arXiv subjects

Daniel Steil

Publications and source records attributed to Daniel Steil.

At least 19 recordsLinked to original sources

arXiv2026

The 2026 Skyrmionics Roadmap

Magnetic skyrmions and related topological spin textures have emerged as a central topic in condensed-matter physics, combining fundamental significance with potential for transformative applications in spintronics, magnonics, and beyond. Over the past decade, advances in material platforms, imaging techniques, theoretical modeling, and device concepts have established skyrmionics as a rapidly expanding field. At the same time, challenges remain in stabilizing, controlling, and integrating such textures into functional architectures, while novel phenomena such as antiskyrmions, higher-order skyrmions, hopfions, and antiferromagnetic textures arise. The 2026 Skyrmionics Roadmap represents a collective effort of many authors, providing a comprehensive perspective on the current state-of-the-art and the outlook for the coming years. In 33 focused sections, each co-authored by two researchers, we chart progress in theory and modeling, material systems, skyrmion dynamics, and skyrmion technologies. By offering a consolidated vision, this Roadmap aims to guide both fundamental research and application-driven efforts, accelerating the transition of skyrmionics from conceptual breakthroughs toward practical technologies.

cond-mat.mes-hall↗

arXiv2025

Controlling bubble and skyrmion lattice order and dynamics via stripe domain engineering in ferrimagnetic Fe/Gd multilayers

Ferrimagnetic Fe/Gd multilayers host maze-like stripe domains that transform into a disordered bubble/skyrmion lattice under out-of-plane magnetic fields at ambient temperature. Femtosecond magneto-optics distinguishes these textures via their distinct coherent breathing dynamics. Crucially, applying a brief in-plane ``set'' magnetic field to the stripe state enhances both frequency and amplitude of the bubble/skyrmion lattice breathing mode. Lorentz transmission electron microscopy, magnetic force microscopy, and micromagnetic simulations reveal that this enhancement arises from field-aligned stripes nucleating a dense, near-hexagonal bubble/skyrmion lattice upon out-of-plane field application, with strong indications for a pure skyrmion lattice. Thus, modifying the initial domain configuration by in-plane fields enables precise control of coherent magnetization dynamics on picosecond to nanosecond timescales and potentially even of topology.

cond-mat.mes-hall↗

arXiv2025

Femtosecond photocurrents by the Dresselhaus bulk spin-galvanic effect in an inversion-asymmetric ferromagnet

We study ultrafast photocurrents in thin films of a model ferromagnetic metal with broken bulk inversion symmetry, the half-metallic Heusler compound NiMnSb, following excitation with an optical pump pulse with photon energy 1.55 eV. Remarkably, in terms of the direction of the sample magnetization M, all photocurrents are found to be a superposition of a component with Rashba- and Dresselhaus-type symmetry. We explain the Dresselhaus bulk photocurrent as follows: Pump-induced electron heating induces an excess of spin {\mu}_s||M, which transfers spin angular momentum into states with Dresselhaus-type spin-momentum locking. The resulting charge current relaxes on a time scale of 10 fs by momentum relaxation and, thus, follows {\mu}_s quasi-instantaneously. The relaxation of {\mu}_s is governed by the cooling of the electrons and not by the significantly slower spin-lattice relaxation of half-metals. Our findings add the Dresselhaus spin-galvanic effect (SGE) to the set of ultrafast spin-charge-conversion phenomena. They indicate a route to more efficient spintronic terahertz emitters and detectors based on the volume scaling of the bulk SGE.

cond-mat.mtrl-sci↗

arXiv2025

The role of non-equilibrium populations in dark exciton formation

In two-dimensional transition metal dichalcogenide structures, the optical excitation of a bright exciton may be followed by the formation of a plethora of lower energy dark states. In these formation and relaxation processes between different exciton species, non-equilibrium exciton and phonon populations play a dominant role, but remain so far largely unexplored as most states are inaccessible by regular spectroscopies. Here, on the example of homobilayer 2H-MoS$_2$, we realize direct access to the full exciton relaxation cascade from experiment and theory. By measuring the energy- and in-plane momentum-resolved photoemission spectral function, we reveal a distinct fingerprint for dark excitons in a non-equilibrium excitonic occupation distribution. In excellent agreement with microscopic many-particle calculations, we quantify the timescales for the formation of a non-equilibrium dark excitonic occupation and its subsequent thermalization to 85~fs and 150~fs, respectively. Our results provide a previously inaccessible view of the complete exciton relaxation cascade, which is of paramount importance for the future characterization of non-equilibrium excitonic phases and the efficient design of optoelectronic devices based on two-dimensional materials.

