arXiv subjects

F. Stefan Tautz

Publications and source records attributed to F. Stefan Tautz.

At least 19 recordsLinked to original sources

arXiv2026

Giant orbital Zeeman effects in a magnetic topological van der Waals interphase

Van der Waals (vdW) heterostructures allow the engineering of magnetic and electronic properties via interfacial orbital hybridisation and charge transfer. The resulting electric fields can give rise to Rashba spin-orbit coupling and Dzyaloshinskii-Moriya interactions, which may stabilise novel two-dimensional magnetic phases. While such emergent magnetic 'interphases' may offer a promising platform for spin-based electronics, direct spectroscopic evidence for them is still lacking. Here, we report electric-field tunable Zeeman effects with Landé $g$-factors up to $\approx230$ at the interface of graphene and the vdW ferromagnet Fe$_3$GeTe$_2$. They arise from an interplay of local-moment canting and the itinerant orbital moments of Fe$_3$GeTe$_2$, producing a giant asymmetric level splitting. Exploiting the inelastic phonon gap of graphene, scanning tunnelling spectroscopy allows us to access the buried interface properties, and quantify Faraday-like screening. Our findings provide new insights and opportunities for electrically controlled interface magnetism, e.g. for spintronics and orbitronics devices.

cond-mat.mes-hall↗

arXiv2026

Highly crystalline superconducting TiN resonators grown on thermally reconstructed sapphire

High quality crystalline growth of a thin film on sapphire requires sufficient substrate preparation, often achieved via the use of aggressive chemical cleaning. Direct thermal reconstruction of the sapphire substrate via a CO$_2$ laser beam may allow for an alternative way to prepare the substrate for epitaxy without the use of any chemical processing. Within this work, we demonstrate that thermal annealing of sapphire into its ($\sqrt{31}$$\times$$\sqrt{31}$)$R$$\pm$9° reconstruction is a valid alternative preparation technique for sapphire substrates. TiN films grown via plasma-assisted molecular beam epitaxy upon these substrates exhibit greater crystallinity than those grown on chemically cleaned sapphire substrates. Superconducting resonators fabricated from these films exhibit similar performance, with many possessing internal quality factors at single photon levels greater than 10$^6$ for both substrate preparation methods.

cond-mat.supr-con↗

arXiv2026

A miniature evaporator for in-operando deposition of isolated atoms in a low-temperature scanning tunneling microscope

Depositing dilute atomic ensembles onto cold samples is challenging in low-temperature scanning tunneling microscopes (STM) because radiation shields and restricted internal geometries often preclude a direct deposition path, particularly in instruments designed for millikelvin operation. We present a compact, milliwatt-range evaporation source fabricated from a commercial miniature incandescent lamp and integrated directly into a millikelvin STM head. The exposed tungsten filament is coated with a micrometre-thick Fe film and positioned about 1 cm from the sample. We deposit isolated Fe atoms onto MgO/Ag(100) while operating the microscope near 5 K. Evaporation increases the STM-body temperature by only about 2 K, and the same nanoscopic surface region can be readily scanned after deposition with a lateral displacement of less than 5 nm. Differential-conductance spectra displaying symmetric inelastic steps near $\pm$14 mV identify the deposited atoms on MgO as Fe. From STM images, we estimate a local deposition flux of $1.5\times10^{-5}~\mathrm{nm^{-2}\,s^{-1}}$, corresponding to a nominal evaporator lifetime of ~150 h. The fixed evaporator enables repeated low-flux deposition without a room-temperature line of sight, the need for movable radiation shields, or mechanical evaporator access after cooldown, while preserving access to the same atomic-scale surface region before and after deposition.

cond-mat.mes-hall↗

arXiv2026

Contactless terahertz mapping of wafer-scale superconducting NbTiN thin films

For large-scale superconducting quantum technology, e.g. quantum computing, the homogeneity of wafer-scale superconducting thin films is vital for consistent performance of the fabricated devices. Terahertz (THz) spectroscopy as a contactless and non-destructive measurement technique is a powerful tool to characterize the superconducting films. In this work, a set of niobium titanium nitride (NbTiN) thin films on 4-inch and 6-inch silicon wafers, grown via plasma-enhanced magnetron sputtering, are investigated via THz spectroscopy: full wafers are mapped at room temperatures and exemplary segments are characterized at cryogenic temperatures. The deviations in observed sheet resistance depend on the used deposition device and the film thickness. While the deviations in superconducting sheet kinetic inductance match those of the normal-state sheet resistance, the critical temperature and energy gap exhibit little variation. This THz mapping technique demonstrates the feasibility of evaluating wafer-scale superconducting thin films before lithography, facilitating preparation of the thin films for reproducible device fabrication.

