction to disentangle spin-lattice coupling of granular FePt in the time domain. The reduced dimensionality of single-crystalline FePt nanoparticles leads to strong coupling of magnetic order and a highly anisotropic three-dimensional lattice motion characterized by a- and b-axis expansion and c-axis contraction. The resulting increase of the FePt lattice tetragonality, the key quantity determining the energy barrier between opposite FePt magnetization orientations, persists for tens of picoseconds. These results suggest a novel approach to laser-assisted magnetic switching in future data storage applications.

cond-mat.mtrl-sci↗

arXiv2017

A tilted pulse-front setup for femtosecond extreme ultraviolet transient grating spectroscopy in highly non-collinear geometries

We demonstrate a tilted pulse-front transient grating technique that allows to optimally utilize time-resolution as well as transient grating line density while probing under grazing incidence as typically done in extreme ultraviolet (EUV) or soft x-ray (SXR) experiments. Our optical setup adapts the pulse front tilt of the two pulses that create the transient grating to the relative tilt grazing incident pulse. We demonstrate the technique using all 800 nm femtosecond laser pulses for transient grating generation on a vanadium dioxide film. We probe that grating via diffraction of a third 800 nm pulse. The time resolution of 100 fs is an improvement by a factor 30 compared to our previous experiments on the same system (1,2). The scheme paves the way for EUV and SXR probing of optically induced transient gratings on any material.

physics.ins-det↗

arXiv2017

Ultrafast imprinting of topologically protected magnetic textures via pulsed electrons

Short electron pulses are demonstrated to trigger and control magnetic excitations, even at low electron current densities. We show that the tangential magnetic field surrounding a picosecond electron pulse can imprint topologically protected magnetic textures such as skyrmions in a sample with a residual Dzyaloshinskii-Moriya spin-orbital coupling. Characteristics of the created excitations such as the topological charge can be steered via the duration and the strength of the electron pulses. The study points to a possible way for a spatio-temporally controlled generation of skyrmionic excitations.

physics.app-ph↗

arXiv2017

Terahertz-driven magnetism dynamics in the orthoferrite DyFeO3

Terahertz driven magnetization dynamics are explored in the orthoferrite DyFeO3. A high-field, single cycle THz pulse is used to excite magnon modes in the crystal together with other resonances. Both quasi-ferromagnetic and quasi-antiferromagnetic magnon modes are excited and appear in time-resolved measurements of the Faraday rotation. Other modes are also observed in the measurements of the time-resolved linear birefringence. Analysis of the excitation process reveals that despite larger than expected electro-optical susceptibility it is mainly the THz magnetic field that couples to the quasi-ferromagnetic and quasi-antiferromagnetic magnon branches.

cond-mat.mtrl-sci↗

arXiv2017

Stacking order dynamic in the quasi-two-dimensional dichalcogenide 1T-TaS$_2$ probed with MeV ultrafast electron diffraction

Transitions between different charge density wave (CDW) states in quasi-two-dimensional materials may be accompanied also by changes in the inter-layer stacking of the CDW. Using MeV ultrafast electron diffraction, the out-of-plane stacking order dynamics in the quasi-two-dimensional dichalcogenide 1T-TaS$_2$ is investigated for the first time. From the intensity of the CDW satellites aligned around the commensurate $l$ = 1/6 characteristic stacking order, it is found out that this phase disappears with a 0.5 ps time constant. Simultaneously, in the same experiment, the emergence of the incommensurate phase, with a slightly slower 2.0 ps time constant, is determined from the intensity of the CDW satellites aligned around the incommensurate $l$ = 1/3 characteristic stacking order. These results might be of relevance in understanding the metallic character of the laser-induced metastable "hidden" state recently discovered in this compound.

cond-mat.mtrl-sci↗

arXiv2016

Ultrafast THz Field Control of Electronic and Structural Interactions in Vanadium Dioxide

Vanadium dioxide, an archetypal correlated-electron material, undergoes an insulator-metal transition near room temperature that exhibits electron-correlation-driven and structurally-driven physics. Using ultrafast optical spectroscopy and x-ray scattering we show that these processes can be disentangled in the time domain. Specifically, following intense sub-picosecond electric-field excitation, a partial collapse of the insulating gap occurs within the first ps. Subsequently, this electronic reconfiguration initiates a change in lattice symmetry taking place on a slower timescale. We identify the kinetic energy increase of electrons tunneling in the strong electric field as the driving force, illustrating a novel method to control electronic interactions in correlated materials on an ultrafast timescale.

cond-mat.str-el↗

arXiv2016

THz-driven ultrafast spin-lattice scattering in amorphous metallic ferromagnets

We use single-cycle THz fields and the femtosecond magneto-optical Kerr effect to respectively excite and probe the magnetization dynamics in two thin-film ferromagnets with different lattice structure: crystalline Fe and amorphous CoFeB. We observe Landau-Lifshitz-torque magnetization dynamics of comparable magnitude in both systems, but only the amorphous sample shows ultrafast demagnetization caused by the spin-lattice depolarization of the THz-induced ultrafast spin current. Quantitative modelling shows that such spin-lattice scattering events occur on similar time scales than the conventional spin conserving electronic scattering ($\sim30$ fs). This is significantly faster that optical laser-induced demagnetization. THz conductivity measurements point towards the influence of lattice disorder in amorphous CoFeB as the driving force for enhanced spin-lattice scattering.