cond-mat.mes-hall↗

arXiv2025

Table-top three-dimensional photoemission orbital tomography with a femtosecond extreme ultraviolet light source

Following electronic processes in molecules and materials at the level of the quantum mechanical electron wavefunction with angstrom-level spatial resolution and with full access to its femtosecond temporal dynamics is at the heart of ultrafast condensed matter physics. A breakthrough invention allowing experimental access to electron wavefunctions was the reconstruction of molecular orbitals from angle-resolved photoelectron spectroscopy data in 2009, termed photoemission orbital tomography (POT). This invention puts ultrafast three-dimensional (3D) POT in reach, with many new prospects for the study of ultrafast light-matter interaction, femtochemistry and photo-induced phase transitions. Here, we develop a synergistic experimental-algorithmic approach to realize the first 3D-POT experiment using a short-pulse extreme ultraviolet light source. We combine a new variant of photoelectron spectroscopy, namely ultrafast momentum microscopy, with a table-top spectrally-tunable high-harmonic generation light source and a tailored algorithm for efficient 3D reconstruction from sparse, undersampled data. This combination dramatically speeds up the experimental data acquisition, while at the same time reducing the sampling requirements to achieve complete 3D information. We demonstrate the power of this approach by full 3D imaging of the frontier orbitals of a prototypical organic semiconductor absorbed on pristine Ag(110).

cond-mat.mtrl-sci↗

arXiv2025

Pathways to Bubble and Skyrmion Lattice Formation in Fe/Gd Multilayers

The creation and control of magnetic spin textures is of great interest in fundamental research and future device-oriented applications. Fe/Gd multilayers host a rich variety of magnetic textures including topologically trivial bubbles and topologically protected skyrmions. Using time-resolved Kerr spectroscopy, we highlight how various control strategies, including temperature, out-of-plane magnetic fields and femtosecond light excitation, can be used to create such textures via different pathways. We find that varying the magnetic field for constant temperature leads to a different ($H, T$)-phase diagram of magnetic textures than moving along a temperature trajectory for constant magnetic field. Micromagnetic simulations corroborate this finding and allow to visualize the different paths taken. Furthermore, we show that the creation of bubbles and skyrmions in this material via impulsive light excitation is not solely governed by temperature-driven processes, since bubbles and skyrmions can be stabilized in parts of the ($H, T$)-phase diagram, where neither the constant temperature nor the constant magnetic field trajectory predict their existence. Using this phase diagram, we reason why bubble and skyrmion creation in this particular system is only possible from the stripe domain state. Our observations provide a versatile toolkit for tailoring the creation of magnetic spin textures in Fe/Gd multilayers.

cond-mat.mes-hall↗

arXiv2024

Hybrid Frenkel-Wannier excitons facilitate ultrafast energy transfer at a 2D-organic interface

Two-dimensional transition metal dichalcogenides (TMDs) and organic semiconductors (OSCs) have emerged as promising material platforms for next-generation optoelectronic devices. The combination of both is predicted to yield emergent properties while retaining the advantages of their individual components. In OSCs the optoelectronic response is typically dominated by localized Frenkel-type excitons, whereas TMDs host delocalized Wannier-type excitons. However, much less is known about the spatial and electronic characteristics of excitons at hybrid TMD/OSC interfaces, which ultimately determine the possible energy and charge transfer mechanisms across the 2D-organic interface. Here, we use ultrafast momentum microscopy and many-body perturbation theory to elucidate a hybrid exciton at an TMD/OSC interface that forms via the ultrafast resonant F\"orster energy transfer process. We show that this hybrid exciton has both Frenkel- and Wannier-type contributions: Concomitant intra- and interlayer electron-hole transitions within the OSC layer and across the TMD/OSC interface, respectively, give rise to an exciton wavefunction with mixed Frenkel-Wannier character. By combining theory and experiment, our work provides previously inaccessible insights into the nature of hybrid excitons at TMD/OSC interfaces. It thus paves the way to a fundamental understanding of charge and energy transfer processes across 2D-organic heterostructures.

