arXiv subjects

Stefan Mathias

Publications and source records attributed to Stefan Mathias.

At least 19 recordsLinked to original sources

arXiv2026

Ultrafast order-selective electron imaging and spectroscopy

Ultrafast pump-probe spectroscopies in energy and momentum have become indispensable for probing non-equilibrium dynamics in quantum materials, revealing pathways in ultrafast energy conversion and light-induced phase transitions. Different modalities uniquely access the coupled lattice, charge, and spin degrees of freedom that underpin the functionality of these materials. However, investigating technologically relevant nanoscale devices also requires high spatial resolution. Although electron microscopy provides nanometer-scale imaging, it frequently lacks the simultaneous ultrafast temporal resolution and spectroscopic specificity needed for such studies. In this perspective, we review recent advances in dark-field electron and photoelectron microscopy, focusing on two complementary techniques: femtosecond photoelectron momentum microscopy and ultrafast transmission electron microscopy. Their application enables comprehensive insights into the ultrafast dynamics of the electron, lattice, and spin subsystems. These order-selective electron imaging and spectroscopy techniques open broad scientific opportunities for a microscopic understanding of non-equilibrium phenomena in quantum materials, nanostructures and devices.

cond-mat.mtrl-sci↗

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↗

arXiv2026

A comparative study of perturbative and nonequilibrium Green's function approaches for Floquet sidebands in periodically driven quantum systems

We compare two complementary theoretical approaches to compute and interpret Floquet sidebands in periodically driven quantum materials: a first-order perturbative approach (first-order perturbative Born approximation, PB1) and time-dependent nonequilibrium Green's functions (tdNEGF). Using graphene as a model Dirac system, we disentangle in pump-probe setups Floquet-dressed initial states, Volkov-dressed final states (also known as laser-assisted photoelectric effect, LAPE), and their interference. We quantify how photoemission matrix elements, polarization, incidence angle, and near-surface screening shape the momentum-resolved sideband intensity observed in tr-ARPES. PB1 yields an analytical expression for the momentum-dependent sideband intensity, and for graphene it captures the correct symmetry trends, such as the magnitude of the intensities when considering the interference between the Floquet and Volkov states and photoemission matrix elements. tdNEGF reproduces the full energy-momentum-resolved spectra, including hybridization gaps and spectral-weight redistribution. We find qualitative agreement between PB1 and tdNEGF once matrix elements are included; quantitative differences arise near hybridization regions and at specific angles where higher-order processes and self-energies are essential. Thus, for systems with simple band structures and away from these regions, the two approaches can be used in a complementary way.

cond-mat.mes-hall↗

arXiv2025

Nonvolatile photoswitching of a Mott state via reversible stacking rearrangement

Nonvolatile control of the Mott transition is a central goal in correlated-electron physics, offering access to fascinating emergent states and great potential for technological applications. Compared to chemical or mechanical approaches, ultrafast optical excitation further promises a path to create and manipulate novel non-equilibrium phases with ultimate spatiotemporal precision. However, achieving a truly nonvolatile electronic phase transition in laser-excited Mott systems remains an elusive challenge. Here, we present a highly robust and reversible method for optical control of the Mott state in van der Waals systems. Specifically, using angle-resolved photoemission spectroscopy, we observe a nonvolatile Mott-to-metallic transition in the ultrafast laser-excited charge density wave (CDW) material 1T-TaSe2. Complementary theoretical calculations reveal that this transition originates from a rearrangement of the interlayer CDW stacking. This new stacking order, formed following the ultrafast quenching of the CDW, circumvents the need for large-scale atomic sliding. Intriguingly, it introduces a significant in-plane component to the electron hopping and effectively reduces the ratio of on-site Coulomb interaction to bandwidth, thereby suppressing the Mott state and stabilizing a metallic phase. Our results establish optical-control of interlayer stacking as a versatile strategy for inducing nonvolatile phase transitions, opening a new route to tailor correlated electronic phases and realize reconfigurable high-frequency devices.

cond-mat.str-el↗

arXiv2025

ARPES signatures of trions in van der Waals materials

Angle-resolved photoemission spectroscopy (ARPES) has recently emerged as a direct probe of excitonic correlations in two-dimensional semiconductors, resolving their dispersion and dynamics in energy-momentum space, including dark exciton states inaccessible to optical techniques. However, the ARPES fingerprint of charged excitons (trions), which plays a key role in all doped and gated 2D material systems, has remained unknown so far. We present a first theoretical analysis of trion signatures in monolayer transition-metal dichalcogenides, highlighting how the additional charge carrier modifies the spectral position and shape relative to neutral excitons in ARPES spectra. Interestingly, we further predict that mass-imbalanced trions yield a characteristic double-peak structure, clearly separated in energy and line shape from neutral excitons. The predicted temperature dependence of these features offers guidance for experimental investigations aimed at identifying trionic states, thereby establishing a framework for ARPES studies of many-body Coulomb complexes in doped two-dimensional semiconductors.