cond-mat.supr-con↗

arXiv2026

Imaging the transition from diffusive to Landauer resistivity dipoles

A point-like defect in a uniform current-carrying conductor induces a dipole in the electrochemical potential, which counteracts the original transport field. If the mean free path of the carriers is much smaller than the size of the defect, the dipole results from the purely diffusive motion of the carriers around the defect. In the opposite limit, ballistic carriers scatter from the defect -- for this situation, Rolf Landauer postulated the emergence of residual resistivity dipoles that are independent of the defect size and thus impose a fundamental limit on the resistance of the parent conductor. Here, we study resistivity dipoles around holes of different sizes in two-dimensional Bi films on Si(111). Using scanning tunneling potentiometry to image the dipoles, we find a crossover from linear to constant scaling behavior of their amplitudes with defect size, manifesting the transition from diffusive to Landauer dipoles. The extracted parameters of the transition allow us to estimate the Fermi wave vector and the carrier mean free path in our Bi films.

cond-mat.mes-hall↗

arXiv2026

Circular dichroism in the photoelectron angular distribution of achiral molecules

Circular dichroism in the angular distribution (CDAD) is the effect that the angular intensity distribution of photoemitted electrons depends on the handedness of the incident circularly polarized light. A CDAD may arise from intrinsic material properties like chirality, spin-orbit interaction, or quantum-geometrical effects on the electronic structure. In addition, CDAD has also been reported for achiral organic molecules at the interface to metallic substrates. For this latter case, we investigate two prototypical $π$-conjugated molecules, namely tetracene and pentacene, whose frontier orbitals have a similar shape but exhibit distinctly different symmetries. By comparing experimental CDAD momentum maps with simulations within time-dependent density functional theory, we show how the final state of the photoelectron must be regarded as the source of the CDAD in such otherwise achiral systems. We gain additional insight into the mechanism by employing a simple scattering model for the final state, which allows us to decompose the CDAD signal into partial wave contributions.

cond-mat.mtrl-sci↗

arXiv2026

Orbitals of Artificial Atoms in a Gapped Two-Dimensional Vacuum

Advances in nanotechnology now allow the creation of artificial atoms - engineered structures whose electronic states closely mimic those of real atoms. Understanding how these artificial atoms interact and bond is key to designing new materials with tailored electronic properties. Here, we use scanning tunnelling microscopy to visualise the bound states of nanostructures patterned in a two-dimensional molecular film featuring a parabolic band with multiple partial energy gaps. The lowest-energy states split off from the bottom of the band and resemble the familiar $s$ and $p$ orbitals of natural atoms, even bonding in the same way. Yet, artificial atoms go beyond this analogy: the gapped two-dimensional vacuum in which they reside gives rise to entirely new orbitals with no counterparts in real atoms. These quasi-one-dimensional localised states enrich the orbital vocabulary of chemistry, adding a new class of orbitals that are predominantly shaped by the surrounding electronic vacuum.

cond-mat.mes-hall↗

arXiv2026

Tracing the film structure of an organic semiconductor with photoemission orbital tomography

Photoemission orbital tomography (POT) is a powerful tool for investigating the orbitals and electronic band structure of oriented layers of organic molecules. In many cases, POT allows conclusions to be drawn regarding the geometric structure, but so far it has been mainly applied to (sub)monolayers and rarely to bilayers, raising the question of whether POT can also provide structure information for thicker films. Here, we use POT to analyze the band dispersion in up to eight layers of $α$-sexithiophene (6T) adsorbed on Cu(110)-p($2\times1$)O. This linear oligomer turns out to be a textbook example that exemplifies the concepts of intra- and intermolecular band dispersion in molecules. Moreover, the rich band and orbital structure information available from POT for this system enables us to trace subtle changes in the crystal structure as a function of layer thickness. Specifically, we find that the periodicity of an intermolecular band changes with film thickness, revealing an increase of the intralayer distance between the molecules with the number of layers. At the same time, the momentum distribution of photoemission from the highest occupied molecular orbital of 6T discloses a decrease of the molecular tilt angle. Following the evolution of tilt angle and lattice constant with layer thickness, we observe -- purely based on electronic structure data -- that the surface-templated monolayer structure relaxes into the structure of bulk 6T crystals. The experimental findings agree well with the results of density functional theory calculations.

