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Stefan Eisebitt

Publications and source records attributed to Stefan Eisebitt.

At least 19 recordsLinked to original sources

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↗

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↗

Emergent Chaos-Like Dynamics of Spin-Orbit Torque-Driven Magnetic Transitions

Spin-orbit torques (SOTs) are widely used to control magnetization in nanoscale electric systems and are typically assumed to drive skyrmion nucleation and motion in a deterministic manner, especially in materials with strong Dzyaloshinskii-Moriya interaction. Here, using time-resolved holography-based x-ray microscopy supported by micromagnetic simulations, we reveal that on nano- to picosecond timescales the actual dynamics can deviate strikingly from this expectation by producing transient regimes of chaos-like behavior. By exploiting deterministic skyrmion generation at an anisotropy-engineered defect and implementing a high-resolution pump-probe scheme, we directly track the magnetization evolution in real space. This approach uncovers a dynamic phase transition that separates coherent SOT-driven motion from a regime of transient instability characterized by picosecond-scale fluctuations, strong domain disorder, topological instabilities, and skyrmion shedding, experimentally observed here for the first time. During SOT actuation, the system briefly enters this instability regime, showing short-lived chaos-like behavior, yet it reliably relaxes into robust and reproducible final states. Our results demonstrate a powerful methodology for accessing time-averaged nano- to picosecond dynamics in magnetic systems and reveal a previously hidden layer of transient, topologically rich behavior underlying nominally deterministic skyrmion control.

cond-mat.mes-hall↗

Soft-X-ray momentum microscopy of nonlinear magnon interactions below 100-nm wavelength

Magnons are quantised collective excitations of long-range ordered spins. At nanometre wavelengths, exchange interactions increasingly govern their dynamics, giving rise to a largely unexplored regime of couplings between magnons and other quasiparticles. Yet, detecting such short-wavelength spin waves has remained a key experimental challenge. Here, we introduce Magnon Momentum Microscopy (MMM) -- a quasi-elastic, resonant magnetic soft-X-ray scattering technique that directly images magnon populations across two-dimensional momentum space. Owing to its remarkable sensitivity, MMM can capture nonlinear magnon-magnon interactions over large regions of the dispersion plane. Applying MMM to the prototypical magnonic material yttrium iron garnet (YIG), we uncover a rich variety of previously unobserved nonlinear magnon interactions. With its element specificity, bulk sensitivity, as well as intrinsic access to nanometre-scale wavelengths without frequency limitation, soft-X-ray MMM establishes a powerful and versatile platform for exploring short-wavelength and nonlinear magnonics.

cond-mat.mes-hall↗

A fluctuation-free pathway for a topological magnetic phase transition

Topological magnetic textures are particle-like spin configurations stabilized by competing interactions. Their formation is commonly attributed to fluctuation-driven, first-order nucleation processes requiring activation over a topological energy barrier. Here, we demonstrate an alternative barrier- and fluctuation-free pathway for nucleating topological magnetic textures, triggered in our experiments by an excitation-induced spin reorientation transition. By combining x-ray imaging, scattering and micromagnetic simulations, we show that the system follows a deterministic cascade of symmetry-breaking phase transitions after excitation. First, the system undergoes a second-order phase transition from a homogeneous state to weak stripe domains, then a first-order transition to topologically trivial bubbles, and finally a topological switching event into skyrmionic textures. Through simulations, we generalize our findings and demonstrate that this pathway is active in a vast range of low-anisotropy materials. This previously unrecognized, spontaneous transition pathway suggests strategies for rapid, low-energy generation of topological spin textures and points to a general role of intrinsic modulational instabilities in phase transitions beyond magnetism.

cond-mat.mtrl-sci↗

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↗

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↗

Laser-driven resonant soft-X-ray scattering for probing picosecond dynamics of nanometre-scale order

X-ray scattering has been an indispensable tool in advancing our understanding of matter, from the first evidence of the crystal lattice to recent discoveries of nuclei's fastest dynamics. In addition to the lattice, ultrafast resonant elastic scattering of soft X-rays provides a sensitive probe of charge, spin, and orbital order with unparalleled nanometre spatial and femto- to picosecond temporal resolution. However, the full potential of this technique remains largely unexploited due to its high demand on the X-ray source. Only a selected number of instruments at large-scale facilities can deliver the required short-pulsed and wavelength-tunable radiation, rendering laboratory-scale experiments elusive so far. Here, we demonstrate time-resolved X-ray scattering with spectroscopic contrast at a laboratory-based instrument using the soft-X-ray radiation emitted from a laser-driven plasma source. Specifically, we investigate the photo-induced response of magnetic domains emerging in a ferrimagnetic heterostructure with 9$\,$ps temporal resolution. The achieved sensitivity allows for tracking the reorganisation of the domain network on pico- to nanosecond time scales in great detail. This instrumental development and experimental demonstration break new ground for studying material dynamics in a wide range of laterally ordered systems in a flexible laboratory environment.

cond-mat.mes-hall↗

Ultrafast X-ray sonography reveals the spatial heterogeneity of the laser-induced magneto-structural phase transition in FeRh