cond-mat.mes-hall↗

arXiv2024

All optical control of bubble and skyrmion breathing

Controlling the dynamics of topologically protected spin objects by all optical means promises enormous potential for future spintronic applications. Excitation of bubbles and skyrmions in ferrimagnetic [Fe(0.35 nm)/Gd(0.40 nm)]$_{160}$ multilayers by ultrashort laser pulses leads to a periodic modulation of the core diameter of these spin objects, the so-called breathing mode. We demonstrate versatile amplitude and phase control of this breathing using a double excitation scheme, where the observed dynamics is controlled by the excitation delay. We gain insight into both the time scale on which the breathing mode is launched and the role of the spin object size on the dynamics. Our results demonstrate that ultrafast optical excitation allows for precise tuning of the spin dynamics of trivial and non-trivial spin objects, showing a possible control strategy in device applications.

cond-mat.mes-hall↗

arXiv2024

Observation of Floquet states in graphene

Recent advances in the field of condensed-matter physics have unlocked the potential to realize and control emergent material phases that do not exist in thermal equilibrium. One of the most promising concepts in this regard is Floquet engineering, the coherent dressing of matter via time-periodic perturbations. However, the broad applicability of Floquet engineering to quantum materials is still unclear. For the paradigmatic case of monolayer graphene, the theoretically predicted Floquet-induced effects, despite a seminal report of the light-induced anomalous Hall effect, have been put into question. Here, we overcome this problem by using electronic structure measurements to provide direct experimental evidence of Floquet engineering in graphene. We report light-matter-dressed Dirac bands by measuring the contribution of Floquet sidebands, Volkov sidebands, and their quantum path interference to graphene's photoemission spectral function. Our results finally demonstrate that Floquet engineering in graphene is possible, paving the way for the experimental realization of the many theoretical proposals on Floquet-engineered band structures and topological phases.

cond-mat.mes-hall↗

arXiv2023

Dynamics of electronic phase separation at the laser-induced insulator-metal transition in (La$_{0.6}$Pr$_{0.4}$)$_{0.7}$Ca$_{0.3}$MnO$_3$

Ultrafast optical excitations allow creating new metastable and hidden states in quantum materials. However, the fundamental material properties required to support new emergent order are largely unknown. Here we show for two colossal magnetoresistive (CMR) manganites that electronic phase separation (EPS) strongly favors non-thermal behavior and exploit this to stabilize an optically-induced conducting state. Our results shed light on the role of EPS in optical control of CMR manganites and provide guidance for the design of materials that can exhibit non-equilibrium states of matter.

cond-mat.str-el↗

arXiv2023

Laser-induced real-space topology control of spin wave resonances

Femtosecond laser excitation of materials that exhibit magnetic spin textures promises advanced magnetic control via the generation of ultrafast and non-equilibrium spin dynamics. We explore such possibilities in ferrimagnetic [Fe(0.35 nm)/Gd(0.40 nm)]$_{160}$ multilayers, which host a rich diversity of magnetic textures from stripe domains at low magnetic fields, a dense bubble/skyrmion lattice at intermediate fields, and a single domain state for high magnetic fields. Using femtosecond magneto-optics, we observe distinct coherent spin wave dynamics in response to a weak laser excitation allowing us to unambiguously identify the different magnetic spin textures. Moreover, employing strong laser excitation we show that we achieve versatile control of the coherent spin dynamics via non-equilibrium and ultrafast transformation of magnetic spin textures by both creating and annihilating bubbles/skyrmions. We corroborate our findings by micromagnetic simulations and by Lorentz transmission electron microscopy before and after laser exposure.