cond-mat.mtrl-sci↗

arXiv2026

Subcycle videography of lightwave-driven Landau-Zener-Majorana transitions in graphene

Strong light fields have unlocked previously unthinkable possibilities to tailor coherent electron trajectories, engineer band structures and shape emergent phases of matter all-optically. Unravelling the underlying quantum mechanisms requires a visualisation of the lightwave-driven electron motion directly in the band structure. While photoelectron momentum microscopy has imaged optically excited electrons averaged over many cycles of light, actual subcycle band-structure videography has been limited to small electron momenta. Yet lightwave-driven elementary processes in quantum materials often occur throughout momentum space. Here, we introduce attosecond-precision, subcycle band-structure videography covering the entire first Brillouin zone (BZ) and visualize one of the most fundamental but notoriously elusive strong-field processes: non-adiabatic Landau-Zener-Majorana (LZM) tunnelling. The interplay of field-driven acceleration within the Dirac-like band structure of graphene and periodic LZM interband tunnelling manifest in a coherent displacement and distortion of the momentum distribution at the BZ edge. The extremely non-thermal electron distributions also allow us to disentangle competing scattering processes and assess their impact on coherent electronic control through electron redistribution and thermalization. Our panoramic view of strong-field-driven electron motion in quantum materials lays the foundation for a microscopic understanding of some of the most discussed light-driven phenomena in condensed matter physics.

cond-mat.mes-hall↗

arXiv2025

Observing the spatial and temporal evolution of exciton wave functions

Excitons, the correlated electron-hole pairs governing optical and transport properties in organic semiconductors, have long resisted direct experimental access to their full quantum-mechanical wave functions. Here, we use femtosecond time-resolved photoemission orbital tomography (trPOT), combining high-harmonic probe pulses with time- and momentum-resolved photoelectron spectroscopy, to directly image the momentum-space distribution and ultrafast dynamics of excitons in $α$-sexithiophene thin films. We introduce a quantitative model that enables reconstruction of the exciton wave function in real space, including both its spatial extent and its internal phase structure. The reconstructed wave function reveals coherent delocalization across approximately three molecular units and exhibits a characteristic phase modulation, consistent with ab initio calculations within the framework of many-body perturbation theory. Time-resolved measurements further show a $\sim 20$\% contraction of the exciton radius within 400 fs, providing direct evidence of self-trapping driven by exciton-phonon coupling. These results establish trPOT as a general and experimentally accessible approach for resolving exciton wave functions -- with spatial, phase, and temporal sensitivity -- in a broad class of molecular and low-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2025

Distributed Current Injection into a One-Dimensional Ballistic Edge Channel

We generalize Landauer's theory of ballistic transport in a one-dimensional (1D) conductor to situations where charge carrier injection and extraction are not any more confined to electrodes at either end of the channel, but may occur along its whole length. This type of distributed injection is expected to occur from the two-dimensional (2D) bulk of, e.g., a quantum spin (or anomalous) Hall insulator to its topologically protected edge states. We apply our conceptual solution to the case of two metal electrodes contacting the 2D bulk, enabling us to derive criteria that discriminate ballistic from resistive edge channels in multi-terminal transport experiments.

cond-mat.mes-hall↗

arXiv2025

Bond-resolved STM with density-based methods

Bond-resolved STM (BRSTM) is a recent technique that combines the advantages of scanning tunneling microscopy (STM) with the outstanding intramolecular resolution provided by non-contact atomic force microscopy (ncAFM) using a CO-functionalized tips, offering unique insights into molecular interactions at surfaces. In this work, we present a novel and easily implementable approach for simulating BRSTM images, which we have applied to reproduce new experimental BRSTM data of Perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) on Ag(111), obtained with unprecedented control of tip-sample separation ($\sim$10~pm). Our method integrates the Full-Density-Based Model (FDBM) developed for High-Resolution Atomic Force Microscopy (HRAFM) with Chen's derivative approximation for tunneling channels, effectively capturing the contributions of both $σ$ and $π$ channels, while accounting for the CO-tip deflection induced by probe-sample interactions. This approach accurately reproduces the experimental results for both PTCDA/Ag(111) and 1,5,9-trioxo-13-azatriangulene (TOAT)/Cu(111) systems, including intricate tip-sample distance-dependent features. Furthermore, we also demonstrate the important role of substrate-induced effects, which can modify molecular orbital occupation and the relaxation of the CO probe, resulting in distinct BRSTM image characteristics.