Phase transitions are governed by both intrinsic and extrinsic heterogeneities, yet capturing their spatio-temporal dynamics remains a challenge. While ultrafast techniques track phase changes on femtosecond timescales, the spatial complexity and stochastic nature of the processes often remain hidden. Here, we present an experimental approach that combines well-established ultrafast hard-X-ray diffraction with a propagating strain pulse as a universal and non-invasive probe. This ultrafast X-ray sonography can capture the spatio-temporal phase heterogeneity in great detail by resolving the phase-specific strain response. We apply this approach to the antiferromagnetic-to-ferromagnetic magneto-structural phase transition in FeRh and identify the ferromagnetic phase to nucleate at the surface as narrow columnar domains of approximately $30\,\text{nm}$ diameter. Besides reconciling the diverse experimental results in the literature on FeRh, X-ray sonography offers a versatile platform for investigating a wide range of phase transitions accompanied by structural changes.

cond-mat.mtrl-sci↗

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↗

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↗

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↗

Soft X-ray imaging with coherence tomography in the water window spectral range using high-harmonic generation

High-harmonic generation (HHG) is used as a source for various imaging applications in the extreme ultraviolet spectral range. It offers spatially coherent radiation and unique elemental contrast with the potential for attosecond time resolution. The unfavorable efficiency scaling to higher photon energies prevented the imaging application in the soft X-ray range so far. In this work we demonstrate the feasibility of using harmonics for imaging in the water window spectral region (284$\,$eV to 532$\,$eV). We achieve nondestructive depth profile imaging in a heterostructure by utilizing a broadband and noise-resistant technique called soft X-ray Coherence Tomography (SXCT) at a high-flux lab-scale HHG source. SXCT is derived from Optical Coherence Tomography, a Fourier based technique, that can use the full bandwidth of the source to reach an axial resolution of 12$\,$nm in this demonstration. The employed source covers the entire water window, with a photon flux exceeding 10$^\text{6}\,$photons/eV/s at a photon energy of 500$\,$eV. We show local cross sections of a sample consisting of Aluminium oxide and Platinum layers of varying thickness on a Zinc oxide substrate. We validate the findings with scanning and transmission electron microscopy after preparation with focused ion beam milling.

physics.optics↗

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↗

Ultrafast energy-dispersive soft-x-ray diffraction in the water window with a laser-driven source

Time-resolved soft-x-ray-diffraction experiments give access to microscopic processes in a broad range of solid-state materials by probing ultrafast dynamics of ordering phenomena. While laboratory-based high-harmonic generation (HHG) light sources provide the required photon energies, their limited photon flux is distributed over a wide spectral range, rendering typical monochromatic diffraction schemes challenging. Here, we present a scheme for energy-dispersive soft-x-ray diffraction with femtosecond temporal resolution and photon energies across the water window from 200 to 600 eV. The experiment utilizes the broadband nature of the HHG emission to efficiently probe large slices in reciprocal space. As a proof-of-concept, we study the laser-induced structural dynamics of a Mo/Si superlattice in an ultrafast, non-resonant soft-x-ray diffraction experiment. We extract the underlying strain dynamics from the measured shift of its first order superlattice Bragg peak in reciprocal space at photon energies around 500 eV via soft-x-ray scattering simulations.

physics.optics↗

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↗

Coherent x-ray magnetic imaging with 5 nm resolution

Soft x-ray microscopy plays an important role in modern spintronics. However, the achievable resolution of most x-ray magnetic imaging experiments is above 10 nm, limiting access to fundamental and technologically relevant length scales. Here, we demonstrate x-ray magnetic microscopy with 5 nm resolution by combining holography-assisted coherent diffractive imaging with heterodyne amplification of the weak magnetic signal. The gain in resolution and contrast allows direct access to key magnetic properties, including domain wall profiles and the position of pinning sites. The ability to detect and map such properties with photons opens new horizons for element-specific, time-resolved, and in-operando research on magnetic materials and beyond.

cond-mat.mtrl-sci↗

Three-dimensional coherent diffraction snapshot imaging using extreme ultraviolet radiation from a free electron laser

The possibility to obtain a three-dimensional representation of a single object with sub-$μ$m resolution is crucial in many fields, from material science to clinical diagnostics. This is typically achieved through tomography, which combines multiple two-dimensional images of the same object captured at different orientations. However, this serial imaging method prevents single-shot acquisition in imaging experiments at free electron lasers. In the present experiment, we report on a new approach to 3D imaging using extreme-ultraviolet radiation. In this method, two EUV pulses hit simultaneously an isolated 3D object from different sides, generating independent coherent diffraction patterns, resulting in two distinct bidimensional views obtained via phase retrieval. These views are then used to obtain a 3D reconstruction using a ray tracing algorithm. This EUV stereoscopic imaging approach, similar to the natural process of binocular vision, provides sub-$μ$m spatial resolution and single shot capability. Moreover, ultrafast time resolution and spectroscopy can be readily implemented, a further extension to X-ray wavelengths can be envisioned as well.

physics.optics↗