cond-mat.mtrl-sci↗

arXiv2023

Verification of ultrafast spin transfer effects in FeNi alloys

The optical intersite spin transfer (OISTR) effect was recently verified in Fe$_{50}$Ni$_{50}$ using magneto-optical Kerr measurements in the extreme ultraviolet range. However, one of the main experimental signatures analyzed in this work, namely a magnetic moment increase at a specific energy in Ni, was subsequently found also in pure Ni, where no transfer from one element to another is possible. Hence, it is a much-discussed issue whether OISTR in FeNi alloys is real and whether it can be verified experimentally or not. Here, we present a comparative study of spin transfer in Fe$_{50}$Ni$_{50}$, Fe$_{19}$Ni$_{81}$ and pure Ni. We conclusively show that an increase in the magneto-optical signal is indeed insufficient to verify OISTR. However, we also show how an extended data analysis overcomes this problem and allows to unambiguously identify spin transfer effects. Concomitantly, our work solves the long-standing riddle about the origin of delayed demagnetization behavior of Ni in FeNi alloys.

cond-mat.mtrl-sci↗

arXiv2023

Unraveling Femtosecond Spin and Charge Dynamics with EUV T-MOKE Spectroscopy

The magneto-optical Kerr effect (MOKE) in the extreme ultraviolet (EUV) regime has helped to elucidate some of the key processes that lead to the manipulation of magnetism on ultrafast timescales. However, as we show in this paper, the recently introduced spectrally-resolved analysis of such data can lead to surprising experimental observations, which might cause misinterpretations. Therefore, an extended analysis of the EUV magneto-optics is necessary. Via experimental determination of the dielectric tensor, we find here that the non-equilibrium excitation in an ultrafast magnetization experiment can cause a rotation of the off-diagonal element of the dielectric tensor in the complex plane. In direct consequence, the commonly analyzed magneto-optic asymmetry may show time-dependent behaviour that is not directly connected to the magnetic properties of the sample. We showcase such critical observations for the case of ultrafast magnetization dynamics in Ni, and give guidelines for the future analysis of spectrally-resolved magneto-optical data and its comparison with theory.

cond-mat.mtrl-sci↗

arXiv2023

Ultrafast nano-imaging of dark excitons

The role and impact of spatial heterogeneity in two-dimensional quantum materials represents one of the major research quests regarding the future application of these materials in optoelectronics and quantum information science. In the case of transition-metal dichalcogenide heterostructures, in particular, direct access to heterogeneities in the dark-exciton landscape with nanometer spatial and ultrafast time resolution is highly desired, but remains largely elusive. Here, we introduce ultrafast dark field momentum microscopy to spatio-temporally resolve dark exciton formation dynamics in a twisted WSe$_2$/MoS$_2$ heterostructure with 55 femtosecond time- and 500~nm spatial resolution. This allows us to directly map spatial heterogeneity in the electronic and excitonic structure, and to correlate these with the dark exciton formation and relaxation dynamics. The benefits of simultaneous ultrafast nanoscale dark-field momentum microscopy and spectroscopy is groundbreaking for the present study, and opens the door to new types of experiments with unprecedented spectroscopic and spatiotemporal capabilities.

cond-mat.mes-hall↗

arXiv2023

Ultrafast dynamics of bright and dark excitons in monolayer WSe$_2$ and heterobilayer WSe$_2$/MoS$_2$

The energy landscape of optical excitations in mono- and few-layer transition metal dichalcogenides (TMDs) is dominated by optically bright and dark excitons. These excitons can be fully localized within a single TMD layer, or the electron- and the hole-component of the exciton can be charge-separated over multiple TMD layers. Such intra- or interlayer excitons have been characterized in detail using all-optical spectroscopies, and, more recently, photoemission spectroscopy. In addition, there are so-called hybrid excitons whose electron- and/or hole-component are delocalized over two or more TMD layers, and therefore provide a promising pathway to mediate charge-transfer processes across the TMD interface. Hence, an in-situ characterization of their energy landscape and dynamics is of vital interest. In this work, using femtosecond momentum microscopy combined with many-particle modeling, we quantitatively compare the dynamics of momentum-indirect intralayer excitons in monolayer WSe$_2$ with the dynamics of momentum-indirect hybrid excitons in heterobilayer WSe$_2$/MoS$_2$, and draw three key conclusions: First, we find that the energy of hybrid excitons is reduced when compared to excitons with pure intralayer character. Second, we show that the momentum-indirect intralayer and hybrid excitons are formed via exciton-phonon scattering from optically excited bright excitons. And third, we demonstrate that the efficiency for phonon absorption and emission processes in the mono- and the heterobilayer is strongly dependent on the energy alignment of the intralayer and hybrid excitons with respect to the optically excited bright exciton. Overall, our work provides microscopic insights into exciton dynamics in TMD mono- and bilayers.