cond-mat.mtrl-sci↗

arXiv2025

Multi-Orbital Charge Transfer into Nonplanar Cycloarenes Revealed with CO-Functionalized Tips

On-surface synthesis has allowed for the tuneable preparation of numerous molecular systems with variable properties. Recently, we demonstrated the highly selective synthesis of kekulene (>99%) on Cu(111) and isokekulene (92%) on Cu(110) from the same molecular precursor (Ruan et al., Angew. Chem. Int. Ed. 2025, e202509932). Scanning tunneling microscopy with CO-functionalized tips can identify the single molecules on the basis of their geometric structure at a low coverage on Cu(110), but it also detects complex features due to electronic contributions close to the Fermi energy. Here, we investigate the origin of these features by simulating STM images based on a weighted sum of multiple molecular orbitals, for which we employ weights based on the calculated molecular-orbital projected density of states. This allows for an experimental confirmation of charge transfer from the surface into multiple formerly unoccupied molecular orbitals for single molecules of kekulene as well as isokekulene in its two nonplanar adsorption configurations. In comparison, the area-integrating photoemission orbital tomography technique confirms the charge transfer as well as the high selectivity for the formation of a full monolayer of mainly isokekulene on Cu(110). Our STM-based approach is applicable to a wide range of adsorbed molecular systems and specifically also suited for strongly interacting surfaces, nonplanar molecules, and such molecules which can only be prepared at extremely low yields.

physics.chem-ph↗

arXiv2025

Solving the Phase Problem of Diffraction: X-ray Standing Waves Imaging on Bismuthene/SiC(0001)

The phase retrieval problem is a fundamental shortcoming of all diffraction-based methods, arising from the inability to measure the phase of scattered waves. The (normal incidence) X-ray standing wave (NIXSW) technique circumvents this issue by introducing a (Bragg-generated) X-ray standing wave field throughout the sample, relative to which any atomic species can be localized by probing its fluorescence or photoelectron yield. In essence, in a single measurement the complex scattering factor (i.e., its amplitude \textit{and} phase) corresponding to the used Bragg reflection is determined. Performing this for multiple Bragg reflections enables one to reconstruct the scattering density of the sample in three dimensions, straightforwardly as the Fourier sum of all measured (complex) scattering factors. Here, we utilize this technique to reveal the structural key features involved in the formation of the quantum spin Hall insulator bismuthene on silicon carbide. In this prominent example, the two-dimensional Bi layer is confined between a 4H-SiC substrate crystal and an epitaxial graphene layer. The key finding is a change in the adsorption site of the Bi atoms underneath the graphene upon hydrogenation, caused by the H-saturation of one (out of three) Si dangling bonds per unit cell. This structural change, clearly revealed by our NIXSW imaging experiment, is the key feature leading to the formation of the characteristic band structure of the 2D bismuthene honeycomb.

cond-mat.mes-hall↗

arXiv2025

Reversible Switching of the Environment-Protected Quantum Spin Hall Insulator Bismuthene at the Graphene/SiC Interface

Quantum Spin Hall Insulators (QSHI) have been extensively studied both theoretically and experimentally because they exhibit robust helical edge states driven by spin-orbit coupling and offer the potential for applications in spintronics through dissipationless spin transport. However, to realize devices, it is indispensable to gain control over the interaction of the active layer with the substrate, and to protect it from environmental influences. Here we show that a single layer of elemental Bi, formed by intercalation of an epitaxial graphene buffer layer on SiC(0001), is a promising candidate for a QSHI. This layer can be reversibly switched between an electronically inactive precursor state and a ``bismuthene state'', the latter exhibiting the predicted band structure of a true two-dimensional bismuthene layer. Switching is accomplished by hydrogenation (dehydrogenation) of the sample, i.e., a partial passivation (activation) of dangling bonds of the SiC substrate, causing a lateral shift of Bi atoms involving a change of the adsorption site. In the bismuthene state, the Bi honeycomb layer is a prospective QSHI, inherently protected by the graphene sheet above and the H-passivated substrate below. Thus, our results represent an important step towards protected QSHI systems beyond graphene.

cond-mat.mes-hall↗

arXiv2025

Tomographic identification of all molecular orbitals in a wide binding energy range