cond-mat.mtrl-sci↗

arXiv2016

Measurement of collective excitations in VO$_2$ by resonant inelastic X-ray scattering

Vanadium dioxide is of broad interest as a spin-1/2 electron system that realizes a metal-insulator transition near room temperature, due to a combination of strongly correlated and itinerant electron physics. Here, resonant inelastic X-ray scattering is used to measure the excitation spectrum of charge, spin, and lattice degrees of freedom at the vanadium L-edge under different polarization and temperature conditions. These spectra reveal the evolution of energetics across the metal-insulator transition, including the low temperature appearance of a strong candidate for the singlet-triplet excitation of a vanadium dimer.

cond-mat.str-el↗

arXiv2015

Direct measurement of non-equilibrium phonon occupations in femtosecond laser heated Au films

We use ultrafast electron diffraction to detect the temporal evolution of phonon populations in femtosecond laser-excited ultrathin single-crystalline gold films. From the time-dependence of the Debye-Waller factor we extract a 4.7 ps time-constant for the increase in mean-square atomic displacements. We show from the increase of the diffuse scattering intensity that the population of phonon modes near the X and K points in the Au fcc Brillouin zone grows with timescales of 2.3 and 2.9 ps, respectively, faster than the Debye-Waller average. We find that thermalization continues within the initially non-equilibrium phonon distribution after 10 ps. The observed momentum dependent timescale of phonon populations is in contrast to what is usually predicted in a two-temperature model.

cond-mat.mtrl-sci↗

arXiv2015

Generation of high-frequency strain waves during femtosecond demagnetization of Fe/MgO films

We use femtosecond time-resolved hard x-ray scattering to detect coherent acoustic phonons excited during ultrafast laser demagnetization of bcc Fe films. We determine the lattice strain propagating through the film through analysis of the oscillations in the x-ray scattering signal as a function of momentum transfer. The width of the strain wavefront is ~100 fs, similar to demagnetization timescales. First-principles calculations show that the high-frequency Fourier components of the strain, which give rise to the sharp wavefront, could in part originate from non-thermal dynamics of the lattice not considered in the two-temperature model.

cond-mat.mtrl-sci↗

arXiv2015

Direct observation and imaging of a spin-wave soliton with $p-$like symmetry

The prediction and realization of magnetic excitations driven by electrical currents via the spin transfer torque effect, enables novel magnetic nano-devices where spin-waves can be used to process and store information. The functional control of such devices relies on understanding the properties of non-linear spin-wave excitations. It has been demonstrated that spin waves can show both an itinerant character, but also appear as localized solitons. So far, it was assumed that localized solitons have essentially cylindrical, $s-$like symmetry. Using a newly developed high-sensitivity time-resolved magnetic x-ray microscopy, we instead observe the emergence of a novel localized soliton excitation with a nodal line, i.e. with $p-$like symmetry. Micromagnetic simulations identify the physical mechanism that controls the transition from $s-$ to $p-$like solitons. Our results suggest a potential new pathway to design artificial atoms with tunable dynamical states using nanoscale magnetic devices.

cond-mat.mes-hall↗

arXiv2015

Correlation-driven insulator-metal transition in near-ideal vanadium dioxide films

We use polarization- and temperature-dependent x-ray absorption spectroscopy, in combination with photoelectron microscopy, x-ray diffraction and electronic transport measurements, to study the driving force behind the insulator-metal transition in VO2. We show that both the collapse of the insulating gap and the concomitant change in crystal symmetry in homogeneously strained single-crystalline VO2 films are preceded by the purely-electronic softening of Coulomb correlations within V-V singlet dimers. This process starts 7 K (+/- 0.3 K) below the transition temperature, as conventionally defined by electronic transport and x-ray diffraction measurements, and sets the energy scale for driving the near-room-temperature insulator-metal transition in this technologically-promising material.

cond-mat.str-el↗

arXiv2010

Electron-phonon coupling and momentum-dependent electron dynamics in EuFe2As2 using time- and angle-resolved photoemission spectroscopy

The Fe pnictide parent compound EuFe2As2 exhibits a strongly momentum dependent carrier dynamics around the hole pocket at the center of the Brillouin zone. The very different dynamics of electrons and holes cannot be explained solely by intraband scattering and interband contributions have to be considered. In addition, three coherently excited modes at frequencies of 5.6, 3.1 and 2.4 THz are observed. An estimate of the electron-phonon coupling parameter reveals lambda < 0.5, suggesting a limited importance of e-ph coupling to superconductivity in Fe pnictides.

cond-mat.supr-con↗