cond-mat.mes-hall↗

arXiv2023

Probing correlations in the exciton landscape of a moir\'e heterostructure

Excitons are two-particle correlated bound states that are formed due to Coulomb interaction between single-particle holes and electrons. In the solid-state, cooperative interactions with surrounding quasiparticles can strongly tailor the exciton properties and potentially even create new correlated states of matter. It is thus highly desirable to access such cooperative and correlated exciton behavior on a fundamental level. Here, we find that the ultrafast transfer of an exciton's hole across a type-II band-aligned moir\'e heterostructure leads to a surprising sub-200-fs upshift of the single-particle energy of the electron being photoemitted from the two-particle exciton state. While energy relaxation usually leads to an energetic downshift of the spectroscopic signature, we show that this unusual upshift is a clear fingerprint of the correlated interactions of the electron and hole parts of the exciton quasiparticle. In this way, time-resolved photoelectron spectroscopy is straightforwardly established as a powerful method to access exciton correlations and cooperative behavior in two-dimensional quantum materials. Our work highlights this new capability and motivates the future study of optically inaccessible correlated excitonic and electronic states in moir\'e heterostructures.

cond-mat.mtrl-sci↗

arXiv2023

Multiorbital exciton formation in an organic semiconductor

Harnessing the optoelectronic response of organic semiconductors requires a thorough understanding of the fundamental light-matter interaction that is dominated by the excitation of correlated electron-hole pairs, i.e. excitons. The nature of these excitons would be fully captured by knowing the quantum-mechanical wavefunction, which, however, is difficult to access both theoretically and experimentally. Here, we use femtosecond photoemission orbital tomography in combination with many-body perturbation theory to gain access to exciton wavefunctions in organic semiconductors. We find that the coherent sum of multiple electron-hole pair contributions that typically make up a single exciton can be experimentally evidenced by photoelectron spectroscopy. For the prototypical organic semiconductor buckminsterfullerene (C$_{60}$), we show how to disentangle such multiorbital contributions and thereby access key properties of the exciton wavefunctions including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.

cond-mat.mes-hall↗

arXiv2021

Formation of moir\'e interlayer excitons in space and time

Moir\'e superlattices in atomically thin van-der-Waals heterostructures hold great promise for an extended control of electronic and valleytronic lifetimes, the confinement of excitons in artificial moir\'e lattices, and the formation of novel exotic quantum phases. Such moir\'e-induced emergent phenomena are particularly strong for interlayer excitons, where the hole and the electron are localized in different layers of the heterostructure. In order to exploit the full potential of correlated moir\'e and exciton physics, a thorough understanding of the ultrafast interlayer exciton formation process and the real-space wavefunction confinement in the moir\'e potential is indispensable. However, direct experimental access to these parameters is limited since most excitonic quasiparticles are optically dark. Here we show that femtosecond photoemission momentum microscopy provides quantitative access to these key properties of the moir\'e interlayer excitons. We find that interlayer excitons are dominantly formed on the sub-50~fs timescale via interlayer tunneling at the K valleys of the Brillouin zones. In addition, we directly measure energy-momentum fingerprints of the moir\'e interlayer excitons by mapping their spectral signatures within the mini Brillouin zone that is built up by the twisted heterostructure. From these momentum-fingerprints, we gain quantitative access to the modulation of the exciton wavefunction within the moir\'e potential in real-space. Our work provides the first direct access to the interlayer moir\'e exciton formation dynamics in space and time and reveals new opportunities to study correlated moir\'e and exciton physics for the future realization of exotic quantum phases of matter.

cond-mat.mes-hall↗