In the past decade, photoemission orbital tomography (POT) has evolved into a powerful tool to investigate the electronic structure of organic molecules adsorbed on surfaces. Here we show that POT allows for the comprehensive experimental identification of all molecular orbitals in a substantial binding energy range, in the present case more than 10 eV. Making use of the angular distribution of photoelectrons as a function of binding energy, we exemplify this by extracting orbital-resolved partial densities of states (pDOS) for 15 $π$ and 23 $σ$ orbitals from the experimental photoemission intensities of the prototypical organic molecule bisanthene (C$_{28}$H$_{14}$) on a Cu(110) surface. In their entirety, these experimentally measured orbital-resolved pDOS for an essentially complete set of orbitals serve as a stringent benchmark for electronic structure methods, which we illustrate by performing density functional theory (DFT) calculations employing four frequently-used exchange-correlation functionals. By computing the respective molecular-orbital-projected densities of states of the bisanthene/Cu(110) interface, a one-to-one comparison with experimental data for an unprecedented number of 38 orbital energies becomes possible. The quantitative analysis of our data reveals that the range-separated hybrid functional HSE performs best for the investigated organic/metal interface. At a more fundamental level, the remarkable agreement between the experimental and the Kohn-Sham orbital energies over a binding energy range larger than 10\,eV suggests that -- perhaps unexpectedly -- Kohn-Sham orbitals approximate Dyson orbitals, which would rigorously account for the electron extraction process in photoemission spectroscopy but are notoriously difficult to compute, in a much better way than previously thought.

physics.chem-ph↗

arXiv2024

Shear-resistant topology in quasi one-dimensional van der Waals material Bi$_4$Br$_4$

Bi$_4$Br$_4$ is a prototypical quasi one-dimensional (1D) material in which covalently bonded bismuth bromide chains are arranged in parallel, side-by-side and layer-by-layer, with van der Waals (vdW) gaps in between. So far, two different structures have been reported for this compound, $α$-Bi$_4$Br$_4$ and $β$-Bi$_4$Br$_4$ , in both of which neighboring chains are shifted by $\mathbf{b}/2$, i.e., half a unit cell vector in the plane, but which differ in their vertical stacking. While the different layer arrangements are known to result in distinct electronic properties, the effect of possible in-plane shifts between the atomic chains remains an open question. Here, using scanning tunneling microscopy and spectroscopy (STM/STS), we report a new Bi$_4$Br$_4$(001) structure, with a shift of $\mathbf{b}/3$ between neighboring chains in the plane and AB layer stacking. We determine shear strain to be the origin of this new structure, which can readily result in shifts of neighboring atomic chains because of the weak inter-chain bonding. For the observed $b/3$ structure, the (residual) atomic chain shift corresponds to an in-plane shear strain of $γ\approx7.5\%$. STS reveals a bulk insulating gap and metallic edge states at surface steps, indicating that the new structure is also a higher-order topological insulator, just like $α$-Bi$_4$Br$_4$, in agreement with density functional theory (DFT) calculations.

cond-mat.mes-hall↗

arXiv2024

Epitaxial growth of mono- and (twisted) multilayer graphene on SiC(0001)

To take full advantage of twisted bilayers of graphene or other two-dimensional materials, it is essential to precisely control the twist angle between the stacked layers, as this parameter determines the properties of the heterostructure. In this context, a growth routine using borazine as a surfactant molecule on SiC(0001) surfaces has been reported, leading to the formation of high-quality epitaxial graphene layers that are unconventionally oriented, i.e., aligned with the substrate lattice (G-$R0^\circ$) [Bocquet et al. Phys. Rev. Lett. 125, 106102 (2020)]. Since the G-$R0^\circ$ layer sits on a buffer layer, also known as zeroth-layer graphene (ZLG), which is rotated $30^\circ$ with respect to the SiC substrate and still covalently bonded to it, decoupling the ZLG-$R30^\circ$ from the substrate can lead to high-quality twisted bilayer graphene (tBLG). Here we report the decoupling of ZLG-$R30^\circ$ by increasing the temperature during annealing in a borazine atmosphere. While this converts ZLG-$R30^\circ$ to G-$R30^\circ$ and thus produces tBLG, the growth process at elevated temperature is no longer self-limiting, so that the surface is covered by a patchwork of graphene multilayers of different thicknesses. We find a 20% coverage of tBLG on ZLG, while on the rest of the surface tBLG sits on one or more additional graphene layers. In order to achieve complete coverage with tBLG only, alternative ways of decoupling the ZLG, e.g., by intercalation with suitable atoms, may be advantageous.

cond-mat.mtrl-sci↗