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

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

Algorithmic approaches to avoiding bad local minima in nonconvex inconsistent feasibility

We report on the use of algorithms to avoid or move away from ``bad'' local minima in nonconvex optimization. Our study is phenomenological and empirical, focusing on the performance of cyclic projections, the cyclic relaxed Douglas-Rachford algorithm, and relaxed Douglas-Rachford splitting on the product space for orbital tomographic imaging from angle-resolved photon emission spectroscopy (ARPES) measurements, with both synthetic and laboratory data. Cyclic projections and Douglas-Rachford on the product space are both well-known methods, but cyclic relaxed Douglas-Rachford was only recently fully characterized in a companion paper to the present study. Only one other study of note has investigated the performance of all three of these algorithms for inconsistent nonconvex feasibility. We show that the relaxed Douglas-Rachford algorithm on the product space, while exhibiting very poor convergence rates, can be used to filter out bad local minima from all cyclic algorithms. Our numerical experiments lead to the following recommendation: run cyclic projections to find some fixed point, and from this fixed point run relaxed Douglas-Rachford algorithm on the product space with as large a relaxation parameter as is numerically stable in order to escape poor local minima. This advice runs counter to the current practice for phase retrieval, where a Douglas-Rachford-type algorithm is run for several iterations, and then cyclic projections is used to ``clean up'' the images.

math.OC↗

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

Interlayer charge transfer in graphene 2D polyimide heterostructures

The vertical integration of multiple two-dimensional (2D) materials in heterostructures, held together by van der Waals forces, has opened unprecedented possibilities for modifying the (opto-)electronic properties of nanodevices. Graphene, with its remarkable opto-electronic properties, is an ideal candidate for such applications. Further candidates are 2D polymers, crystalline polymeric materials with customizable structure and electronic properties that can be synthesized in all mathematically possible Bravais lattices. In this study, we investigated the optoelectronic properties of a heterostructure created by pristine graphene and a rectangular 2D polyimide (2DPI) film. This imprints a new superlattice on graphene in conjunction with a direct influence on its electronic properties. Theoretical and experimental analyses reveal that interlayer charge exchange between the 2D polymer and graphene induces hole doping in the graphene layer. We have also observed that the properties of the heterostructure are dependent on the substrate used in experiments, likely due to the porous character of the 2DPI allowing direct interaction of graphene with the support. These findings highlight the unique ability to tailor functionalities in 2D polymers-based heterostructures, allowing the development of optoelectronic devices with precisely engineered properties and stimulating further exploration of the diverse phenomena accessible through tailored designs of the 2D polymers.

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↗

arXiv2024

Fast spectroscopic imaging using extreme ultraviolet interferometry

Extreme ultraviolet pulses as generated by high harmonic generation (HHG) are a powerful tool for both time-resolved spectroscopy and coherent diffractive imaging. However, the integration of spectroscopy and microscopy to harness the unique broadband spectra provided by HHG is hardly explored due to the challenge to decouple spectroscopic and microscopic information. Here, we present an interferometric approach to this problem that combines Fourier transform spectroscopy (FTS) with Fourier transform holography (FTH). This is made possible by the generation of phase-locked pulses using a pair of HHG sources. Crucially, in our geometry the number of interferometric measurements required is at most equal to the number of high harmonics in the illumination, and can be further reduced by incorporating prior knowledge about the structure of the FTH sample. Compared to conventional FTS, this approach achieves over an order of magnitude increase in acquisition speed for full spectro-microscopic data, and furthermore allows diffraction-limited computational imaging.

physics.optics↗

arXiv2024

Probing excitons with time-resolved momentum microscopy

Excitons -- two-particle correlated electron-hole pairs -- are the dominant low-energy optical excitation in the broad class of semiconductor materials, which range from classical silicon to perovskites, and from two-dimensional to organic materials. Recently, the study of excitons has been brought on a new level of detail by the application of photoemission momentum microscopy -- a technique that has dramatically extended the experimental capabilities of time- and angle-resolved photoemission spectroscopy (trARPES). Here, we review how the energy- and momentum-resolved photoelectron detection scheme enables direct access to the energy landscape of bright and dark excitons, and, more generally, to the momentum-coordinate of the exciton that is fundamental to its wavefunction. Focusing on two-dimensional materials and organic semiconductors as two tuneable platforms for exciton physics, we first discuss the typical photoemission fingerprint of excitons in momentum microscopy and highlight that is is possible to obtain information not only on the electron- but also hole-component of the former exciton. Second, we focus on the recent application of photoemission orbital tomography to such excitons, and discuss how this provides a unique access to the real-space properties of the exciton wavefunction. Throughout the review, we detail how studies performed on two-dimensional transition metal dichalcogenides and organic semiconductors lead to very similar conclusions, and, in this manner, highlight the strength of time-resolved momentum microscopy for the study of optical excitations in semiconductors.

cond-mat.mtrl-sci↗

arXiv2024

A minimalist approach to 3D photoemission orbital tomography: algorithms and data requirements

Photoemission orbital tomography provides direct access from laboratory measurements to the real-space molecular orbitals of well-ordered organic semiconductor layers. Specifically, the application of phase retrieval algorithms to photon-energy- and angle-resolved photoemission data enables the direct reconstruction of full 3D molecular orbitals without the need for simulations using density functional theory or the like. A major limitation for the direct approach has been the need for densely-sampled, well-calibrated 3D photoemission patterns. Here, we present an iterative projection algorithm that completely eliminates this challenge: for the benchmark case of the pentacene frontier orbitals, we demonstrate the reconstruction of the full orbital based on a dataset containing only four simulated photoemission momentum measurements. We discuss the algorithm performance, sampling requirements with respect to the photon energy, optimal measurement strategies, and the accuracy of orbital images that can be achieved.

cond-mat.mtrl-sci↗

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↗